Computational Modelling — Two-Dimensional Conductive Metal-Organic Frameworks as Highly Efficient Electrocatalysts for Lithium-Sulfur Batteries

58 measurement groups · 182 results

Reported values remain attached to the sample, method, conditions, extraction quality and source location that produced them.

DFT-derived dissolution potential calculation versus standard hydrogen electrode

Density functional theory

Co3(HHTP)2 DFT monolayer model · Model

Udiss = U0diss - Ediff/(n*e); positive Udiss used as criterion for electrochemical stability.

Geometry: periodic 2D slab model
Context: electrochemical stability model
Measurement source: PDF p4 / article p.61208 · Results and Discussion - Electronic Structures and Stability · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
number of electrons in dissolution calculation	2	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
energy difference Ediff	-4.35 eV	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
experimental reversible potential U0 used in calculation	-0.28 V	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
computed dissolution potential Udiss	1.9 V vs SHE	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1

DFT+D2 binding-energy calculation for Li2S4, Li2S6, and Li2S8 adsorption

Density functional theory

Co3(HHTP)2 DFT monolayer model · Model

Binding energy Eb = EMOF + Es - Etotal; positive Eb denotes favourable binding. Most stable adsorption structures considered.

Geometry: periodic 2D slab model
Context: LiPS anchoring model
Measurement source: PDF p2 / article p.61206 · Methods and Computational Details · Equation 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
binding energy to Li2S4	1.59 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S6	0.31 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S8	0.63 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2

DFT geometry optimisation and electronic-structure calculation

Density functional theory

Co3(HHTP)2 DFT monolayer model · Model

Optimised 2D MOF monolayer; lattice constant, magnetic moment, and electronic band gap reported in Table 1.

Geometry: periodic 2D slab model
Context: pristine computational monolayer
Measurement source: PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
electronic band gapMarked as a best value within this paper	0 eV	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
optimised lattice constant	21.53 Angstrom	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
magnetic moment	3 muB/cell	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

DFT-derived dissolution potential calculation versus standard hydrogen electrode

Density functional theory

Co3(HITP)2 DFT monolayer model · Model

Udiss = U0diss - Ediff/(n*e); positive Udiss used as criterion for electrochemical stability.

Geometry: periodic 2D slab model
Context: electrochemical stability model
Measurement source: PDF p4 / article p.61208 · Results and Discussion - Electronic Structures and Stability · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
number of electrons in dissolution calculation	2	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
energy difference Ediff	-5.97 eV	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
experimental reversible potential U0 used in calculation	-0.28 V	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
computed dissolution potential UdissMarked as a best value within this paper	2.7 V vs SHE	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1

DFT+D2 binding-energy calculation for Li2S4, Li2S6, and Li2S8 adsorption

Density functional theory

Co3(HITP)2 DFT monolayer model · Model

Binding energy Eb = EMOF + Es - Etotal; positive Eb denotes favourable binding. Most stable adsorption structures considered.

Geometry: periodic 2D slab model
Context: LiPS anchoring model
Measurement source: PDF p2 / article p.61206 · Methods and Computational Details · Equation 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
binding energy to Li2S4	1.23 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S6	0.85 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S8	0.99 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2

DFT geometry optimisation and electronic-structure calculation

Density functional theory

Co3(HITP)2 DFT monolayer model · Model

Optimised 2D MOF monolayer; lattice constant, magnetic moment, and electronic band gap reported in Table 1.

Geometry: periodic 2D slab model
Context: pristine computational monolayer
Measurement source: PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
electronic band gap	0.241 eV	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
optimised lattice constant	21.93 Angstrom	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
magnetic moment	3 muB/cell	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

DFT-derived dissolution potential calculation versus standard hydrogen electrode

Density functional theory

Co3(HTTP)2 DFT monolayer model · Model

Udiss = U0diss - Ediff/(n*e); positive Udiss used as criterion for electrochemical stability.

Geometry: periodic 2D slab model
Context: electrochemical stability model
Measurement source: PDF p4 / article p.61208 · Results and Discussion - Electronic Structures and Stability · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
number of electrons in dissolution calculation	2	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
energy difference Ediff	-4.03 eV	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
experimental reversible potential U0 used in calculation	-0.28 V	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
computed dissolution potential Udiss	1.74 V vs SHE	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1

DFT+D2 binding-energy calculation for Li2S4, Li2S6, and Li2S8 adsorption

Density functional theory

Co3(HTTP)2 DFT monolayer model · Model

Binding energy Eb = EMOF + Es - Etotal; positive Eb denotes favourable binding. Most stable adsorption structures considered.

Geometry: periodic 2D slab model
Context: LiPS anchoring model
Measurement source: PDF p2 / article p.61206 · Methods and Computational Details · Equation 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
binding energy to Li2S4	1.49 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S6	0.66 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S8	1.31 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2

DFT geometry optimisation and electronic-structure calculation

Density functional theory

Co3(HTTP)2 DFT monolayer model · Model

Optimised 2D MOF monolayer; lattice constant, magnetic moment, and electronic band gap reported in Table 1.

