Design of well-defined shell–core covalent organic frameworks/metal sulfide as an efficient Z-scheme heterojunction for photocatalytic water splitting,Chemical Science

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Design of well-defined shell–core covalent organic frameworks/metal sulfide as an efficient Z-scheme heterojunction for photocatalytic water splitting
Chemical Science ( IF 7.6 ) Pub Date : 2021-12-01 , DOI: 10.1039/d1sc05893b
Yan Wang ₁ , Zhao Hu ₂ , Wei Wang ₁ , Haichuan He ₁ , Liu Deng _{1,

3} , Yi Zhang ₁ , Jianhan Huang ₁ , Ning Zhao ₃ , Guipeng Yu ₁ , You-Nian Liu _{1,

3}

Affiliation

Development of a covalent–organic framework (COF)-based Z-scheme heterostructure is a promising strategy for solar energy driven water splitting, but the construction of a COF-based Z-scheme heterostructure with well-defined architecture, large contact area and intimate contact interfaces is scarce. Herein, we fabricated a direct Z-scheme heterostructure COF–metal sulfide hybrid (T-COF@CdS) with shell–core architecture by self-polymerization of 1,3,5-benzenetricarboxaldehyde and 2,4,6-tris(4-aminophenyl)-1,3,5-triazine in situ on CdS. The formed C–S chemical bonding between T-COF and CdS could provide a very tight and stable interface. Owing to the properly staggered band alignment, strong interfacial interaction and large interfacial contact area between T-COF and CdS, a Z-scheme route for charge separation and transfer is realized, resulting in electron accumulation in CdS for H₂O reduction. The obtained Z-scheme heterostructure T-COF@CdS-3 exhibits a high apparent quantum efficiency of 37.8% under 365 nm monochromatic light irradiation, and long-term stability arising from shell–core structures in which the T-COF shell protects the catalytic centers of CdS against deactivation, as well as acts as oxidation sites to avoid the photocorrosion of CdS. This work provides a strategy for the construction of a shell–core direct Z-scheme heterostructure photocatalyst for water splitting with high performance.

中文翻译：

设计明确的壳核共价有机框架/金属硫化物作为光催化水分解的高效 Z 型异质结

开发基于共价有机框架（COF）的Z型异质结构是太阳能驱动水分解的一种有前景的策略，但是基于COF的Z型异质结构的构建具有明确的结构、大的接触面积和紧密的接触面积。接触接口稀少。在此，我们通过1,3,5-苯三甲醛和2,4,6-三(4-)的自聚合制备了具有壳核结构的直接Z型异质结构COF-金属硫化物杂化物（T-COF@CdS）。氨基苯基)-1,3,5-三嗪在 CdS 上原位。 T-COF 和 CdS 之间形成的 C-S 化学键可以提供非常紧密且稳定的界面。由于T-COF和CdS之间适当交错的能带排列、强界面相互作用和大界面接触面积，实现了电荷分离和转移的Z型路线，导致电子在CdS中积累以还原H ₂ O。所获得的Z型异质结构T-COF@CdS-3在365 nm单色光照射下表现出37.8%的高表观量子效率，并且由于T-COF壳保护催化层的壳核结构而产生长期稳定性。 CdS 的中心防止失活，并充当氧化位点以避免 CdS 的光腐蚀。这项工作为构建高性能水分解壳核直接Z型异质结构光催化剂提供了策略。

更新日期：2021-12-01

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