连接氧化和还原簇以制备用于光催化用HO还原CO的结晶多孔催化剂。
Linking oxidative and reductive clusters to prepare crystalline porous catalysts for photocatalytic CO reduction with HO.
作者信息
Zhou Jie, Li Jie, Kan Liang, Zhang Lei, Huang Qing, Yan Yong, Chen Yifa, Liu Jiang, Li Shun-Li, Lan Ya-Qian
机构信息
School of Chemistry, South China Normal University, Guangzhou, 510006, P.R. China.
出版信息
Nat Commun. 2022 Aug 10;13(1):4681. doi: 10.1038/s41467-022-32449-z.
Mimicking natural photosynthesis to convert CO with HO into value-added fuels achieving overall reaction is a promising way to reduce the atmospheric CO level. Casting the catalyst of two or more catalytic sites with rapid electron transfer and interaction may be an effective strategy for coupling photocatalytic CO reduction and HO oxidation. Herein, based on the MOF ∪ COF collaboration, we have carefully designed and synthesized a crystalline hetero-metallic cluster catalyst denoted MCOF-TiCu with spatial separation and functional cooperation between oxidative and reductive clusters. It utilizes dynamic covalent bonds between clusters to promote photo-induced charge separation and transfer efficiency, to drive both the photocatalytic oxidative and reductive reactions. MCOF-TiCu exhibits fine activity in the conversion of CO with water into HCOOH (169.8 μmol gh). Remarkably, experiments and theoretical calculations reveal that photo-excited electrons are transferred from Ti to Cu, indicating that the Cu cluster is the catalytic reduction center.
模仿自然光合作用将二氧化碳与水转化为增值燃料以实现整体反应，是降低大气中二氧化碳水平的一种有前景的方法。构建具有快速电子转移和相互作用的两个或更多催化位点的催化剂，可能是耦合光催化二氧化碳还原和水氧化的有效策略。在此，基于金属有机框架（MOF）与共价有机框架（COF）的协作，我们精心设计并合成了一种晶体异金属簇催化剂，命名为MCOF-TiCu，其氧化簇和还原簇之间具有空间分离和功能协同作用。它利用簇之间的动态共价键来提高光致电荷分离和转移效率，从而驱动光催化氧化和还原反应。MCOF-TiCu在将二氧化碳与水转化为甲酸（169.8 μmol g⁻¹ h⁻¹）方面表现出良好的活性。值得注意的是，实验和理论计算表明，光激发电子从钛转移到铜，这表明铜簇是催化还原中心。
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