Key Laboratory of Material Chemistry for Energy Conversion and Storage (Ministry of Education), Hubei Key Laboratory of Material Chemistry and Service Failure, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Luoyu Road No. 1037, 430074, Wuhan, China.
College of Chemistry and Molecular Science, Wuhan University, Bayi Road No. 299, 430072, Wuhan, China.
Nat Commun. 2019 Feb 8;10(1):676. doi: 10.1038/s41467-019-08651-x.
Significant efforts have been devoted to develop efficient visible-light-driven photocatalysts for the conversion of CO to chemical fuels. The photocatalytic efficiency for this transformation largely depends on CO adsorption and diffusion. However, the CO adsorption on the surface of photocatalysts is generally low due to their low specific surface area and the lack of matched pores. Here we report a well-defined porous hypercrosslinked polymer-TiO-graphene composite structure with relatively high surface area i.e., 988 m g and CO uptake capacity i.e., 12.87 wt%. This composite shows high photocatalytic performance especially for CH production, i.e., 27.62 μmol g h, under mild reaction conditions without the use of sacrificial reagents or precious metal co-catalysts. The enhanced CO reactivity can be ascribed to their improved CO adsorption and diffusion, visible-light absorption, and photo-generated charge separation efficiency. This strategy provides new insights into the combination of microporous organic polymers with photocatalysts for solar-to-fuel conversion.
研究人员投入了大量精力来开发高效的可见光驱动光催化剂，以将 CO 转化为化学燃料。这种转化的光催化效率在很大程度上取决于 CO 的吸附和扩散。然而，由于光催化剂的比表面积低且缺乏匹配的孔道，其对 CO 的吸附通常较低。在此，我们报道了一种具有明确孔结构的超交联聚合物-TiO2-石墨烯复合结构，其比表面积高达 988 m2 g，CO 吸附量高达 12.87wt%。在没有使用牺牲试剂或贵金属共催化剂的情况下，该复合结构在温和的反应条件下表现出高的光催化性能，特别是在 CH4 生成方面，其产率高达 27.62 μmol g h。增强的 CO 反应活性可归因于其提高的 CO 吸附和扩散、可见光吸收以及光生电荷分离效率。该策略为将微孔有机聚合物与光催化剂结合用于太阳能到燃料的转化提供了新的思路。
