Dual-functional photoredox catalysis over Ni/CdS composite

IF 4.3 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis Pub Date : 2026-03-01 Epub Date: 2026-01-30 DOI:10.1016/j.mcat.2026.115763

Hui-Li Wu , Jia-Wei Liu , Chang-Long Tan , Zi-Rong Tang

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引用次数: 0

Abstract

Selective photocatalytic dehydrogenation of saturated N-heterocycles represents a sustainable photoredox route for synthesizing valuable nitrogen-containing unsaturated heteroaromatic organics. Herein, we report a Ni-decorated 3D sea urchin-like CdS composite (Ni/CdS) as a dual-functional photocatalyst for the efficient and selective semi-dehydrogenation of 1,2,3,4-tetrahydroisoquinoline (THIQ) to 3,4-dihydroisoquinoline (DHIQ) coupled with H₂ evolution under visible light irradiation. The surface-decorated Ni nanoparticles significantly enhance the separation and transfer of photogenerated electron–hole pairs over Ni/CdS, and act as reactive sites for proton reduction to H₂, thereby leading to the improved dual-functional photoredox catalysis. Mechanistic studies identify the carbon-centered radical (•CH(NH)C₈H₈) as a pivotal intermediate in the photocatalytic semi-dehydrogenation of THIQ. This study establishes an effective strategy for designing noble-metal-free photocatalytic systems that integrate selective organic transformations with H₂ evolution in a cooperative manner.

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Ni/CdS复合材料的双功能光氧化还原催化

饱和n-杂环的选择性光催化脱氢为合成有价含氮不饱和杂芳烃有机物提供了一条可持续的光氧化还原途径。本文报道了一种镍修饰的三维海胆样CdS复合材料（Ni/CdS）作为双功能光催化剂，在可见光照射下高效、选择性地将1,2,3,4-四氢异喹啉（THIQ）半脱氢为3,4-二氢异喹啉（DHIQ），并伴有H2的析出。表面修饰的Ni纳米粒子显著增强了Ni/CdS上光生电子空穴对的分离和转移，并作为质子还原H2的反应位点，从而改善了双功能光氧化还原催化。机理研究发现碳中心自由基（•CH(NH)C8H8）是THIQ光催化半脱氢的关键中间体。本研究建立了一种设计无贵金属光催化系统的有效策略，该系统将选择性有机转化与H2进化以合作的方式结合起来。

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来源期刊

Molecular Catalysis Chemical Engineering-Process Chemistry and Technology

CiteScore

6.90

自引率

10.90%

发文量

700

审稿时长

40 days

期刊介绍： Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods