Zhao Qiu-Ping, Shi Wen-Xiong, Wang Bo, Sun Zuo-Shu, Yao Shuang, Lu Tong-Bu, Zhang Zhi-Ming
State Key Laboratory of Crystal Materials, Institute for New Energy Materials and Low Carbon Technologies, School of Materials Science & Engineering, Tianjin University of Technology, Tianjin, 300384, China.
Tianjin Key Laboratory of Life and Health Detection, Life and Health Intelligent Research Institute, Tianjin University of Technology, Tianjin, 300384, China.
Angew Chem Int Ed Engl. 2025 Aug 25;64(35):e202510693. doi: 10.1002/anie.202510693. Epub 2025 Jul 7.
Tandem CO 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-, Mn-, Fe-, Co-, and Cu-NC) with M-N coordination microenvironment. This vacancy-defect endows Ni-NC with excellent performance for CO electroreduction, achieving a CO faradaic efficiency exceeding 90% across a wide range of current densities up to 300 mA cm. 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 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 separation and utilization by feeding industrial waste gas to carbonylation reactions.
串联式一氧化碳还原与羰基化反应是一种将温室气体转化为有价值化学品的有前景的方法。在此，我们提出一种通用的“N/O混合预配位热解”策略，以构建具有M-N配位微环境的空位缺陷单原子催化剂（Ni-NC、Mn-NC、Fe-NC、Co-NC和Cu-NC）。这种空位缺陷赋予Ni-NC在CO电还原方面优异的性能，在高达300 mA cm的宽电流密度范围内实现了超过90%的CO法拉第效率。生成的CO被直接用于羰基化反应，生产有机化学品，产率高达91.7%，单次运行可生产1.13 g二苯甲酮。首次将膜分离CO系统与串联催化系统集成，使烟道气能够直接用于二苯甲酮合成，产率为76.6%。这项工作通过将工业废气输送到羰基化反应中，提供了一种可持续、环保的CO分离和利用方法。
