4.7 Article

Stability and Catalytic Performance of Single-Atom Catalysts Supported on Doped and Defective Graphene for CO2 Hydrogenation to Formic Acid: A First-Principles Study

期刊

ACS APPLIED NANO MATERIALS
卷 4, 期 7, 页码 6893-6902

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acsanm.1c00959

关键词

single-atom catalysts; doped and defective carbon; CO2 hydrogenation; formic acid; density functional theory

资金

  1. Southern University of Science and Technology, Shenzhen, China
  2. National Natural Science Foundation of China (NSFC) [51972312]
  3. China Postdoc Council

向作者/读者索取更多资源

Support materials play a crucial role in determining the dispersion, utilization, and stability of single metal atoms as part of single-atom catalysts. Defective and doped graphene was explored as a potential support for CO2 conversion to formic acid by having higher adsorption energy for Cu, Pd, and Ru supported on it. Path B, involving H2 adsorption on the support material, was found to dominate the CO2 hydrogenation reaction with lower energy barriers, especially in the case of Pd supported on defective graphene.
As an essential component of single-atom catalysts, support materials determine the dispersion, utilization, and stability of single metal atoms. Here, we reported the potential of defective and doped graphene as a single-atom catalyst (SAC) support for CO2 conversion to formic acid by hydrogenation. The support effect was screened based on the stability of a single-metal atom. Our calculation revealed that Cu, Pd, and Ru supported on defective graphene with monovacancy (m-VacG) have higher adsorption energy than the cohesive energy of their bulk counterparts; therefore we selected Cu, Pd, and Ru supported on m-VacG as potential SACs to examine the catalytic reaction. The stability and reactivity of SACs/ m-VacG were uncovered by molecular dynamics (MD) simulations, migration barrier calculation, and electronic structure analysis. The reaction of CO2 hydrogenation proceeds through two pathways starting from different initial states, i.e., the coadsorption of H-2 and CO2 on SACs/m-VacG (path A) and H-2 adsorption on SACs/m-VacG (path B). From the reaction pathways analysis, it is found that path B dominates the entire reaction thermodynamically with lower energy barrier compared with path A. Moreover, Pd supported on m-VacG is predicted to be the highest active SAC with the lowest energy barrier along the reaction path.

作者

我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。

评论

主要评分

4.7
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

暂无数据
暂无数据