中国科学技术大学江俊团队报道了层间电荷转移调节电子/石墨烯2D异质结的单原子催化活性。相关研究成果发表在2023年2月17日出版的《美国化学会杂志》。

具有结构和活性可调的单原子催化剂在能源和环境应用中引起了极大的关注。

该文中，研究人员报道了二维石墨烯和电异质结构上单原子催化的第一原理研究。带电层中的负离子电子气体能够向石墨烯层进行巨大的电子转移，转移程度可通过选择带电层来控制。电荷转移调节了单个金属原子的d轨道电子占有率，增强了析氢反应和氧还原反应的催化活性。吸附能Eads与电荷变化Δq之间的强相关性表明，界面电荷转移是异质结构基催化剂的关键催化描述符。多项式回归模型证明了电荷转移的重要性，并准确预测了离子和分子的吸附能。

该研究提供了一种利用二维异质结构获得高效单原子催化剂的策略。

附：英文原文

Title: Interlayer Charge Transfer Regulates Single-Atom Catalytic Activity on Electride/Graphene 2D Heterojunctions

Author: Wei Li, Cong Liu, Chenkai Gu, Jin-Ho Choi, Song Wang, Jun Jiang

Issue&Volume: February 17, 2023

Abstract: Single-atom catalysts with structure and activity tunability have attracted significant attention for energy and environmental applications. Herein we present a first-principles study of single-atom catalysis on two-dimensional graphene and electride heterostructures. The anion electron gas in the electride layer enables a colossal electron transfer to the graphene layer, with the degree of transfer being controllable by the selection of electride. The charge transfer tunes the d-orbital electron occupancy of a single metal atom, enhancing the catalytic activity of hydrogen evolution reactions and oxygen reduction reactions. The strong correlation between the adsorption energy Eads and the charge variation Δq suggests that interfacial charge transfer is a critical catalytic descriptor for the heterostructure-based catalysts. The polynomial regression model proves the importance of charge transfer and accurately predicts the adsorption energy of ions and molecules. This study provides a strategy to obtain high-efficiency single-atom catalysts using two-dimensional heterostructures.

DOI: 10.1021/jacs.2c13596

Source: https://pubs.acs.org/doi/10.1021/jacs.2c13596