Vacancy‐Defect Single‐Atom Catalysts for Tandem CO <sub>2</sub> Electroreduction and Carbonylation Reactions from Flue Gas

Q Qiu‐Ping Zhao (Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China) W Wen‐Xiong Shi (Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China) B Bo Wang Z Zuo‐Shu Sun (State Key Laboratory of Crystal Materials, Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science &amp; Engineering Tianjin University of Technology Tianjin 300384 China) S Shuang Yao (Department of Otolaryngology Head and Neck Surgery, Beijing Tongren Hospital) T Tong‐Bu Lu (State Key Laboratory of Crystal Materials Tianjin Key Laboratory of Functional Crystal Materials Institute of Functional Crystals Tianjin University of Technology Tianjin China) Z Zhi‐Ming Zhang (State Key Laboratory of Crystal Materials Institute for New Energy Materials and Low Carbon Technologies School of Materials Science and Engineering Tianjin University of Technology Tianjin China)

Abstract

Abstract Tandem CO 2 reduction with carbonylation reactions represents a promising approach to convert greenhouse gases into valuable chemicals. Herein, we propose a universal “N/O mixed pre‐coordination pyrolysis” strategy to construct vacancy‐defect single atom catalysts (Ni 1 ‐, Mn 1 ‐, Fe 1 ‐, Co 1 ‐, and Cu 1 ‐NC) with M‐N 3 coordination microenvironment. This vacancy‐defect endows Ni 1 ‐NC with excellent performance for CO 2 electroreduction, achieving a CO faradaic efficiency exceeding 90% across a wide range of current densities up to 300 mA cm −2 . The generated CO was directly fed to carbonylation reactions, producing organic chemicals with yields of up to 91.7% and leading to produce 1.13 g of benzophenone in a single run. For the first time, the membrane separation CO 2 system was integrated with tandem catalytic system, enabling direct utilization of flue gas for benzophenone synthesis with a 76.6% yield. This work offers a sustainable, eco‐friendly method for CO 2 separation and utilization by feeding industrial waste gas to carbonylation reactions.

Article Details

Volume / Issue Vol. 64, Issue 35
Published August 25, 2025
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (7)

Q

Qiu‐Ping Zhao

Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China

W

Wen‐Xiong Shi

Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China

B

Bo Wang

Z

Zuo‐Shu Sun

State Key Laboratory of Crystal Materials, Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science &amp; Engineering Tianjin University of Technology Tianjin 300384 China

S

Shuang Yao

Department of Otolaryngology Head and Neck Surgery, Beijing Tongren Hospital

T

Tong‐Bu Lu

State Key Laboratory of Crystal Materials Tianjin Key Laboratory of Functional Crystal Materials Institute of Functional Crystals Tianjin University of Technology Tianjin China

Z

Zhi‐Ming Zhang

State Key Laboratory of Crystal Materials Institute for New Energy Materials and Low Carbon Technologies School of Materials Science and Engineering Tianjin University of Technology Tianjin China