Concurrent Ammonia Synthesis and Alcohol Oxidation Boosted by Glutathione‐Capped Quantum Dots under Visible Light

作者：Shu‐Lin Meng, Jia‐Hao Li, Chen Ye, Yu‐Lin Yin, X. K. Zhang, Chen Zhang, Xu‐Bing Li, Chen‐Ho Tung, Li‐Zhu Wu · 发表于：Advanced Materials · 年份：2024 · DOI：10.1002/adma.202311982 · 被引用次数：17 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Advanced Photocatalysis Techniques、Carbon and Quantum Dots Applications

Abstract Mother nature accomplishes efficient ammonia synthesis via cascade N 2 oxidation by lightning strikes followed with enzyme‐catalyzed nitrogen oxyanion (NO x − , x = 2,3) reduction. The protein environment of enzymatic centers for NO x − ‐to‐NH 4 + process greatly inspires the design of glutathione‐capped (GSH) quantum dots (QDs) for ammonia synthesis under visible light (440 nm) in tandem with plasma‐enabled N 2 oxidation. Mechanistic studies reveal that GSH induces positive shift of surface charge to strengthen the interaction between NO x − and QDs. Upon visible light irradiation of QDs, the balanced and rapid hole and electron transfer furnish GS·radicals for 2e − /2H + alcohol oxidation and H·for 8e − /10H + NO 3 − ‐to‐NH 4 + reduction simultaneously. For the first time, mmol‐scale ammonia synthesis is realized with apparent quantum yields of 5.45% ± 0.64%, and gram‐scale synthesis of value‐added acetophenone and NH 4 Cl proceeds with 1:4 stoichiometry and stability, demonstrating promising multielectron and multiproton ammonia synthesis efficiency and sustainability with nature‐inspired artificial photocatalysts.