Yang Siwei, Lyu Lingshan, Zhao Chaoyu, Liu Huiling, Huang Xuri
Laboratory of Theoretical and Computational Chemistry, Institute of Theoretical Chemistry, Jilin University, Liutiao Road 2, Changchun 130023, China.
Langmuir. 2021 Jan 12;37(1):428-436. doi: 10.1021/acs.langmuir.0c03080. Epub 2020 Dec 23.
In recent years, one of the research directions of proton-exchange membrane fuel cells (PEMFCs) was to exploit efficient electrocatalysts for oxygen reduction reaction (ORR) instead of precious metals. In this study, on the basis of the density-functional theory (DFT) calculations, we designed a new type of single-atom ORR electrocatalyst by doping single iron atoms into the N-coordination cavity of the substrate graphite carbonitride (Fe/g-CN). The adsorption site and the adsorption energy of all the intermediates, the reaction energy barriers, potential energy surface, and Mulliken charges have been analyzed. The feasible ORR reaction paths and the most favorable ORR reaction mechanism were performed. Our calculation results prove that Fe/g-CN is a potential electrocatalyst toward ORR. This work proposes a novel notion for the development of cathode materials in PEMFCs.
近年来，质子交换膜燃料电池（PEMFCs）的研究方向之一是开发用于氧还原反应（ORR）的高效电催化剂以替代贵金属。在本研究中，基于密度泛函理论（DFT）计算，我们通过将单个铁原子掺杂到基底石墨碳氮化物（Fe/g-CN）的N配位空腔中，设计了一种新型单原子ORR电催化剂。分析了所有中间体的吸附位点和吸附能、反应能垒、势能面和穆利肯电荷。研究了可行的ORR反应路径和最有利的ORR反应机理。我们的计算结果证明Fe/g-CN是一种潜在的ORR电催化剂。这项工作为PEMFCs中阴极材料的开发提出了一个新的概念。
