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通过使用黄金纳米粒子限制界面基激素,有效的光催化CH4转化为乙醇

Quan Zhang^1,2, Chao Yang¹, Yangshen Chen¹

¹Laboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, 200438, China.

Angewandte Chemie (International ed. in English)

|December 11, 2024

概括

这项研究引入了一种新型的金纳米粒子功能化木瓦纳酸盐 (BiVO₄@Au) 光催化剂,用于将甲 (CH₄) 转化为乙醇. 催化剂通过控制基 (⋅OH) 水平来增强乙醇选择性,在环境条件下实现高产量.

科学领域:

材料科学材料科学材料科学
光催化作用的光催化
绿色化学绿色化学

背景情况:

选择性氧化甲 (CH4) 到像乙醇这样的多碳产品是非常理想的,但由于惰性C-H键,具有挑战性.
基基 (⋅OH) 对于CH4激活至关重要,但可以导致过度氧化,形成不必要的C1产品而不是乙醇.
开发可选择性激活CH4和促进C-C合的光催化剂对于高效的乙醇合成至关重要.

研究的目的:

开发一种高度选择性的光催化剂,在环境条件下将CH4转化为乙醇.
研究表面修饰金纳米颗粒 (Au) 在BiVO₄上控制活性氧物种和增强乙醇选择性的作用.
优化光催化系统,以提高CH4到乙醇的转化效率和稳定性.

主要方法:

用Au纳米粒子 (BiVO₄@Au) 功能化的BiVO₄光催化剂的合成.
在环境条件下使用开发的BiVO₄@Au催化剂对CH₄进行光催化氧化.
使用气体扩散层来增强CH4运输到光催化界面.
反应性氧物种 (ROS) 和反应中间体的表征,以了解反应机制.

主要成果:

BiVO₄@Au光催化剂证明了有效的CH₄激活和选择性氧化到乙醇.
使用Au纳米颗粒的表面功能化有助于产生甲基基 (⋅CH₃) 和消耗⋅OH,增强⋅CH₃/⋅OH比率.
使用气体扩散层进一步提高了乙醇的选择性和生产率.
达到680μmol·g-1的峰值乙醇产量,具有86%的选择性和>100小时的稳定光转换.

结论:

BiVO₄@Au光催化剂为选择性CH₄转化为乙醇提供了一个有效的策略.
在现场生成和调节⋅OH水平对于促进C-C合和抑制过度氧化至关重要.
这种方法为从甲中可持续生产多碳化学品提供了一个有希望的途径.

关键词:

在AU纳米粒子.在CH4氧化过程中.乙醇生产乙醇生产光催化作用的光催化作用有活性氧物种的反应性氧物种.

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