脱氢
镍
催化作用
纳米颗粒
光化学
化学
制氢
光催化
金属有机骨架
选择性
金属
材料科学
组合化学
化学工程
有机化学
纳米技术
吸附
工程类
作者
Xiang-Yu Lin,Ming‐Yu Qi,Zi‐Rong Tang,Yi‐Jun Xu
标识
DOI:10.1016/j.apcatb.2022.121708
摘要
Photochemical dehydrogenation of N-heterocyclic amines to corresponding N-heteroaromatics paired with hydrogen (H2) production represents a promising route for the green and sustainable organic synthesis and clean fuel generation. Herein, metal-organic frameworks (MOFs)-supported CdS nanoparticles are gingerly fabricated for the visible light-initiated acceptorless dehydrogenation of diverse N-heterocycles at ambient conditions. With further nickel cocatalysts modification via a simple photodeposition method, the optimized MIL-101 @CdS-Ni composite exhibits remarkably enhanced activities, which are 8 folds higher than that of binary MIL-101 @CdS and 2.8 times higher than that of MOF-removed CdS-Ni counterparts, along with high selectivity and good stability. Mechanism studies reveal that active nickel species plays a key role in accelerating the separation of photogenerated charge carries and the cleavage of C−H and N−H bonds in the scaffold of N-heterocycles on the catalyst surface. This work is expected to guide the rational catalysts design of MOF-based multifunctional materials for photochemical coupling of concurrent organic synthesis with H2 production.
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