Li Junshan, Wei Ruilin, Wang Xiang, Zuo Yong, Han Xu, Arbiol Jordi, Llorca Jordi, Yang Yaoyue, Cabot Andreu, Cui Chunhua
Molecular Electrochemistry Laboratory, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, 610054, Chengdu, P. R. China.
School of Chemistry and Environment, Southwest Minzu University, 610041, Chengdu, P. R. China.
Angew Chem Int Ed Engl. 2020 Nov 16;59(47):20826-20830. doi: 10.1002/anie.202004301. Epub 2020 Sep 9.
A methanol economy will be favored by the availability of low-cost catalysts able to selectively oxidize methanol to formate. This selective oxidation would allow extraction of the largest part of the fuel energy while concurrently producing a chemical with even higher commercial value than the fuel itself. Herein, we present a highly active methanol electrooxidation catalyst based on abundant elements and with an optimized structure to simultaneously maximize interaction with the electrolyte and mobility of charge carriers. In situ infrared spectroscopy combined with nuclear magnetic resonance spectroscopy showed that branched nickel carbide particles are the first catalyst determined to have nearly 100 % electrochemical conversion of methanol to formate without generating detectable CO as a byproduct. Electrochemical kinetics analysis revealed the optimized reaction conditions and the electrode delivered excellent activities. This work provides a straightforward and cost-efficient way for the conversion of organic small molecules and the first direct evidence of a selective formate reaction pathway.
甲醇经济将因能够将甲醇选择性氧化为甲酸盐的低成本催化剂的可用性而受到青睐。这种选择性氧化将能够提取大部分燃料能量，同时生产出一种商业价值甚至高于燃料本身的化学品。在此，我们展示了一种基于丰富元素且具有优化结构的高活性甲醇电氧化催化剂，以同时最大化与电解质的相互作用和电荷载流子的迁移率。原位红外光谱与核磁共振光谱相结合表明，支链碳化镍颗粒是第一种被确定能将甲醇几乎100%电化学转化为甲酸盐且不产生可检测副产物CO的催化剂。电化学动力学分析揭示了优化的反应条件，且该电极具有出色的活性。这项工作为有机小分子的转化提供了一种直接且经济高效的方法，并首次直接证明了选择性甲酸盐反应途径。
