Vacancy‐Defect Single‐Atom Catalysts for Tandem CO <sub>2</sub> Electroreduction and Carbonylation Reactions from Flue Gas
Tandem CO<sub>2</sub> 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<sub>1</sub>-, Mn<sub>1</sub>-, Fe<sub>1</sub>-, Co<sub>1</sub>-, and Cu<sub>1</sub>-NC) with M-N<sub>3</sub> coordination microenvironment. This vacancy-defect endows Ni<sub>1</sub>-NC with excellent performance for CO<sub>2</sub> electroreduction, achieving a CO faradaic efficiency exceeding 90% across a wide range of current densities up to 300 mA cm<sup>-2</sup>. 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<sub>2</sub> 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<sub>2</sub> separation and utilization by feeding industrial waste gas to carbonylation reactions.
Authors
- Shuang Yao (ORCID: https://orcid.org/0000-0001-7511-5759)
- Qiuping Zhao (ORCID: https://orcid.org/0009-0005-3654-1735)
- Tong‐Bu Lu (ORCID: https://orcid.org/0000-0002-6087-4880)
- Wenxiong Shi (ORCID: https://orcid.org/0000-0002-7969-3780)
- Zhiming Zhang (ORCID: https://orcid.org/0000-0003-3116-756X)
- Zuo-Shu Sun
- Bo Wang (ORCID: https://orcid.org/0000-0003-3327-2646)
Institutions
- Tianjin University of Technology (CN)
Publication Details
- Journal
- Angewandte Chemie International Edition
- Published
- 2025-07-01
- DOI
- https://doi.org/10.1002/anie.202510693
- Citations
- 4
- Primary Topic
- CO2 Reduction Techniques and Catalysts
- Type
- article
- Field-Weighted Citation Impact
- 1.45