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Lowering C−C coupling barriers for efficient electrochemical CO2 reduction to C2H4 by jointly engineering single Bi atoms and oxygen vacancies on CuO
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2022-08-10 , DOI: 10.1016/j.apcatb.2022.121823
Wenjie Li , Lifen Li , Qineng Xia , Song Hong , Lijun Wang , Zhibo Yao , Tai-Sing Wu , Yun-Liang Soo , Hao Zhang , Tsz Woon Benedict Lo , Alex W. Robertson , Qingya Liu , Leiduan Hao , Zhenyu Sun

Electrochemical CO2 reduction (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 C2H4 by decreasing C–C coupling barriers. The overpotential for C2H4 production 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 CO2 adsorption and lowers C–C coupling energy barriers, thereby improving the C2H4 selectivity.



中文翻译:

通过在 CuO 上联合设计单个 Bi 原子和氧空位来降低 C-C 耦合势垒,以有效地将 CO2 电化学还原为 C2H4

将电化学 CO 2还原 (ECR) 转化为商品化学品为减轻温室效应和推动从依赖化石燃料向可持续经济转型提供了一种有前景的方法。为此,设计和开发活性强的电催化剂是关键。在这里,我们首次报道了在有缺陷的 CuO 上掺入铋 (Bi) 单原子可以通过降低 C-C 耦合势垒显着增强对 C 2 H 4的 ECR 反应。C 2 H 4产生的过电位至少降低了 50 mV,同时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 小时后仍能保持高性能。控制实验以及密度泛函理论计算表明,Bi 和氧空位的联合掺入极大地促进了 CO 2的吸附并降低了 C-C 耦合能垒,从而提高了 C 2 H 4的选择性。

更新日期:2022-08-10
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