Geometry: periodic 2D slab model
Context: pristine computational monolayer
Measurement source: PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
electronic band gap	0.437 eV	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
optimised lattice constant	23.24 Angstrom	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
magnetic moment	3 muB/cell	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

DFT-derived dissolution potential calculation versus standard hydrogen electrode

Density functional theory

Cu3(C18H9O3N3)2 DFT monolayer model · Model

Udiss = U0diss - Ediff/(n*e); positive Udiss used as criterion for electrochemical stability.

Geometry: periodic 2D slab model
Context: electrochemical stability model
Measurement source: PDF p4 / article p.61208 · Results and Discussion - Electronic Structures and Stability · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
number of electrons in dissolution calculation	2	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
energy difference Ediff	-3.02 eV	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
experimental reversible potential U0 used in calculation	+0.34 V	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
computed dissolution potential Udiss	1.85 V vs SHE	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1

DFT binding-energy values read from Figure 2g for additional lithiation states

Density functional theory

Cu3(C18H9O3N3)2 DFT monolayer model · Model

Graphical binding energies for S8, Li2S2, and Li2S on candidate 2D MOFs; exact table values were not available in the text layer.

Geometry: periodic 2D slab model
Context: LiPS/S8 anchoring model
Measurement source: PDF p4 / article p.61208 · Results and Discussion - Anchoring Ability to LiPSs · Figure 2g

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
binding energy to Li2S	approximately 3.02 eV	—	—	Figure Axis Approximate	PDF p4 / article p.61208 · Results and Discussion - Anchoring Ability to LiPSs · Figure 2g
binding energy to Li2S2	approximately 2.32 eV	—	—	Figure Axis Approximate	PDF p4 / article p.61208 · Results and Discussion - Anchoring Ability to LiPSs · Figure 2g
binding energy to S8	approximately 0.4 eV	—	—	Figure Axis Approximate	PDF p4 / article p.61208 · Results and Discussion - Anchoring Ability to LiPSs · Figure 2g

CI-NEB/DFT Li2S delithiation barrier and Li-S bond activation calculation

Density functional theory

Cu3(C18H9O3N3)2 DFT monolayer model · Model

Dissociation pathway Li2S -> LiS + Li+ + e- on selected 2D MOF anchoring material.

Geometry: periodic 2D slab model
Context: Li-S charge electrocatalysis model
Measurement source: PDF p6 / article p.61210 · Results and Discussion - Li2S Decomposition Kinetics and Li+ Diffusion · Figure 5b

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
Li2S decomposition barrierMarked as a best value within this paper	0.83 eV	—	—	Text Exact Reported	PDF p6 / article p.61210 · Results and Discussion - Li2S Decomposition Kinetics and Li+ Diffusion · Figure 5b
Li-S bond length in adsorbed Li2S	2.25 Angstrom	—	—	Text Exact Reported	PDF p6 / article p.61210 · Results and Discussion - Li2S Decomposition Kinetics and Li+ Diffusion

DFT+D2 binding-energy calculation for Li2S4, Li2S6, and Li2S8 adsorption

Density functional theory

Cu3(C18H9O3N3)2 DFT monolayer model · Model

Binding energy Eb = EMOF + Es - Etotal; positive Eb denotes favourable binding. Most stable adsorption structures considered.

Geometry: periodic 2D slab model
Context: LiPS anchoring model
Measurement source: PDF p2 / article p.61206 · Methods and Computational Details · Equation 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
binding energy to Li2S4Marked as a best value within this paper	1.48 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S6Marked as a best value within this paper	1.29 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S8Marked as a best value within this paper	1.37 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2

DFT energetic comparison of intact and decomposed adsorbed Li2Sn species

Density functional theory

Cu3(C18H9O3N3)2 DFT monolayer model · Model

Energy differences defined by Equations 6 and 7; negative values imply intact Li2Sn is more stable than decomposed configurations.

Geometry: periodic 2D slab model
Context: LiPS stability on catalyst model
Measurement source: PDF p7 / article p.61211 · Results and Discussion - Stability of Li2Sn Species · Figure 6b

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
DeltaE1 intact Li2S4 vs Li + LiS4	-0.82 eV	—	—	Visual Estimate Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Stability of Li2Sn Species · Figure 6b
DeltaE2 intact Li2S4 vs Li + Li + S4	-1.86 eV	—	—	Visual Estimate Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Stability of Li2Sn Species · Figure 6b
DeltaE1 intact Li2S6 vs Li + LiS6	-1.48 eV	—	—	Visual Estimate Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Stability of Li2Sn Species · Figure 6b

DFT Gibbs free-energy pathway for sulfur reduction reaction (SRR)

Density functional theory

Cu3(C18H9O3N3)2 DFT monolayer model · Model

Reaction coordinate S8 -> Li2S8 -> Li2S6 -> Li2S4 -> Li2S2 -> Li2S on selected 2D MOF catalyst model.

