材料科学
量子点
可见光谱
氮氧化物
光化学
氨
激进的
氧化还原
石墨烯
纳米技术
组合化学
光电子学
有机化学
化学
燃烧
冶金
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
标识
DOI:10.1002/adma.202311982
摘要
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.
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