<br>用于高效 S-S 耦合反应的钙钛矿 MAPbBr3/COF 纳米异质结构的可调能带工程管理,Small

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用于高效 S-S 耦合反应的钙钛矿 MAPbBr3/COF 纳米异质结构的可调能带工程管理
Small ( IF 13.0 ) Pub Date : 2023-09-01 , DOI: 10.1002/smll.202304776
Qianying Lin ₁ , Siyi Tan _{1,

2} , Jiwu Zhao ₁ , Xiao Fang _{1,

3} , Ying Wang ₁ , Na Wen _{1,

4} , Zizhong Zhang ₁ , Zhengxin Ding ₁ , Rusheng Yuan ₁ , Guiyang Yan ₂ , Shengye Jin ₅ , Jinlin Long ₁

Affiliation

二硫键的高效人工光合作用有望促进遗传密码的反向解码和蛋白质多级折叠的秘密，以及生命科学和先进功能材料的发展。然而，现有的合成策略遇到了─S─S─偶联反应中离去基团产生的分离挑战。本研究根据自由基引发的─S─S─偶联反应机理，定制并构建了光驱动异质结功能光催化剂，使其能够高效产生自由基并引发偶联反应。具体而言，钙钛矿和共价有机框架（COF）因其优异的光捕获和光电性能以及灵活且可调谐的能带结构而被筛选为目标材料。原位组装的Z型异质结MAPB-M-COF（MAPbBr ₃ = MAPB，MA ⁺ = CH ₃ NH ₂ ⁺ ）通过能带工程管理证明了量子效率和氧化还原化学势之间的完美权衡。 MAPB-M-COF实现了100%的─S─S─耦合产率，创纪录的11.50%的光量子效率和出色的循环稳定性，可与所有现有的类似反应系统相媲美。凸显了面向应用的能带工程管理在设计高效多功能光催化剂方面的有效性和优越性。这项研究展示了一种从概念到验证的研究方法，用于开发用于光驱动化学反应和能量转换的各种集成异质结半导体。

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Tunable Band Engineering Management on Perovskite MAPbBr3/COFs Nano-Heterostructures for Efficient S–S Coupling Reactions

Efficient artificial photosynthesis of disulfide bonds holds promises to facilitate reverse decoding of genetic codes and deciphering the secrets of protein multilevel folding, as well as the development of life science and advanced functional materials. However, the incumbent synthesis strategies encounter separation challenges arising from leaving groups in the ─S─S─ coupling reaction. In this study, according to the reaction mechanism of free-radical-triggered ─S─S─ coupling, light-driven heterojunction functional photocatalysts are tailored and constructed, enabling them to efficiently generate free radicals and trigger the coupling reaction. Specifically, perovskites and covalent organic frameworks (COFs) are screened out as target materials due to their superior light-harvesting and photoelectronic properties, as well as flexible and tunable band structure. The in situ assembled Z-scheme heterojunction MAPB-M-COF (MAPbBr₃ = MAPB, MA⁺ = CH₃NH₂⁺) demonstrates a perfect trade-off between quantum efficiency and redox chemical potential via band engineering management. The MAPB-M-COF achieves a 100% ─S─S─ coupling yield with a record photoquantum efficiency of 11.50% and outstanding cycling stability, rivaling all the incumbent similar reaction systems. It highlights the effectiveness and superiority of application-oriented band engineering management in designing efficient multifunctional photocatalysts. This study demonstrates a concept-to-proof research methodology for the development of various integrated heterojunction semiconductors for light-driven chemical reaction and energy conversion.

更新日期：2023-09-01

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