Geometry: periodic 2D slab model
Context: Li-S discharge electrocatalysis model
Measurement source: PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
SRR rate-limiting free-energy stepMarked as a best value within this paper	DeltaG4 = 0.46 eV	—	—	Text Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Gibbs Free Energies in the SRR
DeltaG1 S8 to Li2S8	-6.55 eV	—	—	Figure Axis Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a
DeltaG2 Li2S8 to Li2S6	-0.23 eV	—	—	Figure Axis Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a
DeltaG3 Li2S6 to Li2S4	0.29 eV	—	—	Figure Axis Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a
DeltaG4 Li2S4 to Li2S2	0.46 eV	—	—	Figure Axis Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a
DeltaG5 Li2S2 to Li2S	0.37 eV	—	—	Figure Axis Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a

DFT geometry optimisation and electronic-structure calculation

Density functional theory

Cu3(C18H9O3N3)2 DFT monolayer model · Model

Optimised 2D MOF monolayer; lattice constant, magnetic moment, and electronic band gap reported in Table 1.

Geometry: periodic 2D slab model
Context: pristine computational monolayer
Measurement source: PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
electronic band gapMarked as a best value within this paper	0 eV	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
optimised lattice constant	21.96 Angstrom	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
magnetic moment	0.98 muB/cell	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

DFT comparison of binding energies with and without vdW correction

Density functional theory

Cu3(C18H9O3N3)2 DFT monolayer model · Model

Ratio R = (Eb_vdW - Eb_withoutvdW)/Eb_vdW * 100% for Li2Sn adsorption.

Geometry: periodic 2D slab model
Context: LiPS anchoring mechanism
Measurement source: PDF p2 / article p.61206 · Methods and Computational Details · Equation 2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
vdW interaction contribution range for Li2Sn (n = 4, 6, 8)	29-47%	—	—	Text Range	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Figure 2h

DFT-derived dissolution potential calculation versus standard hydrogen electrode

Density functional theory

Cu3(HHTP)2 DFT monolayer model · Model

Udiss = U0diss - Ediff/(n*e); positive Udiss used as criterion for electrochemical stability.

Geometry: periodic 2D slab model
Context: electrochemical stability model
Measurement source: PDF p4 / article p.61208 · Results and Discussion - Electronic Structures and Stability · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
number of electrons in dissolution calculation	2	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
energy difference Ediff	-2.45 eV	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
experimental reversible potential U0 used in calculation	+0.34 V	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
computed dissolution potential Udiss	1.57 V vs SHE	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1

DFT+D2 binding-energy calculation for Li2S4, Li2S6, and Li2S8 adsorption

Density functional theory

Cu3(HHTP)2 DFT monolayer model · Model

Binding energy Eb = EMOF + Es - Etotal; positive Eb denotes favourable binding. Most stable adsorption structures considered.

Geometry: periodic 2D slab model
Context: LiPS anchoring model
Measurement source: PDF p2 / article p.61206 · Methods and Computational Details · Equation 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
binding energy to Li2S4	1.72 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S6	1.1 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S8	1.29 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2

DFT geometry optimisation and electronic-structure calculation

Density functional theory

Cu3(HHTP)2 DFT monolayer model · Model

Optimised 2D MOF monolayer; lattice constant, magnetic moment, and electronic band gap reported in Table 1.

Geometry: periodic 2D slab model
Context: pristine computational monolayer
Measurement source: PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
electronic band gapMarked as a best value within this paper	0 eV	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
optimised lattice constant	21.8 Angstrom	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
magnetic moment	1 muB/cell	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

TDOS/PDOS calculation for S8 and Li2Sn adsorbed on Cu3(HITP)2

Cu3(HITP)2 DFT monolayer model · Model

Electronic density of states with Fermi level set to 0 for S8 and Li2Sn@Cu3(HITP)2 (n = 8, 6, 4, 2, 1).

Geometry: periodic 2D slab model
Context: adsorbate-covered conductive MOF model
Measurement source: PDF p6 / article p.61210 · Results and Discussion - Electrical Conductivity · Figure 3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
metallic character retained during LiPS adsorption	metallic features remain intact	—	—	Text Qualitative	PDF p5 / article p.61209 · Results and Discussion - Electrical Conductivity · Figure 3

DFT-derived dissolution potential calculation versus standard hydrogen electrode

Density functional theory

Cu3(HITP)2 DFT monolayer model · Model

Udiss = U0diss - Ediff/(n*e); positive Udiss used as criterion for electrochemical stability.

Geometry: periodic 2D slab model
Context: electrochemical stability model
Measurement source: PDF p4 / article p.61208 · Results and Discussion - Electronic Structures and Stability · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
number of electrons in dissolution calculation	2	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
energy difference Ediff	-3.54 eV	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
experimental reversible potential U0 used in calculation	+0.34 V	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
computed dissolution potential Udiss	2.11 V vs SHE	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1

DFT binding-energy values read from Figure 2g for additional lithiation states

Density functional theory

Cu3(HITP)2 DFT monolayer model · Model

Graphical binding energies for S8, Li2S2, and Li2S on candidate 2D MOFs; exact table values were not available in the text layer.

