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调节活性的供应和O2吸附:硫空缺问题促进H2O光合作用性能

Yamin Xi¹, Chaoqi Zhang¹, Wenjing Tu¹

¹School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200241, P.R. China.

Angewandte Chemie (International ed. in English)

|April 11, 2025

概括

这项研究引入了一种新的双位点光催化剂,Ni-doped ZnS空心纳米立方体与S空位 (Ni-ZnS-Sv),通过两电子氧降解反应 (2e−ORR) 通过高效的过氧化 (H2O2) 生产. 催化剂在人工光合作用中表现出卓越的性能.

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
电化学电化学电化学

背景情况:

两电子氧降解反应 (2e−ORR) 是产生过氧化 (H2O2) 的关键途径.
目前的光催化剂往往缺乏高效的O2吸附和化能力,限制了H2O2的产生.
开发先进的光催化剂对于高效的人工光合作用和H2O2合成至关重要.

研究的目的:

设计和合成一种新的双站点光催化剂,用于增强2e− ORR.
调查 (Ni) 兴奋剂和硫 (S) 空缺在调节光催化活性中的作用.
通过人工光合作用来实现高效的H2O2生产.

主要方法:

合成Ni-doped ZnS空心纳米立方体,其中有S空位 (Ni-ZnS-Sv).
对光催化剂的结构和性能进行实验性表征.
密度函数理论 (DFT) 计算以阐明反应机制.
在UV-V照射下对H2O2生产的光催化性能评估.

主要成果:

Ni-ZnS-Sv光催化剂有效地促进了2e− ORR通路.
硫空缺调节Ni和S站点的电子结构,增强选择性和活动性.
原子分散的Ni位点促进了最佳的O2吸附和中介物的中度结合.
缺电子的S位点通过促进*Hads迁移来加速化动力学.
在纯水中实现了5649.49 μmol g-1 h-1 的高H2O2产量.

结论:

Ni-ZnS-Sv作为一个有效的双站点光催化剂,用于H2O2生产.
对于高光催化性能而言,Ni和S空缺的协同效应至关重要.
这项工作为设计用于人工H2O2光合作用的光催化剂提供了宝贵的见解.

关键词:

产生 H2O2 的时间.尼克尔被使用过的.光催化作用的光催化在硫空缺的职位.过渡金属硫化物过渡金属硫化物

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