傅里叶变换红外光谱
光化学
羟基化
催化作用
光催化
氢
氢原子萃取
化学
分子
光谱学
无机化学
化学工程
有机化学
物理
量子力学
酶
工程类
作者
Fan Dong,Xian Shi,Zhihao Cui,Weidong Dai,Fan Dong
出处
期刊:ACS Nano
[American Chemical Society]
日期:2024-03-22
卷期号:18 (13): 9670-9677
标识
DOI:10.1021/acsnano.4c00975
摘要
Employing water as a hydrogen source to participate in the hydrogen atom transfer (HAT) process is a low-cost and carbon-free process demonstrating great economic and environmental potential in catalysis. However, the low efficiency of hydrogen atom abstraction from water leads to slow kinetics of HAT for most hydrogenative reactions. Here, we prepared ultrathin Bi4O5Cl2 nanosheets where the surface can be in situ reconstructed via hydroxylation under light illumination to facilitate the abstraction of hydrogen atoms from pure water for efficient nitrogen fixation. Consequently, the isotope labeling in situ Fourier-transform infrared spectroscopy (FT-IR) involving H2O and D2O has clearly revealed that the hydroxyl groups tend to be adsorbed on the chloride vacancy sites on the Bi4O5Cl2 surface to form hydroxylated surfaces, where the hydroxylated photocatalyst surface enables partial dehydrogenation of water into H2O2, allowing the utilization of H atoms for efficient of N2 hydrogenation via HAT steps. This work elucidates the in-depth reaction mechanism of hydrogen atom extraction from H2O molecules via the light-generated chloride vacancy to promote photocatalytic nitrogen fixation, ultimately enabling the inspiration and providing crucial rules for the design of important functional materials that can efficiently deliver active hydrogen for chemical synthesis.
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