Charge State Dependence of Phase Transition Catalysis of Dynamic Cu Clusters in CO2 DissociationClick to copy article linkArticle link copied!
- Qi-Yuan FanQi-Yuan FanState Key Laboratory of Physical Chemistry of Solid Surface, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, ChinaMore by Qi-Yuan Fan
- Zhong-Hao ShiZhong-Hao ShiState Key Laboratory of Physical Chemistry of Solid Surface, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, ChinaMore by Zhong-Hao Shi
- Ye WangYe WangState Key Laboratory of Physical Chemistry of Solid Surface, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, ChinaMore by Ye Wang
- Jun Cheng*Jun Cheng*E-mail: [email protected]State Key Laboratory of Physical Chemistry of Solid Surface, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, ChinaMore by Jun Cheng
Abstract

The reactivity of subnanometer cluster catalysts depends on their charge state and dynamical evolutions of configurations under reaction environments. There have been some studies on how the dynamic configurational evolutions of neutral clusters influence their catalytic performances. However, there is little work on the charge state sensitivity of dynamic effects of metal clusters. In the present work, we investigate the dynamic process of CO2 dissociation on negatively and positively charged Cu13 clusters and calculate the reaction free energy profiles using ab initio molecular dynamics. It is interesting to find that the reaction entropies are charge sensitive and show a different temperature dependence as compared to their neutral counterpart. In contrast to the single peaked shape shown in the neutral Cu13 cluster, the entropy curves of the charged clusters exhibit an abnormal pulse shape. Further analysis indicates that such nontrivial entropy curves can be attributable to the adsorption-induced solid-to-liquid phase transitions of the charged clusters under finite temperature conditions. Our work reveals a complex temperature dependence of the chemical reaction on the charge state of the metal cluster.
Cited By
Smart citations by scite.ai include citation statements extracted from the full text of the citing article. The number of the statements may be higher than the number of citations provided by ACS Publications if one paper cites another multiple times or lower if scite has not yet processed some of the citing articles.
This article is cited by 6 publications.
- Yun-Pei Liu, Qi-Yuan Fan, Fu-Qiang Gong, Jun Cheng. CatFlow: An Automated Workflow for Training Machine Learning Potentials to Compute Free Energies in Dynamic Catalysis. The Journal of Physical Chemistry C 2025, 129
(2)
, 1089-1102. https://doi.org/10.1021/acs.jpcc.4c05568
- Qi-Yuan Fan, Fu-Qiang Gong, Yun-Pei Liu, Hao-Xuan Zhu, Jun Cheng. Modeling Dynamic Catalysis at ab Initio Accuracy: The Need for Free-Energy Calculation. ACS Catalysis 2024, 14
(21)
, 16086-16097. https://doi.org/10.1021/acscatal.4c05372
- Jian-Feng Li, Jinlong Yang, Qiang Fu. The Journal of Physical Chemistry C Virtual Special Issue on “Energy and Catalysis in China”. The Journal of Physical Chemistry C 2022, 126
(5)
, 2301-2306. https://doi.org/10.1021/acs.jpcc.2c00111
- Fu‐Qiang Gong, Yun‐Pei Liu, Ye Wang, Weinan E, Zhong‐Qun Tian, Jun Cheng. Machine Learning Molecular Dynamics Shows Anomalous Entropic Effect on Catalysis through Surface Pre‐melting of Nanoclusters. Angewandte Chemie 2024, 136
(27)
https://doi.org/10.1002/ange.202405379
- Fu‐Qiang Gong, Yun‐Pei Liu, Ye Wang, Weinan E, Zhong‐Qun Tian, Jun Cheng. Machine Learning Molecular Dynamics Shows Anomalous Entropic Effect on Catalysis through Surface Pre‐melting of Nanoclusters. Angewandte Chemie International Edition 2024, 63
(27)
https://doi.org/10.1002/anie.202405379
- Juan-Juan Sun, Qi-Yuan Fan, Xin Jin, Jing-Li Liu, Tong-Tong Liu, Bin Ren, Jun Cheng. Size-dependent phase transitions boost catalytic activity of sub-nanometer gold clusters. The Journal of Chemical Physics 2022, 156
(14)
https://doi.org/10.1063/5.0084165
Article Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.
Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.
The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated.