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Electrochemical Conversion of CO2 to Syngas with Controllable CO/H2 Ratios over Co and Ni Single-Atom Catalysts.
Angewandte Chemie International Edition ( IF 16.6 ) Pub Date : 2020-01-09 , DOI: 10.1002/anie.201912719
Qun He 1, 2 , Daobin Liu 3 , Ji Hoon Lee 2 , Yumeng Liu 2 , Zhenhua Xie 2, 4 , Sooyeon Hwang 5 , Shyam Kattel 6 , Li Song 1 , Jingguang G Chen 2, 4
Affiliation  

The electrochemical CO2 reduction reaction (CO2 RR) to yield synthesis gas (syngas, CO and H2 ) has been considered as a promising method to realize the net reduction in CO2 emission. However, it is challenging to balance the CO2 RR activity and the CO/H2 ratio. To address this issue, nitrogen-doped carbon supported single-atom catalysts are designed as electrocatalysts to produce syngas from CO2 RR. While Co and Ni single-atom catalysts are selective in producing H2 and CO, respectively, electrocatalysts containing both Co and Ni show a high syngas evolution (total current >74 mA cm-2 ) with CO/H2 ratios (0.23-2.26) that are suitable for typical downstream thermochemical reactions. Density functional theory calculations provide insights into the key intermediates on Co and Ni single-atom configurations for the H2 and CO evolution. The results present a useful case on how non-precious transition metal species can maintain high CO2 RR activity with tunable CO/H2 ratios.

中文翻译:

在Co和Ni单原子催化剂上以可控的CO / H2比将CO2电化学转化为合成气。

电化学的CO2还原反应(CO2 RR)产生合成气(合成气,CO和H2)被认为是实现CO2排放净减少的一种有前途的方法。但是,要平衡CO2 RR活性和CO / H2比具有挑战性。为了解决这个问题,设计了氮掺杂碳担载的单原子催化剂作为电催化剂,以从CO2 RR产生合成气。尽管Co和Ni单原子催化剂分别具有选择性生产H2和CO的能力,但同时包含Co和Ni的电催化剂显示出高的合成气逸出度(总电流> 74 mA cm-2),且CO / H2比为(0.23-2.26),适用于典型的下游热化学反应。密度泛函理论计算提供了有关H和CO逸出的Co和Ni单原子构型的关键中间体的见识。
更新日期:2020-01-10
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