Geometry: periodic 2D slab model
Context: LiPS/S8 anchoring model
Measurement source: PDF p4 / article p.61208 · Results and Discussion - Anchoring Ability to LiPSs · Figure 2g

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
binding energy to Li2S	approximately 1.9 eV	—	—	Figure Axis Approximate	PDF p4 / article p.61208 · Results and Discussion - Anchoring Ability to LiPSs · Figure 2g
binding energy to Li2S2	approximately 1.75 eV	—	—	Figure Axis Approximate	PDF p4 / article p.61208 · Results and Discussion - Anchoring Ability to LiPSs · Figure 2g
binding energy to S8	approximately 0.4 eV	—	—	Figure Axis Approximate	PDF p4 / article p.61208 · Results and Discussion - Anchoring Ability to LiPSs · Figure 2g

CI-NEB/DFT Li2S delithiation barrier and Li-S bond activation calculation

Density functional theory

Cu3(HITP)2 DFT monolayer model · Model

Dissociation pathway Li2S -> LiS + Li+ + e- on selected 2D MOF anchoring material.

Geometry: periodic 2D slab model
Context: Li-S charge electrocatalysis model
Measurement source: PDF p6 / article p.61210 · Results and Discussion - Li2S Decomposition Kinetics and Li+ Diffusion · Figure 5b

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
Li2S decomposition barrier	0.84 eV	—	—	Text Exact Reported	PDF p6 / article p.61210 · Results and Discussion - Li2S Decomposition Kinetics and Li+ Diffusion · Figure 5b
Li-S bond length in adsorbed Li2S	2.22 Angstrom	—	—	Text Exact Reported	PDF p6 / article p.61210 · Results and Discussion - Li2S Decomposition Kinetics and Li+ Diffusion

DFT+D2 binding-energy calculation for Li2S4, Li2S6, and Li2S8 adsorption

Density functional theory

Cu3(HITP)2 DFT monolayer model · Model

Binding energy Eb = EMOF + Es - Etotal; positive Eb denotes favourable binding. Most stable adsorption structures considered.

Geometry: periodic 2D slab model
Context: LiPS anchoring model
Measurement source: PDF p2 / article p.61206 · Methods and Computational Details · Equation 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
binding energy to Li2S4Marked as a best value within this paper	1.32 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S6Marked as a best value within this paper	1.03 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S8Marked as a best value within this paper	1.32 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2

DFT energetic comparison of intact and decomposed adsorbed Li2Sn species

Density functional theory

Cu3(HITP)2 DFT monolayer model · Model

Energy differences defined by Equations 6 and 7; negative values imply intact Li2Sn is more stable than decomposed configurations.

Geometry: periodic 2D slab model
Context: LiPS stability on catalyst model
Measurement source: PDF p7 / article p.61211 · Results and Discussion - Stability of Li2Sn Species · Figure 6b

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
DeltaE1 intact Li2S4 vs Li + LiS4	-1.07 eV	—	—	Visual Estimate Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Stability of Li2Sn Species · Figure 6b
DeltaE2 intact Li2S4 vs Li + Li + S4	-2.04 eV	—	—	Visual Estimate Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Stability of Li2Sn Species · Figure 6b
DeltaE1 intact Li2S6 vs Li + LiS6	-1.27 eV	—	—	Visual Estimate Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Stability of Li2Sn Species · Figure 6b

Continuum-solvation DFT binding energies for long-chain LiPSs on Cu3(HITP)2

Density functional theory

Cu3(HITP)2 DFT monolayer model · Model

Continuum solvent model with dielectric constant 7.8 to mimic DME/DOL electrolyte.

Geometry: periodic 2D slab model
Context: solvated LiPS anchoring model
Measurement source: PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Figure S4

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
solvated binding energy to Li2S4	0.21 eV	—	—	Text Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Figure S4
solvated binding energy to Li2S6	0.5 eV	—	—	Text Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Figure S4
solvated binding energy to Li2S8	0.24 eV	—	—	Text Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Figure S4

DFT Gibbs free-energy pathway for sulfur reduction reaction (SRR)

Density functional theory

Cu3(HITP)2 DFT monolayer model · Model

Reaction coordinate S8 -> Li2S8 -> Li2S6 -> Li2S4 -> Li2S2 -> Li2S on selected 2D MOF catalyst model.

Geometry: periodic 2D slab model
Context: Li-S discharge electrocatalysis model
Measurement source: PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
SRR rate-limiting free-energy step	DeltaG5 = 0.98 eV	—	—	Text Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Gibbs Free Energies in the SRR
DeltaG1 S8 to Li2S8	-6.5 eV	—	—	Figure Axis Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a
DeltaG2 Li2S8 to Li2S6	0.03 eV	—	—	Figure Axis Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a
DeltaG3 Li2S6 to Li2S4	0.07 eV	—	—	Figure Axis Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a
DeltaG4 Li2S4 to Li2S2	0.85 eV	—	—	Figure Axis Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a
DeltaG5 Li2S2 to Li2S	0.98 eV	—	—	Figure Axis Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a

DFT geometry optimisation and electronic-structure calculation

Density functional theory

Cu3(HITP)2 DFT monolayer model · Model

Optimised 2D MOF monolayer; lattice constant, magnetic moment, and electronic band gap reported in Table 1.

