ZIF-8 衍生的 Ag/ZnO 光催化剂具有富集的 Ag-ZnO 界面,可将甲烷有效氧化为液态含氧化合物,同时具有毫摩尔级的生产率和 ∼100 % 的选择性

Yingdong Hao, Yonghui Zhao, Chunlai Zhang, Xinqing Chen, Nannan Sun, Wei Wei
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引用次数: 0

摘要

实现高产氧率和抑制过氧化仍然是 CH 光氧化的挑战。在此,我们报告了一种以 ZIF-8 为前驱体、具有富集 Ag-ZnO 界面的催化剂。所制备的 Ag/Z-450 光催化剂在 CH 的光催化氧化过程中表现出非凡的效率,在 3.0Ag/Z-450 上可获得 57.88 mmol-g (28.94 mmol-g-h)的高液态含氧化合物产率和 ∼100 % 的选择性,其中 HCHO 为主要产物(41.04 mmol-g,∼71 % 的选择性)。机理研究表明,氧化锌和银分别作为电子供体和受体,促进了电荷载体的转移和分离。CH 和 O 可被有效激活,生成 -CH 和活性氧(ROS),它们的后续反应导致 CHOOH 的形成,而 CHOOH 又可进一步转化为 CHOH 和 HCHO。这项工作有助于开发一种 "二合一 "的 CH 光氧化催化剂系统,该系统可同时实现无与伦比的生产率和选择性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
ZIF-8 derived Ag/ZnO photocatalyst with enriched Ag-ZnO interface for effective oxidation of methane to liquid oxygenates with simultaneous mmol-scale productivity and ∼100 % selectivity
Achieving a high yield of oxygenates and inhibiting overoxidation remain challenging for CH photooxidation. Here, we report a catalyst with enriched Ag-ZnO interfaces by using ZIF-8 as the precursor. The resulting Ag/Z-450 photocatalysts show extraordinary efficiency in the photocatalytic oxidation of CH, a high liquid oxygenate yield of 57.88 mmol·g (28.94 mmol·g·h) and a selectivity of ∼100 % were obtained over 3.0Ag/Z-450, with HCHO as the major product (41.04 mmol·g, ∼71 % selectivity). Mechanistic studies revealed that ZnO and Ag species acted as electron donors and acceptors, respectively, which enhanced charge carriers transfer and separation. CH and O can be effectively activated to generate •CH and reactive oxygen species (ROS), their following reaction led to formation of CHOOH, which can be further converted to CHOH and HCHO. This work contributes to the development of a “two-in-one” CH photooxidation catalyst system that simultaneously achieves unparallel productivity and selectivity.
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