Department of Chemistry , University of Illinois at Urbana-Champaign , Urbana , Illinois 61801 , United States.
Graduate University of Science and Technology , Vietnam Academy of Science and Technology , Hanoi , Vietnam.
J Am Chem Soc. 2018 May 2;140(17):5791-5797. doi: 10.1021/jacs.8b01868. Epub 2018 Apr 17.
Electrodeposition of CuAg alloy films from plating baths containing 3,5-diamino-1,2,4-triazole (DAT) as an inhibitor yields high surface area catalysts for the active and selective electroreduction of CO to multicarbon hydrocarbons and oxygenates. EXAFS shows the co-deposited alloy film to be homogeneously mixed. The alloy film containing 6% Ag exhibits the best CO electroreduction performance, with the Faradaic efficiency for CH and CHOH production reaching nearly 60 and 25%, respectively, at a cathode potential of just -0.7 V vs RHE and a total current density of ∼ - 300 mA/cm. Such high levels of selectivity at high activity and low applied potential are the highest reported to date. In situ Raman and electroanalysis studies suggest the origin of the high selectivity toward C products to be a combined effect of the enhanced stabilization of the CuO overlayer and the optimal availability of the CO intermediate due to the Ag incorporated in the alloy.
从含有 3,5-二氨基-1,2,4-三唑 (DAT) 的电镀液中电沉积 CuAg 合金膜可得到高比表面积的催化剂，用于 CO 的活性和选择性电还原为多碳烃和含氧化合物。EXAFS 表明共沉积的合金膜均匀混合。含有 6%Ag 的合金膜表现出最佳的 CO 电还原性能，在阴极电位仅为-0.7 V vs RHE 和总电流密度约为-300 mA/cm 时，CH 和 CHOH 的法拉第效率分别达到近 60%和 25%。在高活性和低应用电位下实现如此高的选择性水平是迄今为止报道的最高水平。原位拉曼和电化学分析研究表明，对 C 产物高选择性的起源是由于合金中掺入 Ag 导致 CuO 覆盖层的增强稳定性和 CO 中间产物的最佳可用性的综合作用。
