苯
氢氧化物
催化作用
选择性
吸附
扩展X射线吸收精细结构
苯酚
层状双氢氧化物
双键
基质(水族馆)
材料科学
纳米颗粒
无机化学
化学
光化学
化学工程
物理化学
吸收光谱法
纳米技术
有机化学
工程类
物理
海洋学
量子力学
地质学
作者
Tianyang Shen,Ziheng Song,Jiaxin Li,Sha Bai,Guihao Liu,Xiaoliang Sun,Shaoquan Li,Wei Chen,Lirong Zheng,Yu‐Fei Song
出处
期刊:Small
[Wiley]
日期:2023-06-13
卷期号:19 (41)
被引量:1
标识
DOI:10.1002/smll.202303420
摘要
Direct and selective oxidation of benzene to phenol is a long-term goal in industry. Although great efforts have been made in homogenous catalysis, it still remains a huge challenge to drive this reaction via heterogeneous catalysts under mild conditions. Herein, a single-atom Au loaded MgAl-layered double hydroxide (Au1 -MgAl-LDH) with a well-defined structure, in which the Au single atoms are located on the top of Al3+ with Au-O4 coordination as revealed by extended x-ray-absorption fine-structure (EXAFS)and density-functional theory (DFT)calculation is reported. The photocatalytic results prove the Au1 -MgAl-LDH is capable of driving benzene oxidation reaction with O2 in water, and exhibits a high selectivity of 99% for phenol. While contrast experiment shows a ≈99% selectivity for aliphatic acid with Au nanoparticle loaded MgAl-LDH (Au-NP-MgAl-LDH). Detailed characterizations confirm that the origin of the selectivity difference can be attributed to the profound adsorption behavior of substrate benzene with Au single atoms and nanoparticles. For Au1 -MgAl-LDH, single Au-C bond is formed in benzene activation and result in the production of phenol. While for Au-NP-MgAl-LDH, multiple AuC bonds are generated in benzene activation, leading to the crack of CC bond.
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