CO<sub>2</sub> electroreduction on single atom catalysts: the role of the DFT functional

Misra, Debolina; Di Liberto, Giovanni; Pacchioni, Gianfranco

doi:10.1039/d4cp00175c

Phys. Chem. Chem. Phys.

2024

DOI: 10.1039/d4cp00175c

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CO₂ electroreduction on single atom catalysts: the role of the DFT functional

Debolina Misra,

Giovanni Di Liberto,

Gianfranco Pacchioni

Abstract: One key process with Single Atom Catalysts (SACs) is the electroreduction of CO2 to fuels. The chemistry of SACs differs largely from that of extended catalytic surfaces, and this represents...

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Cited by 7 publications

References 101 publications

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Electrochemical Nitrogen Reduction Reaction from Ab Initio Thermodynamics: Single versus Dual Atom Catalysts

Barlocco,

Spotti,

Liberto

et al. 2024

Advcd Theory and Sims

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The electrochemical nitrogen reduction reaction (NRR) is a key process for the energy transition. Transition metal atoms atomically dispersed on a solid support represent a promising approach to the design of new catalytic materials. The interest for single‐ (SACs) and dual‐atom catalysts (DACs) is steadily growing. In general, DACs are considered more active than SACs for NRR. In this work, the complex chemistry behind NRR is investigated on a set of SACs and DACs by means of density functional theory (DFT) calculations. The results indicate that self‐interaction corrected exchange‐correlation functionals must be adopted, at variance with several studies in the literature. Furthermore, it is not possible to extrapolate results obtained on conventional extended catalytic surfaces to SACs and DACs, due to a richer scenario of possible reaction paths. In general, the results show a positive effect on the catalytic activity moving from 3d to 5d metals, and from SACs and DACs. However, if the two effects work together, that is, 5d metals in DACs, the reaction intermediates may be too strongly bound, thus resulting in reduced catalytic activity. In this respect, the fact that DACs are expected to be superior to SACs in NRR is not always verified.

show abstract

Electrochemical Nitrogen Reduction Reaction from Ab Initio Thermodynamics: Single versus Dual Atom Catalysts

Barlocco,

Spotti,

Liberto

et al. 2024

Advcd Theory and Sims

View full text Add to dashboard Cite

show abstract

Key Ingredients for the Screening of Single Atom Catalysts for the Hydrogen Evolution Reaction: The Case of Titanium Nitride

Saetta,

Barlocco,

Liberto

et al. 2024

Small

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A computational screening of Single Atom Catalysts (SACs) bound to titanium nitride (TiN) is presented, for the Hydrogen Evolution Reaction (HER), based on density functional theory. The role of fundamental ingredients is explored to account for a reliable screening of SACs. Namely, the formation of H2‐complexes besides the classical H* one impacts the predicted HER activity, in line with previous studies on other SACs. Also, the results indicate that one needs to adopt self‐interaction‐corrected functionals. Finally, predicting an active catalyst is of little help without an assessment of its stability. Thus, it is included in the theoretical framework the analysis of the stability of the SACs in working conditions of pH and voltage. Once unconventional intermediates and stability are considered in a self‐interaction corrected scheme, the number of potential good catalysts for HER is strongly reduced since i) some potentially good catalysts are not stable against dissolution and ii) the formation of unconventional intermediates leads to thermodynamic barriers. This study highlights the importance of including ingredients for the prediction of new systems, such as the formation of unconventional intermediates, estimating the stability of SACs, and the adoption of self‐interaction corrected functionals. Also, this study highlights some interesting candidates deserving of dedicated work.

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CO2 electroreduction on single atom catalysts: Role of the local coordination

Emken,

Liberto,

Pacchioni

2024

Electrochimica Acta

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CO₂ electroreduction on single atom catalysts: the role of the DFT functional

Abstract: One key process with Single Atom Catalysts (SACs) is the electroreduction of CO2 to fuels. The chemistry of SACs differs largely from that of extended catalytic surfaces, and this represents...

Cited by 7 publications

References 101 publications

Electrochemical Nitrogen Reduction Reaction from Ab Initio Thermodynamics: Single versus Dual Atom Catalysts

Electrochemical Nitrogen Reduction Reaction from Ab Initio Thermodynamics: Single versus Dual Atom Catalysts

Key Ingredients for the Screening of Single Atom Catalysts for the Hydrogen Evolution Reaction: The Case of Titanium Nitride

CO2 electroreduction on single atom catalysts: Role of the local coordination

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CO2 electroreduction on single atom catalysts: the role of the DFT functional

Abstract: One key process with Single Atom Catalysts (SACs) is the electroreduction of CO2 to fuels. The chemistry of SACs differs largely from that of extended catalytic surfaces, and this represents...

Cited by 7 publications

References 101 publications

Electrochemical Nitrogen Reduction Reaction from Ab Initio Thermodynamics: Single versus Dual Atom Catalysts

Electrochemical Nitrogen Reduction Reaction from Ab Initio Thermodynamics: Single versus Dual Atom Catalysts

Key Ingredients for the Screening of Single Atom Catalysts for the Hydrogen Evolution Reaction: The Case of Titanium Nitride

CO2 electroreduction on single atom catalysts: Role of the local coordination

Contact Info

Product

Resources

About

CO₂ electroreduction on single atom catalysts: the role of the DFT functional