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Visible light-driven H2O2 synthesis over Au/C3N4: medium-sized Au nanoparticles exhibiting suitable built-in electric fields and inhibiting reverse H2O2 decomposition
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2022-11-18 , DOI: 10.1039/d2cp04202a
Mengzhen Song 1 , Huijuan Shao 1 , Yi Chen 1 , Xiangyang Deng 1 , Yanyan Chen 2 , Yue Yao 1 , Shuxiang Lu 1 , Xiaoyuan Liao 1
Affiliation  

Visible light-driven H2O2 production presents the unique merits of sustainability and environmental friendliness. The size of noble metal nanoparticles (NPs) determines their dispersion and electronic structure and greatly affects their photocatalytic activity. In this work, a series of sized Au NPs over C3N4 were modulated for H2O2 production. The results show that there is a volcanic trend in H2O2 with the decrease of Au particle size, and the highest H2O2 production rate of 1052 μmol g−1 h−1 is obtained from medium-sized Au particles (∼8.7 nm). The relationship between structure and catalytic performance is supported by experimental and theoretical methods. (1) First, medium-sized Au NPs promote photon absorption, and have a suitable built-in electric field at the heterojunction, which can be successfully tuned to achieve a more efficient h+–e spatial separation. (2) Second, medium-sized Au NPs enhance O2 adsorption, and create selective 2e O2 reduction reaction sites. (3) Particularly, medium-sized Au NPs promote the desorption of produced H2O2 and inhibit H2O2 decomposition, finally leading to the highest H2O2 selectivity. Excellent catalytic performance will be obtained by finely optimizing the particle size in a certain range. This work provides a new idea for preparing high efficiently photocatalysts for H2O2 production.

中文翻译:

Au/C3N4 上的可见光驱动 H2O2 合成:中等大小的 Au 纳米粒子表现出合适的内置电场并抑制 H2O2 逆分解

可见光驱动的 H 2 O 2生产具有可持续性和环境友好性的独特优点。贵金属纳米粒子 (NPs) 的大小决定了它们的分散性和电子结构,并极大地影响了它们的光催化活性。在这项工作中,C 3 N 4上的一系列尺寸 Au NP被调制用于 H 2 O 2生产。结果表明,随着Au粒径的减小,H 2 O 2 呈火山喷发趋势,最高H 2 O 2生成速率1052 μmol g −1 h −1是从中等大小的 Au 颗粒 (~8.7 nm) 中获得的。结构和催化性能之间的关系得到实验和理论方法的支持。(1) 首先,中等大小的 Au NPs 促进光子吸收,并在异质结处具有合适的内置电场,可以成功地对其进行调谐以实现更有效的 h + –e -空间分离。(2) 其次,中等大小的 Au NPs 增强了 O 2吸附,并产生选择性的 2e - O 2还原反应位点。(3) 特别是,中等大小的 Au NPs 促进产生的 H 2 O 2的解吸并抑制 H 2 O 2分解,最终导致最高的 H 2 O 2选择性。通过在一定范围内精细优化粒径,将获得优异的催化性能。该工作为制备H 2 O 2高效光催化剂提供了新思路。
更新日期:2022-11-18
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