Computational Modelling — Regulating Electronic Structure of Bimetallic NiFe-THQ Conductive Metal–Organic Frameworks to Boost Catalytic Activity for Oxygen Evolution Reaction

4 measurement groups · 68 results

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

DFT geometry optimisation

Density functional theory

NixFe1-x-THQ series · Powder

Calculated M-O bond lengths for Fe-THQ, Ni-THQ and Ni0.5Fe0.5-THQ Fe/Ni sites.

Geometry: model
Context: model systems
Measurement source: p018 · S2 Supplementary Figures and Tables · Table S3

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
Fe-THQ M-O1 bond length	1.907	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Fe-THQ M-O2 bond length	2.004	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Fe-THQ M-O3 bond length	2.004	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Fe-THQ M-O4 bond length	1.907	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Fe-THQ M-O5 bond length	1.907	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Fe-THQ M-O6 bond length	2.004	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni0.5Fe0.5-THQ(Fe) M-O1 bond length	2.036	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni0.5Fe0.5-THQ(Fe) M-O2 bond length	2.086	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni0.5Fe0.5-THQ(Fe) M-O3 bond length	2.086	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni0.5Fe0.5-THQ(Fe) M-O4 bond length	2.036	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni0.5Fe0.5-THQ(Fe) M-O5 bond length	2.036	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni0.5Fe0.5-THQ(Fe) M-O6 bond length	2.086	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni0.5Fe0.5-THQ(Ni) M-O1 bond length	2.013	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni0.5Fe0.5-THQ(Ni) M-O2 bond length	2.073	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni0.5Fe0.5-THQ(Ni) M-O3 bond length	2.073	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni0.5Fe0.5-THQ(Ni) M-O4 bond length	2.013	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni0.5Fe0.5-THQ(Ni) M-O5 bond length	2.013	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni0.5Fe0.5-THQ(Ni) M-O6 bond length	2.073	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni-THQ M-O1 bond length	2.017	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni-THQ M-O2 bond length	2.064	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni-THQ M-O3 bond length	2.064	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni-THQ M-O4 bond length	2.017	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni-THQ M-O5 bond length	2.017	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3
Ni-THQ M-O6 bond length	2.064	—	—	SI Table Exact Reported	p018 · S2 Supplementary Figures and Tables · Table S3

DOS/PDOS and differential charge density

Ni0.5Fe0.5-THQ · Powder

TDOS/PDOS used to infer d-band centres and charge transfer in Ni0.5Fe0.5-THQ.

Geometry: model
Context: model systems
Measurement source: p007-p008 · 2.3 DFT Calculations · Figure 4d-f

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
d-pi conjugation charge transfer	Ni transfers part of its electrons to Fe site	—	—	Text Qualitative	p008 · 2.3 DFT Calculations · Figure 4f
Fe-THQ Fe-site d-band centre	-1.661 eV	—	—	Text Exact Reported	p008 · 2.3 DFT Calculations · Figure 4e
Ni0.5Fe0.5-THQ Fe-site d-band centreMarked as a best value within this paper	-1.551 eV	—	—	Text Exact Reported	p008 · 2.3 DFT Calculations · Figure 4e
Ni0.5Fe0.5-THQ Ni-site d-band centre	-1.708 eV	—	—	Text Exact Reported	p008 · 2.3 DFT Calculations · Figure 4e
Ni-THQ Ni-site d-band centre	-1.774 eV	—	—	Text Exact Reported	p008 · 2.3 DFT Calculations · Figure 4e
TDOS electronic states at Fermi level	many electronic states at the Fermi level	—	—	Text Qualitative	p007 · 2.3 DFT Calculations · Figure 4d

DFT/CHE OER energetics

Density functional theory

Ni0.5Fe0.5-THQ · Powder

Calculated Gibbs free energies and elementary reaction free energy changes at 1.23 V.

Temperature: 300
Geometry: model
Context: model systems
Measurement source: p019-p020 · S2 Supplementary Figures and Tables · Table S6; Table S7

