Computational Modelling — A Computation-Guided Design of Highly Defined and Dense Bimetallic Active Sites on a Two-Dimensional Conductive Metal–Organic Framework for Efficient H2O2 Electrosynthesis

Measurement evidence

Computational Modelling

A Computation-Guided Design of Highly Defined and Dense Bimetallic Active Sites on a Two-Dimensional Conductive Metal–Organic Framework for Efficient H2O2 Electrosynthesis · Li Z., Jia J., Sang Z. et al. · Angewandte Chemie - International Edition · 2024 · e202408500

2 measurement groups · 17 results

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

slow-growth AIMD explicit solvation

Molecular dynamics

M2-TCPP(Co) DFT supercell set · Model

48 H2O molecules, NVT, 300 K, time step 0.5 fs, 0.0005 A per AIMD step

Temperature: 300
Context: model_system
Measurement source: S9 · DFT Methods

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
2e-ORR barrier by Co-O bond breakingMarked as a best value within this paper	ΔG = 0.96 eV	—	—	Text Rounded Reported	8 · Figure 5 discussion · Figure 5e
2e-ORR barrier by Ni-O bond breakingMarked as a best value within this paper	ΔG = 1.00 eV	—	—	Text Rounded Reported	8 · Figure 5 discussion · Figure 5b
4e-ORR O-O cleavage barrier at site A	ΔG = 1.10 eV	—	—	Text Rounded Reported	8 · Figure 5 discussion · Figure 5c
4e-ORR O-O cleavage barrier at site B	ΔG = 1.84 eV	—	—	Text Rounded Reported	8 · Figure 5 discussion · Figure 5f

DFT screening; VASP, PAW, PBE-GGA, DFT-D3

Density functional theory

M2-TCPP(Co) DFT supercell set · Model

M2-TCPP(Co) and TCPP(M1) models; cutoff 400 eV; force 0.02 eV/A; energy 1e-6 eV

Temperature: 298.15
Context: model_system
Measurement source: S8 · DFT Methods

Property	Reported value	Normalised value	Uncertainty	Origin and quality	Source
Bader charge Co-TCPP(Co) Co site	0.34 \|e\|	—	—	SI Table Exact Reported	S35 · Supplementary Tables · Table S1
Bader charge Cu-TCPP(Co) Cu site	0.13 \|e\|	—	—	SI Table Exact Reported	S35 · Supplementary Tables · Table S1
Bader charge Fe-TCPP(Co) Fe site	0.38 \|e\|	—	—	SI Table Exact Reported	S35 · Supplementary Tables · Table S1
Bader charge Mn-TCPP(Co) Mn site	0.42 \|e\|	—	—	SI Table Exact Reported	S35 · Supplementary Tables · Table S1
Bader charge Ni-TCPP(Co) Ni site	0.25 \|e\|	—	—	SI Table Exact Reported	S35 · Supplementary Tables · Table S1
Bader charge Ni-TCPP(Co) TCPP(Co) site	0.33 \|e\|	—	—	SI Table Exact Reported	S35 · Supplementary Tables · Table S1
CoN4 site recalculated adsorption energy	4.1 eV	—	—	Text Rounded Reported	2 · DFT Screening · Figure S3
formation energy range for M2-TCPP(Co)	from -1.66 to -9.88 eV	—	—	Text Range	2 · DFT Screening · Figure 1c
site A-site B distance	~1.19 nm	—	—	Text Approximate	2 · DFT Screening
Ni2O8 d-band centre	-1.76 eV	—	—	Text Rounded Reported	3 · DFT Screening · Figure 1e
*Ni2O8 site ΔGOOH**Marked as a best value within this paper	exactly 4.23 eV	—	—	Text Rounded Reported	2 · DFT Screening · Figure 1d
PDOS crosses Fermi level	PDOS plots of both M2-TCPP(Co) sites crossed epsilon = 0; intrinsically high electronic conductivity (metallicity)	—	—	Qualitative Qualitative	3 · DFT Screening · Figure 1e; Figure S4
*TCPP(Co) site ΔGOOH**Marked as a best value within this paper	4.09 eV at U = 0 V	—	—	Text Rounded Reported	2 · DFT Screening · Figure 1b