【摘要】 为了缓解碳基燃料带来的日益严重的生态威胁，通过模拟光合作用机制来构建Z型异质结提供了一种有前景的方法，以实现太阳能驱动的二氧化碳还原为高附加值化学燃料。本文设计并制备了一种基于静电相互作用将类金属卟啉Co_x-CN与Keggin型POM(PMo₁₀V₂O₄₀^5-)偶联的Z机制复合光催化剂。由于其氧化还原性质和电荷转移机制与绿色植物中的叶绿素P700和P680相似，复合异质结表现出宽光谱吸收能力和强CO₂吸收能力，并抑制了光生载流子的复合。在可见光照射下，最佳的0.05PMo₁₀V₂/Co₁-CN异质结显示出最高的CO产量，为101.38μmol·g^-1·h^-1,分别比CN和Co₁-CN增加了约250倍和约9倍，同时抑制了竞争性H₂的产生。这项工作为开发高效、低成本的Z机制CO₂转化光催化剂提供了一种有效的设计策略。更多还原

【Abstract】 To alleviate the growing serious ecological threats brought by carbon-based fuels, it is a promising approach to construct a Z-scheme heterojunction via simulating the photosynthetic mechanism for solar-driven CO₂ reduction into high value-added chemical fuels. Herein, we design and prepare a Z-scheme composite photocatalyst based on coupling metalloporphyrin-like Co_x-CN with Keggin-type POMs(PMo₁₀V₂O₄₀^5-) by electrostatic interactions. By virtue of the redox property and charge transfer mechanism similar to chlorophyll P700 and P680 in green plants, the composite heterojunction exhibits broad-spectrum absorption and strong CO₂ absorption capacity, as well as the inhibition of the recombination of photo-introduced carriers. Under visible light irradiation, the optimized 0.05PMo₁₀V₂/Co₁-CN heterojunction shows the highest CO yield of 101.38 μmol·g^-1·h^-1, which is increased by about 250 and 9 times compared with those of CN and Co₁-CN, respectively, and concomitantly inhibits competitive H₂ generation. This work provides a promising strategy to develop high-efficiency and low-cost Z-scheme photocatalysts for CO₂ conversion.更多还原