Lambie Stephanie, Low Jian Liang, Gaston Nicola, Paulus Beate
MacDiarmid Institute for Advanced Materials and Nanotechnology, Department of Physics, University of Auckland, Private Bag, 92019, Auckland, New Zealand.
Institut für Chemie und Biochemie, Freie Universität Berlin, Arnimallee 22, 14195, Berlin, Germany.
Chemphyschem. 2022 Apr 20;23(8):e202200024. doi: 10.1002/cphc.202200024. Epub 2022 Mar 23.
Catalysts are required to ensure electrochemical reduction of CO to fuels proceeds at industrially acceptable rates and yields. As such, highly active and selective catalysts must be developed. Herein, a density functional theory study of p-block element and noble metal doped graphene-based single-atom catalysts in two defect sites for the electrochemical reduction of CO to CO and HCOOH is systematically undertaken. It is found that on all of the systems considered, the thermodynamic product is HCOOH. Pb/C , Pb/N and Sn/C are identified as having the lowest overpotential for HCOOH production while Al/C , Al/N , Au/C and Ga/C are identified as having the potential to form higher order products due to the strength of binding of adsorbed HCOOH.
需要催化剂来确保将CO电化学还原为燃料的过程以工业上可接受的速率和产率进行。因此，必须开发高活性和高选择性的催化剂。在此，系统地开展了一项密度泛函理论研究，研究对象是p区元素和贵金属掺杂的基于石墨烯的单原子催化剂在两个缺陷位点上将CO电化学还原为CO和HCOOH的情况。研究发现，在所有考虑的体系中，热力学产物都是HCOOH。Pb/C、Pb/N和Sn/C被确定为生成HCOOH时过电位最低的体系，而Al/C、Al/N、Au/C和Ga/C由于吸附的HCOOH的结合强度而被确定有可能形成高阶产物。
