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

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Stability and Catalytic Performance of Single-Atom Catalysts Supported on Doped and Defective Graphene for CO2 Hydrogenation to Formic Acid: A First-Principles Study
ACS Applied Nano Materials ( IF 5.3 ) Pub Date : 2021-06-22 , DOI: 10.1021/acsanm.1c00959
Sajjad Ali _{1,

2} , Rashid Iqbal ₃ , Azim Khan ₂ , Shafiq Ur Rehman ₄ , Muhammad Haneef ₅ , Lichang Yin ₂

Affiliation

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 H₂ and CO₂ on SACs/m-VacG (path A) and H₂ 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.

中文翻译：

掺杂和缺陷石墨烯负载的单原子催化剂在 CO2 加氢制甲酸中的稳定性和催化性能：第一性原理研究

作为单原子催化剂的重要组成部分，载体材料决定了单个金属原子的分散、利用和稳定性。在这里，我们报告了有缺陷和掺杂的石墨烯作为 CO ₂单原子催化剂 (SAC) 载体的潜力加氢转化为甲酸。基于单金属原子的稳定性筛选支撑效应。我们的计算表明，在单空位缺陷石墨烯 (m-VacG) 上负载的 Cu、Pd 和 Ru 的吸附能高于其本体对应物的内聚能；因此，我们选择了 m-VacG 上负载的 Cu、Pd 和 Ru 作为潜在的 SAC 来检查催化反应。分子动力学 (MD) 模拟、迁移势垒计算和电子结构分析揭示了 SACs/m-VacG 的稳定性和反应性。CO ₂加氢反应从不同的初始状态开始通过两条途径进行，即H ₂和CO ₂在SACs/m-VacG（路径A）和H _{2 上的}共吸附SACs/m-VacG 上的吸附（路径 B）。从反应路径分析，发现路径 B 在热力学上占主导地位，与路径 A 相比，具有更低的能垒。此外，预计 m-VacG 上负载的 Pd 是最高活性的 SAC，沿反应的能垒最低小路。

更新日期：2021-07-23

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