Lowering C−C coupling barriers for efficient electrochemical CO2 reduction to C2H4 by jointly engineering single Bi atoms and oxygen vacancies on CuO
Lowering C−C coupling barriers for efficient electrochemical CO2 reduction to C2H4 by jointly engineering single Bi atoms and oxygen vacancies on CuO
复制标题
DOI：
10.1016/j.apcatb.2022.121823
复制
发表时间：
2022-08
期刊：
影响因子：
--
通讯作者：
Wenjie Li;Lifen Li;Qineng Xia;Song Hong;Lijun Wang;Zhibo Yao;Tai‐Sing Wu;Y. Soo;Hao Zhang-Hao-Z
中科院分区：
文献类型：
--
作者：
Wenjie Li;Lifen Li;Qineng Xia;Song Hong;Lijun Wang;Zhibo Yao;Tai‐Sing Wu;Y. Soo;Hao Zhang-Hao-Z
电化学CO2还原（ECR）为商品化学品提供了一种有前途的方法，可以减轻温室效应，并推动从化石燃料依赖到可持续经济的转变。为此，设计和开发活性和耐用的电催化剂是关键。在这里，我们报告的第一次，纳入铋（Bi）单原子缺陷CuO可以显着提高ECR反应C2 H4通过降低C-C耦合势垒。C2 H4生产的过电位降低了至少50 mV，沿着法拉第效率提高了两倍，在400 mA cm-2时达到60%。即使在连续电解20小时后也保持高性能。对照实验沿着的密度泛函理论计算表明，Bi和氧空位的共同引入极大地促进了CO2的吸附，降低了C-C耦合能垒，从而提高了C2 H4的选择性.
Electrochemical CO2reduction (ECR) to commodity chemicals offers a promising way for mitigating the greenhouse effect and driving the transition from fossil-fuel dependence to a sustainable economy. To this end, the design and development of active and robust electrocatalysts is key. Here we report for the first time that incorporation of bismuth (Bi) single atoms on defective CuO could significantly enhance the ECR reaction to C2H4by decreasing C–C coupling barriers. The overpotential for C2H4production is lowered by at least 50 mV, along with a two-fold improvement in the faradaic efficiency, reaching 60% at 400 mA cm−2. The high performance is maintained even after 20 h of consecutive electrolysis. Control experiments along with density functional theory calculations suggest that the joint incorporation of Bi and oxygen vacancies greatly promotes CO2adsorption and lowers C–C coupling energy barriers, thereby improving the C2H4selectivity.