Geometry: periodic 2D slab model
Context: pristine computational monolayer
Measurement source: PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
electronic band gapMarked as a best value within this paper	0 eV	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
optimised lattice constant	22.02 Angstrom	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
magnetic moment	0 muB/cell	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

DFT average Li2S binding and maximum sulfur loading model

Density functional theory

Cu3(HITP)2 DFT monolayer model · Model

Li2S adsorption on one and both sides of Cu3(HITP)2; stable Li30S15 and Li60S30 configurations in Figure S7.

Geometry: periodic 2D slab model
Context: high-sulfur-loading electrocatalyst model
Measurement source: PDF p7 / article p.61211 · Results and Discussion - Sulfur Loading Amount · Figure S7 / Equation 8

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
average Li2S binding energy for one-side Li30S15 loading	3.13 eV	—	—	Text Exact Reported	PDF p7 / article p.61211 · Results and Discussion - Sulfur Loading Amount
average Li2S binding energy for two-side Li60S30 loading	3.03 eV	—	—	Text Exact Reported	PDF p7 / article p.61211 · Results and Discussion - Sulfur Loading Amount
maximum sulfur weight percentageMarked as a best value within this paper	about 70.2 wt %	—	—	Text Approximate	PDF p7 / article p.61211 · Results and Discussion - Sulfur Loading Amount

DFT comparison of binding energies with and without vdW correction

Density functional theory

Cu3(HITP)2 DFT monolayer model · Model

Ratio R = (Eb_vdW - Eb_withoutvdW)/Eb_vdW * 100% for Li2Sn adsorption.

Geometry: periodic 2D slab model
Context: LiPS anchoring mechanism
Measurement source: PDF p2 / article p.61206 · Methods and Computational Details · Equation 2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
vdW interaction contribution range for Li2Sn (n = 4, 6, 8)	29-47%	—	—	Text Range	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Figure 2h

DFT-derived dissolution potential calculation versus standard hydrogen electrode

Density functional theory

Cu3(HTTP)2 DFT monolayer model · Model

Udiss = U0diss - Ediff/(n*e); positive Udiss used as criterion for electrochemical stability.

Geometry: periodic 2D slab model
Context: electrochemical stability model
Measurement source: PDF p4 / article p.61208 · Results and Discussion - Electronic Structures and Stability · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
number of electrons in dissolution calculation	2	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
energy difference Ediff	-3.27 eV	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
experimental reversible potential U0 used in calculation	+0.34 V	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
computed dissolution potential Udiss	1.98 V vs SHE	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1

DFT+D2 binding-energy calculation for Li2S4, Li2S6, and Li2S8 adsorption

Density functional theory

Cu3(HTTP)2 DFT monolayer model · Model

Binding energy Eb = EMOF + Es - Etotal; positive Eb denotes favourable binding. Most stable adsorption structures considered.

Geometry: periodic 2D slab model
Context: LiPS anchoring model
Measurement source: PDF p2 / article p.61206 · Methods and Computational Details · Equation 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
binding energy to Li2S4	1.14 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S6	0.75 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S8	0.85 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2

DFT geometry optimisation and electronic-structure calculation

Density functional theory

Cu3(HTTP)2 DFT monolayer model · Model

Optimised 2D MOF monolayer; lattice constant, magnetic moment, and electronic band gap reported in Table 1.

Geometry: periodic 2D slab model
Context: pristine computational monolayer
Measurement source: PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
electronic band gapMarked as a best value within this paper	0 eV	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
optimised lattice constant	23.29 Angstrom	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
magnetic moment	0 muB/cell	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

Spin-polarised DFT in VASP with PAW potentials, PBE GGA, DFT+D2 vdW correction, CI-NEB barriers, and continuum solvation model for DME/DOL electrolyte.

Density functional theory

Cu3(HITP)2 DFT monolayer model · Model

Plane-wave cutoff 520 eV; Monkhorst-Pack k-points; force convergence below 0.01 eV/Angstrom; 20 Angstrom vacuum normal to monolayer; dielectric constant 7.8 for DME/DOL (1:1).

Geometry: periodic 2D slab model
Context: computational model
Measurement source: PDF p2 / article p.61206 · Methods and Computational Details

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source

DFT-derived dissolution potential calculation versus standard hydrogen electrode

Density functional theory

Ni3(HHTP)2 DFT monolayer model · Model

Udiss = U0diss - Ediff/(n*e); positive Udiss used as criterion for electrochemical stability.

