Zhao Yujie, Cui Yang, Xie Lixia, Geng Kangshuai, Wu Jie, Meng Xiangru, Hou Hongwei
Green Catalysis Center and College of Chemistry, Zhengzhou University, Zhengzhou 450002, Henan, P. R. China.
College of Science, Henan Agricultural University, Zhengzhou 450002, Henan, P. R. China.
Inorg Chem. 2023 Jan 23;62(3):1240-1249. doi: 10.1021/acs.inorgchem.2c03970. Epub 2023 Jan 11.
Photocatalytic reduction of CO to value-added chemicals is known to be a promising approach for CO conversion. The design and preparation of ideal photocatalysts for CO conversion are of pivotal significance for the sustainable development of the whole society. In this work, we integrated two functional organic linkers to prepare a novel metal organic framework (MOF) photocatalyst {[Co(9,10-bis(4-pyridyl)anthracene)(bpda)]·4DMF} (Co-MOF). The existence of anthryl and amino groups leads to a wide range of visible light absorption and efficient separation of photogenerated electrons. To extend the lifetime of photogenerated electrons in the photocatalytic system, we modified Co-MOF particles onto g-CN. As expected, Co-MOF/g-CN composites exhibited an ultrahigh selectivity (more than 97%) in the photocatalytic process, and the highest CO production rate (1824 μmol/g/h) was 7.1 and 27.2 times of Co-MOFs and g-CN, respectively. What's more, we also discussed the reaction mechanism of the Co-MOF/g-CN photocatalytic CO reduction, and this work paves the pathway for designing photocatalysts with ideal CO reduction performance.
光催化将CO还原为增值化学品是一种很有前景的CO转化方法。设计和制备用于CO转化的理想光催化剂对整个社会的可持续发展具有关键意义。在这项工作中，我们整合了两种功能性有机连接体来制备一种新型金属有机框架（MOF）光催化剂{[Co(9,10-双(4-吡啶基)蒽)(bpda)]·4DMF}（Co-MOF）。蒽基和氨基的存在导致其具有广泛的可见光吸收以及光生电子的有效分离。为了延长光催化体系中光生电子的寿命，我们将Co-MOF颗粒修饰到g-CN上。正如预期的那样，Co-MOF/g-CN复合材料在光催化过程中表现出超高的选择性（超过97%），并且最高CO产率（1824 μmol/g/h）分别是Co-MOFs和g-CN的7.1倍和27.2倍。此外，我们还讨论了Co-MOF/g-CN光催化CO还原的反应机理，这项工作为设计具有理想CO还原性能的光催化剂铺平了道路。
