William G. Lowrie Department of Chemical & Biomolecular Engineering, The Ohio State University, 221A Koffolt Laboratories, 140 West 19th Ave., Columbus, OH 43210, USA.
Angew Chem Int Ed Engl. 2013 Feb 25;52(9):2459-62. doi: 10.1002/anie.201208320. Epub 2013 Jan 23.
On the right path: Based on DFT calculations (incorporating the role of water solvation) of the activation barriers of elementary steps, a new path that leads to methane and ethylene for CO(2) electroreduction on Cu(111) was identified. Methane formation proceeds through reduction of CO to COH (path II, see picture), which leads to CH(x) species that can produce both methane and ethylene, as observed experimentally.
基于对基本步骤的激活障碍的 DFT 计算（包括水溶剂化的作用），确定了一条新的路径，该路径可导致 CO(2)在 Cu(111)上的电化学还原生成甲烷和乙烯。甲烷的形成是通过将 CO 还原为 COH（路径 II，见图片）进行的，这导致可以生成甲烷和乙烯的 CH(x)物种，这与实验观察到的结果一致。
