MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, China.
Chemistry and Chemical Engineering of Guangdong Laboratory, Shantou 515063, China.
J Am Chem Soc. 2021 Oct 27;143(42):17424-17430. doi: 10.1021/jacs.1c05839. Epub 2021 Oct 12.
Reducing CO into fuels via photochemical reactions relies on highly efficient photocatalytic systems. Herein, we report a new and efficient photocatalytic system for CO reduction. Driven by electrostatic attraction, an anionic metal-organic framework (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene) as host and a cationic photosensitizer [Ru(phen)] (phen = 1,10-phenanthroline) as guest were self-assembled into a photocatalytic system , which showed high activity for photocatalytic CO reduction under laboratory light source (CO production rate of 130(5) mmol g h, selectivity of 92.9%) or natural sunlight (CO production rate of 69.5 mmol g h, selectivity of 91.3%), representing the remarkable photocatalytic CO reduction performance. More importantly, the photosensitizer [Ru(phen)] in is only about 1/500 in quantity reported in the literature. Theoretical calculations and control experiments suggested that the assembly of the catalysts and photosensitizers via electrostatic attraction interactions can provide a better charge transfer efficiency, resulting in high performance for photocatalytic CO reduction.
通过光化学反应将 CO 转化为燃料依赖于高效的光催化体系。在此，我们报告了一种用于 CO 还原的新型高效光催化体系。受静电吸引的驱动，阴离子金属有机骨架（HHTP = 2,3,6,7,10,11-六羟基三苯）作为主体，阳离子光敏剂[Ru(phen)]（phen = 1,10-菲咯啉）作为客体自组装成光催化体系，在实验室光源（CO 生成速率为 130(5)mmol g h，选择性为 92.9%）或自然光（CO 生成速率为 69.5 mmol g h，选择性为 91.3%）下表现出高的光催化 CO 还原活性，这代表了显著的光催化 CO 还原性能。更重要的是，在 中，光敏剂[Ru(phen)]的用量仅为文献报道的约 1/500。理论计算和控制实验表明，通过静电吸引相互作用组装催化剂和光敏剂可以提供更好的电荷转移效率，从而实现高光催化 CO 还原性能。