Geometry: periodic 2D slab model
Context: electrochemical stability model
Measurement source: PDF p4 / article p.61208 · Results and Discussion - Electronic Structures and Stability · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
number of electrons in dissolution calculation	2	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
energy difference Ediff	-3.89 eV	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
experimental reversible potential U0 used in calculation	-0.26 V	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
computed dissolution potential Udiss	1.69 V vs SHE	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1

DFT+D2 binding-energy calculation for Li2S4, Li2S6, and Li2S8 adsorption

Density functional theory

Ni3(HHTP)2 DFT monolayer model · Model

Binding energy Eb = EMOF + Es - Etotal; positive Eb denotes favourable binding. Most stable adsorption structures considered.

Geometry: periodic 2D slab model
Context: LiPS anchoring model
Measurement source: PDF p2 / article p.61206 · Methods and Computational Details · Equation 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
binding energy to Li2S4	1.66 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S6	0.77 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S8	0.93 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2

DFT geometry optimisation and electronic-structure calculation

Density functional theory

Ni3(HHTP)2 DFT monolayer model · Model

Optimised 2D MOF monolayer; lattice constant, magnetic moment, and electronic band gap reported in Table 1.

Geometry: periodic 2D slab model
Context: pristine computational monolayer
Measurement source: PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
electronic band gapMarked as a best value within this paper	0 eV	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
optimised lattice constant	21.52 Angstrom	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
magnetic moment	0 muB/cell	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

DFT-derived dissolution potential calculation versus standard hydrogen electrode

Density functional theory

Ni3(HITP)2 DFT monolayer model · Model

Udiss = U0diss - Ediff/(n*e); positive Udiss used as criterion for electrochemical stability.

Geometry: periodic 2D slab model
Context: electrochemical stability model
Measurement source: PDF p4 / article p.61208 · Results and Discussion - Electronic Structures and Stability · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
number of electrons in dissolution calculation	2	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
energy difference Ediff	-5.59 eV	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
experimental reversible potential U0 used in calculation	-0.26 V	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
computed dissolution potential Udiss	2.54 V vs SHE	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1

DFT+D2 binding-energy calculation for Li2S4, Li2S6, and Li2S8 adsorption

Density functional theory

Ni3(HITP)2 DFT monolayer model · Model

Binding energy Eb = EMOF + Es - Etotal; positive Eb denotes favourable binding. Most stable adsorption structures considered.

Geometry: periodic 2D slab model
Context: LiPS anchoring model
Measurement source: PDF p2 / article p.61206 · Methods and Computational Details · Equation 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
binding energy to Li2S4	1.16 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S6	0.89 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S8	1.01 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2

DFT geometry optimisation and electronic-structure calculation

Density functional theory

Ni3(HITP)2 DFT monolayer model · Model

Optimised 2D MOF monolayer; lattice constant, magnetic moment, and electronic band gap reported in Table 1.

Geometry: periodic 2D slab model
Context: pristine computational monolayer
Measurement source: PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
electronic band gap	0.126 eV	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
optimised lattice constant	21.89 Angstrom	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
magnetic moment	0 muB/cell	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

DFT-derived dissolution potential calculation versus standard hydrogen electrode

Density functional theory

Ni3(HTTP)2 DFT monolayer model · Model

Udiss = U0diss - Ediff/(n*e); positive Udiss used as criterion for electrochemical stability.

Geometry: periodic 2D slab model
Context: electrochemical stability model
Measurement source: PDF p4 / article p.61208 · Results and Discussion - Electronic Structures and Stability · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
number of electrons in dissolution calculation	2	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
energy difference Ediff	-3.99 eV	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
experimental reversible potential U0 used in calculation	-0.26 V	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
computed dissolution potential Udiss	1.74 V vs SHE	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1

DFT+D2 binding-energy calculation for Li2S4, Li2S6, and Li2S8 adsorption

Density functional theory

Ni3(HTTP)2 DFT monolayer model · Model

Binding energy Eb = EMOF + Es - Etotal; positive Eb denotes favourable binding. Most stable adsorption structures considered.

Geometry: periodic 2D slab model
Context: LiPS anchoring model
Measurement source: PDF p2 / article p.61206 · Methods and Computational Details · Equation 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
binding energy to Li2S4	1.26 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S6	0.74 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S8	0.79 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2

DFT geometry optimisation and electronic-structure calculation

Density functional theory

Ni3(HTTP)2 DFT monolayer model · Model

Optimised 2D MOF monolayer; lattice constant, magnetic moment, and electronic band gap reported in Table 1.

Geometry: periodic 2D slab model
Context: pristine computational monolayer
Measurement source: PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
electronic band gap	0.273 eV	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
optimised lattice constant	23.19 Angstrom	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
magnetic moment	0 muB/cell	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

DFT-derived dissolution potential calculation versus standard hydrogen electrode

Density functional theory

Zn3(HHTP)2 DFT monolayer model · Model

Udiss = U0diss - Ediff/(n*e); positive Udiss used as criterion for electrochemical stability.

