Binary alloys for electrocatalytic CO2 conversion to hydrocarbons and alcohols
Binary alloys for electrocatalytic CO2 conversion to hydrocarbons and alcohols
复制标题
DOI：
10.1016/j.apsusc.2023.157734
复制
发表时间：
2023-10
影响因子：
6.7
通讯作者：
Dai-Jian Su;Shi-Qin Xiang;Yimin Jiang;Xiao-hong Liu;W. Zhang;Liu Zhao
中科院分区：
文献类型：
--
作者：
Dai-Jian Su;Shi-Qin Xiang;Yimin Jiang;Xiao-hong Liu;W. Zhang;Liu Zhao
双金属合金有望通过电子和表面结构的调节，创造出单金属催化剂无法实现的优越催化性能。本文采用DFT计算方法研究了9种ⅠB族金属二元合金的电化学co2转化反应机理和催化动力学。在不同的双金属催化剂上，通过控制单键h键形成、单键h键形成和单键dc偶联的反应动力学，可以产生从CO到CO-beyond产物、从c1到c2碳氢化合物和醇的各种还原产物。在所研究的二元合金中，Au-Ag合金对单质Au和Ag的CO生成能力较强。cu1 / 4au3 /4在促进CORR活性的同时抑制HER副反应，催化co2转化为甲烷和甲醇的性能最好。通过调整COH*中间体的CORR通路，降低了cu3 / 4ag1 /4和cu3 / 4au1 /4催化剂的c单键dc偶联势垒，从而提供了催化co2转化为c2产物的潜在能力。
Bimetallic alloys are expected to create superior catalytic performance that cannot be achieved on monometallic catalysts by regulations of both electronic and surface structures. In this work, the reaction mechanism and catalytic kinetics of electrochemical CO2conversion on nine ⅠB group metal binary alloys are studied by using DFT computations. Various reduction products, from CO to CO-beyond products and from C1to C2hydrocarbons and alcohols, can be produced on different bimetallic catalysts by controlling their reaction kinetics of competing Osingle bondH bond formation, Csingle bondH bond formation, and Csingle bondC coupling. Among all the studied binary alloys, Au-Ag alloys show enhanced CO production ability with respect to elemental Au and Ag. Cu1/4Au3/4gives the best performance to catalyze CO2conversion to methane and methanol as a result of simultaneously promoting CORR activity and suppressing HER side reaction. By adjusting the CORR pathway through COH* intermediate, the Csingle bondC coupling barriers are lowered on Cu3/4Ag1/4and Cu3/4Au1/4catalysts, which deliver potential capacity to catalyze CO2transformation to C2products.