Article

Boosting CO<sub>2</sub>Electroreduction over a Cadmium Single‐Atom Catalyst by Tuning of the Axial Coordination Structure

Yahui WuBeijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences Zhongguancun North First Street 2 Beijing 100190 P. R. ChinaChunjun ChenBeijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences Zhongguancun North First Street 2 Beijing 100190 P. R. ChinaXupeng YanBeijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences Zhongguancun North First Street 2 Beijing 100190 P. R. ChinaXiaofu SunBeijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences Zhongguancun North First Street 2 Beijing 100190 P. R. ChinaQinggong ZhuBeijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences Zhongguancun North First Street 2 Beijing 100190 P. R. ChinaPengsong LiBeijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences Zhongguancun North First Street 2 Beijing 100190 P. R. ChinaYiming LiSchool of Chemistry and Chemical Engineering Southeast University Nanjing 211189 P. R. ChinaShoujie LiuChemistry and Chemical Engineering of Guangdong Laboratory Shantou 515063 ChinaJingyuan MaShanghai Synchrotron Radiation Facility, Zhangjiang Laboratory (SSRF, ZJLab) Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 ChinaYuying HuangShanghai Synchrotron Radiation Facility, Zhangjiang Laboratory (SSRF, ZJLab) Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 ChinaBuxing HanBeijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and Thermodynamics CAS Research/Education Center for Excellence in Molecular Sciences Institute of Chemistry Chinese Academy of Sciences Zhongguancun North First Street 2 Beijing 100190 P. R. China

2021en

ABI

Abstract

Abstract Guided by first‐principles calculations, it was found that Cd single‐atom catalysts (SACs) have excellent performance in activating CO 2 , and the introduction of axial coordination structure to Cd SACs cannot only further decrease the free energy barrier of CO 2 reduction, but also suppress the hydrogen evolution reaction (HER). Based on the above discovery, we designed and synthesized a novel Cd SAC that comprises an optimized CdN 4 S 1 moiety incorporated in a carbon matrix. It was shown that the catalyst exhibited outstanding performance in CO 2 electroreduction to CO. The faradaic efficiency (FE) of CO could reach up to 99.7 % with a current density of 182.2 mA cm −2 in a H‐type electrolysis cell, and the turnover frequency (TOF) value could achieve 73000 h −1 , which was much higher than that reported to date. This work shows a successful example of how to design highly efficient catalysts guided by theoretical calculations.

Identifiers

DOI: 10.1002/anie.202105263

Citations and references

Cited by 20 references

Metrics — AkademScholar