Geometry: periodic 2D slab model
Context: electrochemical stability model
Measurement source: PDF p4 / article p.61208 · Results and Discussion - Electronic Structures and Stability · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
number of electrons in dissolution calculation	2	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
energy difference Ediff	-3.66 eV	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
experimental reversible potential U0 used in calculation	-0.76 V	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
computed dissolution potential Udiss	1.07 V vs SHE	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1

DFT+D2 binding-energy calculation for Li2S4, Li2S6, and Li2S8 adsorption

Density functional theory

Zn3(HHTP)2 DFT monolayer model · Model

Binding energy Eb = EMOF + Es - Etotal; positive Eb denotes favourable binding. Most stable adsorption structures considered.

Geometry: periodic 2D slab model
Context: LiPS anchoring model
Measurement source: PDF p2 / article p.61206 · Methods and Computational Details · Equation 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
binding energy to Li2S4	1.95 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S6	1.56 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S8	1.7 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2

DFT geometry optimisation and electronic-structure calculation

Density functional theory

Zn3(HHTP)2 DFT monolayer model · Model

Optimised 2D MOF monolayer; lattice constant, magnetic moment, and electronic band gap reported in Table 1.

Geometry: periodic 2D slab model
Context: pristine computational monolayer
Measurement source: PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
electronic band gapMarked as a best value within this paper	0 eV	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
optimised lattice constant	21.94 Angstrom	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
magnetic moment	2 muB/cell	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

DFT-derived dissolution potential calculation versus standard hydrogen electrode

Density functional theory

Zn3(HITP)2 DFT monolayer model · Model

Udiss = U0diss - Ediff/(n*e); positive Udiss used as criterion for electrochemical stability.

Geometry: periodic 2D slab model
Context: electrochemical stability model
Measurement source: PDF p4 / article p.61208 · Results and Discussion - Electronic Structures and Stability · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
number of electrons in dissolution calculation	2	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
energy difference Ediff	-4.69 eV	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
experimental reversible potential U0 used in calculation	-0.76 V	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
computed dissolution potential Udiss	1.59 V vs SHE	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1

DFT binding-energy values read from Figure 2g for additional lithiation states

Density functional theory

Zn3(HITP)2 DFT monolayer model · Model

Graphical binding energies for S8, Li2S2, and Li2S on candidate 2D MOFs; exact table values were not available in the text layer.

Geometry: periodic 2D slab model
Context: LiPS/S8 anchoring model
Measurement source: PDF p4 / article p.61208 · Results and Discussion - Anchoring Ability to LiPSs · Figure 2g

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
binding energy to Li2S	approximately 2.85 eV	—	—	Figure Axis Approximate	PDF p4 / article p.61208 · Results and Discussion - Anchoring Ability to LiPSs · Figure 2g
binding energy to Li2S2	approximately 2.25 eV	—	—	Figure Axis Approximate	PDF p4 / article p.61208 · Results and Discussion - Anchoring Ability to LiPSs · Figure 2g
binding energy to S8	approximately 0.78 eV	—	—	Figure Axis Approximate	PDF p4 / article p.61208 · Results and Discussion - Anchoring Ability to LiPSs · Figure 2g

CI-NEB/DFT Li2S delithiation barrier and Li-S bond activation calculation

Density functional theory

Zn3(HITP)2 DFT monolayer model · Model

Dissociation pathway Li2S -> LiS + Li+ + e- on selected 2D MOF anchoring material.

Geometry: periodic 2D slab model
Context: Li-S charge electrocatalysis model
Measurement source: PDF p6 / article p.61210 · Results and Discussion - Li2S Decomposition Kinetics and Li+ Diffusion · Figure 5b

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
Li2S decomposition barrier	1.49 eV	—	—	Text Exact Reported	PDF p6 / article p.61210 · Results and Discussion - Li2S Decomposition Kinetics and Li+ Diffusion · Figure 5b
Li-S bond length in adsorbed Li2S	2.22 Angstrom	—	—	Text Exact Reported	PDF p6 / article p.61210 · Results and Discussion - Li2S Decomposition Kinetics and Li+ Diffusion

DFT+D2 binding-energy calculation for Li2S4, Li2S6, and Li2S8 adsorption

Density functional theory

Zn3(HITP)2 DFT monolayer model · Model

Binding energy Eb = EMOF + Es - Etotal; positive Eb denotes favourable binding. Most stable adsorption structures considered.

Geometry: periodic 2D slab model
Context: LiPS anchoring model
Measurement source: PDF p2 / article p.61206 · Methods and Computational Details · Equation 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
binding energy to Li2S4Marked as a best value within this paper	1.71 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S6Marked as a best value within this paper	1.51 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S8Marked as a best value within this paper	1.69 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2

DFT energetic comparison of intact and decomposed adsorbed Li2Sn species

Density functional theory

Zn3(HITP)2 DFT monolayer model · Model

Energy differences defined by Equations 6 and 7; negative values imply intact Li2Sn is more stable than decomposed configurations.