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
Fe site OH- adsorption energyMarked as a best value within this paper	-0.54 eV	—	—	Text Rounded Reported	p007 · 2.3 DFT Calculations · Figure 4b
Ni site OH- adsorption energy	-0.05 eV	—	—	Text Rounded Reported	p007 · 2.3 DFT Calculations · Figure 4b
Fe-THQ DeltaG1 at 1.23 V	-0.392	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
Fe-THQ DeltaG2 at 1.23 V	-0.0196	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
Fe-THQ DeltaG3 at 1.23 V	0.458	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
Fe-THQ DeltaG4 at 1.23 V	-0.0461	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
Fe-THQ eta_theo at 1.23 V	0.458	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
Ni-THQ DeltaG1 at 1.23 V	0.11	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
Ni-THQ DeltaG2 at 1.23 V	0.0414	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
Ni-THQ DeltaG3 at 1.23 V	0.368	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
Ni-THQ DeltaG4 at 1.23 V	-0.52	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
Ni-THQ eta_theo at 1.23 V	0.368	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
NiFe-THQ(Fe-site) DeltaG1 at 1.23 V	-0.538	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
NiFe-THQ(Fe-site) DeltaG2 at 1.23 V	0.132	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
NiFe-THQ(Fe-site) DeltaG3 at 1.23 V	0.247	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
NiFe-THQ(Fe-site) DeltaG4 at 1.23 V	0.159	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
NiFe-THQ(Fe-site) eta_theo at 1.23 VMarked as a best value within this paper	0.247	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
NiFe-THQ(Ni-site) DeltaG1 at 1.23 V	-0.0505	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
NiFe-THQ(Ni-site) DeltaG2 at 1.23 V	0.536	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
NiFe-THQ(Ni-site) DeltaG3 at 1.23 V	-0.388	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
NiFe-THQ(Ni-site) DeltaG4 at 1.23 V	-0.097	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
NiFe-THQ(Ni-site) eta_theo at 1.23 V	0.536	—	—	SI Table Exact Reported	p020 · S2 Supplementary Figures and Tables · Table S7
*Fe-THQ GO**	-1113.009	—	—	SI Table Exact Reported	p019 · S2 Supplementary Figures and Tables · Table S6
*Fe-THQ GOH**	-1117.624	—	—	SI Table Exact Reported	p019 · S2 Supplementary Figures and Tables · Table S6
*Fe-THQ GOOH**	-1122.156	—	—	SI Table Exact Reported	p019 · S2 Supplementary Figures and Tables · Table S6
Fe-THQ Gsub	-1107.627	—	—	SI Table Exact Reported	p019 · S2 Supplementary Figures and Tables · Table S6
*Ni-THQ GO**	-1052.596	—	—	SI Table Exact Reported	p019 · S2 Supplementary Figures and Tables · Table S6
*Ni-THQ GOH**	-1057.272	—	—	SI Table Exact Reported	p019 · S2 Supplementary Figures and Tables · Table S6
*Ni-THQ GOOH**	-1061.833	—	—	SI Table Exact Reported	p019 · S2 Supplementary Figures and Tables · Table S6
Ni-THQ Gsub	-1047.778	—	—	SI Table Exact Reported	p019 · S2 Supplementary Figures and Tables · Table S6
*NiFe-THQ(Fe-site) GO**	-1083.754	—	—	SI Table Exact Reported	p019 · S2 Supplementary Figures and Tables · Table S6
*NiFe-THQ(Fe-site) GOH**	-1088.521	—	—	SI Table Exact Reported	p019 · S2 Supplementary Figures and Tables · Table S6
*NiFe-THQ(Fe-site) GOOH**	-1093.112	—	—	SI Table Exact Reported	p019 · S2 Supplementary Figures and Tables · Table S6
NiFe-THQ(Fe-site) Gsub	-1078.378	—	—	SI Table Exact Reported	p019 · S2 Supplementary Figures and Tables · Table S6
*NiFe-THQ(Ni-site) GO**	-1082.879	—	—	SI Table Exact Reported	p019 · S2 Supplementary Figures and Tables · Table S6
*NiFe-THQ(Ni-site) GOH**	-1088.049	—	—	SI Table Exact Reported	p019 · S2 Supplementary Figures and Tables · Table S6
*NiFe-THQ(Ni-site) GOOH**	-1092.872	—	—	SI Table Exact Reported	p019 · S2 Supplementary Figures and Tables · Table S6
NiFe-THQ(Ni-site) Gsub	-1078.394	—	—	SI Table Exact Reported	p019 · S2 Supplementary Figures and Tables · Table S6

DFT using VASP, PAW, PBE-GGA

Density functional theory

Ni0.5Fe0.5-THQ · Powder

Plane-wave cutoff 400 eV; Monkhorst-Pack 2x2x1 k-points for optimisation/SCF and 9x9x1 for DOS; residual force <0.01 eV/A; energy <1e-5 eV; z vacuum 15 A; CHE model for OER free energies.

Temperature: 300
Atmosphere: vacuum slab model
Geometry: computational model
Context: Ni0.5Fe0.5-THQ model
Measurement source: p005-p006 · S1.4 DFT calculation

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source