CsPbBr3 in the Activation of the C–Br Bond of CBrX3 (X = Cl, Br) under Sunlight,Chemistry of Materials

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CsPbBr3 in the Activation of the C–Br Bond of CBrX3 (X = Cl, Br) under Sunlight
Chemistry of Materials ( IF 7.2 ) Pub Date : 2023-01-03 , DOI: 10.1021/acs.chemmater.2c03164
Anupam Manna ₁ , Tarun Kumar Dinda ₁ , Subhadip Ghosh ₁ , Prasenjit Mal ₁

Affiliation

A newly synthesized green-fluorescent, orthorhombic, bromide-rich, perovskite nanocrystal (Φ ∼ 0.93, τ ∼ 12.5 ns, E_ox = +1.6 V) obtained from an unprecedented bromide precursor dibromoisocyanuric acid was found to be an excellent visible-light (sunlight or blue-light-emitting diode (LED)) photocatalyst toward the synthesis of gem-dihaloenones for the first time. The photoactivated CsPbBr₃ catalyzed the homolytic cleavage of CBrX₃ (X = Cl, Br) to generate the ^•CX₃ radical, which underwent cascaded C–C cross-coupling with terminal alkynes into the corresponding gem-dihaloenones. Radical-trapping experiments and luminescence-quenching studies helped establish a single-electron-transfer (SET) mechanism. Interestingly, other highly stable CsPbBr₃ NCs, obtained from N-bromosuccinimide (NBS) and dibromohydantoin (DBHT) precursors, are unable to carry out these transformations. These results not only enrich the CsPbBr₃ synthetic methodology but also encourage the research community to develop efficient and cost-effective photocatalytic materials.

中文翻译：

CsPbBr3 在阳光下激活 CBrX3 (X = Cl, Br) 的 C-Br 键

从前所未有的溴化物前体二溴异氰尿酸中获得的新合成的绿色荧光、正交晶系、富含溴化物的钙钛矿纳米晶体（Φ ∼ 0.93，τ ∼ 12.5 ns，E _ox = +1.6 V）被发现具有出色的可见光（太阳光或蓝光发光二极管（LED））光催化剂首次用于合成宝石-二卤烯酮。光活化的 CsPbBr ₃催化 CBrX ₃ (X = Cl, Br) 均裂产生^• CX ₃自由基，其与末端炔烃进行级联 C-C 交叉偶联形成相应的宝石-二卤酮。自由基捕获实验和发光淬灭研究有助于建立单电子转移 (SET) 机制。有趣的是，从N-溴代琥珀酰亚胺 (NBS) 和二溴乙内酰脲 (DBHT) 前体获得的其他高度稳定的 CsPbBr ₃ NC无法进行这些转化。这些结果不仅丰富了 CsPbBr ₃的合成方法，而且鼓励研究界开发高效且具有成本效益的光催化材料。

更新日期：2023-01-03

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