Geometry: periodic 2D slab model
Context: LiPS stability on catalyst model
Measurement source: PDF p7 / article p.61211 · Results and Discussion - Stability of Li2Sn Species · Figure 6b

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
DeltaE1 intact Li2S4 vs Li + LiS4	-1.23 eV	—	—	Visual Estimate Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Stability of Li2Sn Species · Figure 6b
DeltaE2 intact Li2S4 vs Li + Li + S4	-2.05 eV	—	—	Visual Estimate Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Stability of Li2Sn Species · Figure 6b
DeltaE1 intact Li2S6 vs Li + LiS6	-1.42 eV	—	—	Visual Estimate Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Stability of Li2Sn Species · Figure 6b

DFT Gibbs free-energy pathway for sulfur reduction reaction (SRR)

Density functional theory

Zn3(HITP)2 DFT monolayer model · Model

Reaction coordinate S8 -> Li2S8 -> Li2S6 -> Li2S4 -> Li2S2 -> Li2S on selected 2D MOF catalyst model.

Geometry: periodic 2D slab model
Context: Li-S discharge electrocatalysis model
Measurement source: PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
SRR rate-limiting free-energy step	DeltaG4 = 0.75 eV	—	—	Text Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Gibbs Free Energies in the SRR
DeltaG1 S8 to Li2S8	-6.5 eV	—	—	Figure Axis Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a
DeltaG2 Li2S8 to Li2S6	-0.07 eV	—	—	Figure Axis Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a
DeltaG3 Li2S6 to Li2S4	0.29 eV	—	—	Figure Axis Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a
DeltaG4 Li2S4 to Li2S2	0.75 eV	—	—	Figure Axis Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a
DeltaG5 Li2S2 to Li2S	0.47 eV	—	—	Figure Axis Rounded Reported	PDF p7 / article p.61211 · Results and Discussion - Gibbs Free Energies in the SRR · Figure 5a

DFT geometry optimisation and electronic-structure calculation

Density functional theory

Zn3(HITP)2 DFT monolayer model · Model

Optimised 2D MOF monolayer; lattice constant, magnetic moment, and electronic band gap reported in Table 1.

Geometry: periodic 2D slab model
Context: pristine computational monolayer
Measurement source: PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
electronic band gapMarked as a best value within this paper	0 eV	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
optimised lattice constant	22.52 Angstrom	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
magnetic moment	0 muB/cell	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

DFT comparison of binding energies with and without vdW correction

Density functional theory

Zn3(HITP)2 DFT monolayer model · Model

Ratio R = (Eb_vdW - Eb_withoutvdW)/Eb_vdW * 100% for Li2Sn adsorption.

Geometry: periodic 2D slab model
Context: LiPS anchoring mechanism
Measurement source: PDF p2 / article p.61206 · Methods and Computational Details · Equation 2

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
vdW interaction contribution range for Li2Sn (n = 4, 6, 8)	29-47%	—	—	Text Range	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Figure 2h

DFT-derived dissolution potential calculation versus standard hydrogen electrode

Density functional theory

Zn3(HTTP)2 DFT monolayer model · Model

Udiss = U0diss - Ediff/(n*e); positive Udiss used as criterion for electrochemical stability.

Geometry: periodic 2D slab model
Context: electrochemical stability model
Measurement source: PDF p4 / article p.61208 · Results and Discussion - Electronic Structures and Stability · Table S1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
number of electrons in dissolution calculation	2	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
energy difference Ediff	-3.53 eV	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
experimental reversible potential U0 used in calculation	-0.76 V	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1
computed dissolution potential Udiss	1.01 V vs SHE	—	—	SI Table Exact Reported	PDF p9 / SI p.S9 · Supporting Information · Table S1

DFT+D2 binding-energy calculation for Li2S4, Li2S6, and Li2S8 adsorption

Density functional theory

Zn3(HTTP)2 DFT monolayer model · Model

Binding energy Eb = EMOF + Es - Etotal; positive Eb denotes favourable binding. Most stable adsorption structures considered.

Geometry: periodic 2D slab model
Context: LiPS anchoring model
Measurement source: PDF p2 / article p.61206 · Methods and Computational Details · Equation 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
binding energy to Li2S4	2.74 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S6	1.8 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2
binding energy to Li2S8	1.86 eV	—	—	Table Exact Reported	PDF p5 / article p.61209 · Results and Discussion - Anchoring Ability to LiPSs · Table 2

DFT geometry optimisation and electronic-structure calculation

Density functional theory

Zn3(HTTP)2 DFT monolayer model · Model

Optimised 2D MOF monolayer; lattice constant, magnetic moment, and electronic band gap reported in Table 1.

Geometry: periodic 2D slab model
Context: pristine computational monolayer
Measurement source: PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
electronic band gapMarked as a best value within this paper	0 eV	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
optimised lattice constant	23.66 Angstrom	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1
magnetic moment	0.66 muB/cell	—	—	Table Exact Reported	PDF p3 / article p.61207 · Results and Discussion - Electronic Structures and Stability · Table 1