A Few Questions about Single-Atom Catalysts: When Modeling Helps DOI Creative Commons
Giovanni Di Liberto, Sergio Tosoni, Luis A. Cipriano

et al.

Accounts of Materials Research, Journal Year: 2022, Volume and Issue: 3(9), P. 986 - 995

Published: Aug. 11, 2022

ConspectusSingle-atom catalysis (SAC) is a fascinating and rapidly growing field in heterogeneous catalysis. In less than 20 years, this has become one of the most widely investigated subjects by catalytic community for various good reasons: ability to synthesize active catalysts using minimum amount precious metals, expected higher selectivity SACs compared assemblies nanoparticles variable sizes, fact that represent bridge between homogeneous The relative simplicity SAC structures classical based on supported metal stimulated an intense simulation activity aimed at predicting new potential from first principles, often machine learning algorithms. This very ambitious objective ultimately represents final goal every modeling activity: possibility provide realistic predictions material properties reactivity. However, main reasons theory useful remains interpretation analysis experimental results, with no crucial understanding basic principles determine certain functionality or combination advanced characterization techniques theoretical calculations can general conceptual framework better understand structure–function relationships. Account, we will address aspect trying answers some fundamental questions related structure, stability, SACs. We start addressing question arises time synthesized: where are atoms? What their coordination mode support? Once have shown how point, move next question: do single atoms stay put? How does chemical environment depend preparation reaction conditions? Next, analyze importance full mechanism predict SACs, due analogy compounds, form intermediates not exist surface electrodes. formation these influence kinetics process must be considered simulation. Finally, briefly more compare corresponding hand molecular complexes other? message answer take advantage quantum modeling, results should continuously verified data cross-fertilization beneficial both sides.

Language: Английский

Ligand engineering regulates the electronic structure of Ni-N-C sites to promote electrocatalytic acetylene semi-hydrogenation DOI
Kai Xu, Mingqiang Liu,

Xiaohong Song

et al.

Journal of Catalysis, Journal Year: 2024, Volume and Issue: unknown, P. 115784 - 115784

Published: Oct. 1, 2024

Language: Английский

Citations

8
Theoretical insights on potential-dependent oxidation behaviors and antioxidant strategies of MXenes DOI Creative Commons
Yumiao Tian, Pengfei Hou,

H.Y. Zhang

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Nov. 21, 2024

Significant efforts have been devoted to investigating the oxidation of MXenes in various environments. However, underlying mechanism MXene and its dependence on electrode potential remain poorly understood. Here we show behavior under working conditions electrochemical processes terms kinetics thermodynamics by using constant-potential ab initio simulations. The theoretical results indicate that effects can be attributed nucleophilic attack water molecules metal atoms, similar taking place Oxygen Evolution Reaction. Building upon these findings, deduced common MXenes, proposed antioxidant strategies for MXene. Finally, demonstrated MBenes, boron analogs may undergo a inferred molecule-induced Walden inversion is widely present material reconstructions. This work contributes fundamental understanding stability at atomic level, promotes transition materials discovery from trial-and-error synthesis rational design. are two-dimensional with promising applications, but their mechanisms Here, authors use simulations investigate how influenced potential.

Language: Английский

Citations

7
In-situ N-defect and single-metal atom synergetic engineering of high-efficiency Ag–N–C electrocatalysts for CO2 reduction DOI
Luliang Liao, Guomin Xia, Yigang Wang

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 318, P. 121826 - 121826

Published: Aug. 6, 2022

Language: Английский

Citations

26
Understanding the water molecule effect in metal-free B-based electrocatalysts for electrochemical CO2 reduction DOI

Yuxiao Meng,

Zhangmeng Xu,

Zhangfeng Shen

et al.

Journal of Materials Chemistry A, Journal Year: 2022, Volume and Issue: 10(12), P. 6508 - 6522

Published: Jan. 1, 2022

Electrocatalytic CO 2 reduction (CO RR) is a feasible and economical way to eliminate via converting it into useful products.

Language: Английский

Citations

25
A Few Questions about Single-Atom Catalysts: When Modeling Helps DOI Creative Commons
Giovanni Di Liberto, Sergio Tosoni, Luis A. Cipriano

et al.

Accounts of Materials Research, Journal Year: 2022, Volume and Issue: 3(9), P. 986 - 995

Published: Aug. 11, 2022

ConspectusSingle-atom catalysis (SAC) is a fascinating and rapidly growing field in heterogeneous catalysis. In less than 20 years, this has become one of the most widely investigated subjects by catalytic community for various good reasons: ability to synthesize active catalysts using minimum amount precious metals, expected higher selectivity SACs compared assemblies nanoparticles variable sizes, fact that represent bridge between homogeneous The relative simplicity SAC structures classical based on supported metal stimulated an intense simulation activity aimed at predicting new potential from first principles, often machine learning algorithms. This very ambitious objective ultimately represents final goal every modeling activity: possibility provide realistic predictions material properties reactivity. However, main reasons theory useful remains interpretation analysis experimental results, with no crucial understanding basic principles determine certain functionality or combination advanced characterization techniques theoretical calculations can general conceptual framework better understand structure–function relationships. Account, we will address aspect trying answers some fundamental questions related structure, stability, SACs. We start addressing question arises time synthesized: where are atoms? What their coordination mode support? Once have shown how point, move next question: do single atoms stay put? How does chemical environment depend preparation reaction conditions? Next, analyze importance full mechanism predict SACs, due analogy compounds, form intermediates not exist surface electrodes. formation these influence kinetics process must be considered simulation. Finally, briefly more compare corresponding hand molecular complexes other? message answer take advantage quantum modeling, results should continuously verified data cross-fertilization beneficial both sides.

Language: Английский

Citations

24