Chen Ruijie, Yin Haotian, Wang Lei, Zhang Zhiqiang, Ding Jing, Zhang Jinfeng, Wan Hui, Guan Guofeng
State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials, Nanjing Tech University, Nanjing 210009, PR China.
Key Laboratory of Green and Precise Synthetic Chemistry and Applications, Ministry of Education, Huaibei Normal University, Huaibei 235000, PR China.
J Colloid Interface Sci. 2023 Feb;631(Pt A):122-132. doi: 10.1016/j.jcis.2022.11.006. Epub 2022 Nov 7.
The reduction of CO achieved by photocatalysis can simultaneously alleviate the energy crisis and solve environmental issues. Nevertheless, it remains challenging for the rational design of photocatalysts with high-efficiency carrier migration ability. Herein, the Z-scheme g-CN/InO (CN/INO) heterostructure was fabricated via metal-organic frameworks (MOFs) assisted thermal deposition which could form a fully encapsulated hollow tubular structure. The unique structure was based on the MOFs-derived hollow hexagonal InO tubular integrated with ultrathin g-CN. The Z-scheme CN/INO heterojunction exhibited a larger specific surface area and excellent charge separation efficiency. Benefiting from the above features, the Z-scheme CN/INO heterojunction demonstrated superior performance on photocatalytic CO reduction. The formation of CO and CHOH over the optimized CN/INO-2 catalyst was 7.94 and 1.44 µmol⋅g⋅h, respectively. Moreover, the density functional theory (DFT) calculations and Kelvin probe force microscopy (KPFM) was carried out to further investigate the situation of charge transfer on the interface of CN/INO. The in-situ Fourier transform infrared spectroscopy (FTIR) was measured to confirm the immediate products and the possible mechanism of photocatalytic CO reduction was proposed. This work provided a MOFs-assisted strategy to construct a Z-scheme system for photocatalytic CO reduction.
通过光催化实现的一氧化碳还原能够同时缓解能源危机并解决环境问题。然而，合理设计具有高效载流子迁移能力的光催化剂仍然具有挑战性。在此，通过金属有机框架（MOFs）辅助热沉积制备了Z型g-CN/InO（CN/INO）异质结构，该结构可形成完全封装的中空管状结构。这种独特的结构基于MOFs衍生的中空六边形InO管与超薄g-CN的集成。Z型CN/INO异质结表现出更大的比表面积和优异的电荷分离效率。受益于上述特性，Z型CN/INO异质结在光催化一氧化碳还原方面表现出优异的性能。在优化后的CN/INO-2催化剂上，一氧化碳和甲醇的生成量分别为7.94和1.44 μmol⋅g⋅h。此外，进行了密度泛函理论（DFT）计算和开尔文探针力显微镜（KPFM）研究，以进一步探究CN/INO界面上的电荷转移情况。通过原位傅里叶变换红外光谱（FTIR）测量来确认即时产物，并提出了光催化一氧化碳还原的可能机制。这项工作提供了一种MOFs辅助策略，用于构建用于光催化一氧化碳还原的Z型体系。
