H2O及其中间体在缺电子Mn(3+δ)+位的自发增强吸附及其促进光催化产H2O2性能

引用本文: 尹鑫宇, 石海洋, 王玉, 王雪飞, 王苹, 余火根. H₂O及其中间体在缺电子Mn^{(3+^δ)+}位的自发增强吸附及其促进光催化产H₂O₂性能[J]. 物理化学学报, 2024, 40(10): 231200. doi: 10.3866/PKU.WHXB202312007 shu

Citation: Xinyu Yin, Haiyang Shi, Yu Wang, Xuefei Wang, Ping Wang, Huogen Yu. Spontaneously Improved Adsorption of H₂O and Its Intermediates on Electron-Deficient Mn^(3+δ)+ for Efficient Photocatalytic H₂O₂ Production[J]. Acta Physico-Chimica Sinica, 2024, 40(10): 231200. doi: 10.3866/PKU.WHXB202312007 shu

H₂O及其中间体在缺电子Mn^{(3+^δ)+}位的自发增强吸附及其促进光催化产H₂O₂性能

尹鑫宇 ^1, ,
石海洋 ^1, ,
王玉 ^1, ,
王雪飞 ^{1,
,} ,
王苹 ^1, ,
余火根 ^{2,
,}

1.
武汉理工大学材料科学与工程学院和化学化工与生命科学学院, 武汉 430070;
2.
中国地质大学(武汉)材料与化学学院太阳燃料实验室, 武汉 430078

通讯作者: 王雪飞,Email:xuefei@whut.edu.cn; 余火根,Email:yuhuogen@cug.edu.cn

基金项目:
国家自然科学基金（22178276，U22A20147，52073263），湖北省自然科学基金（2022CFA001）资助项目

摘要: 过渡金属羟基氧化物已被证明是水氧化反应的可靠助催化剂。然而，在水氧化过程中它们对H₂O及其中间产物的吸附能力不足，极大制约了水氧化速率的提高。在本研究中，H₂O及其中间体在MnOOH助剂的缺电子Mn^（3+δ）+上的自发增强吸附可以极大地促进水的快速氧化，从而在纯水体系中实现高效的光催化H₂O₂生成。首先，无定形MnOOH通过定向光诱导氧化方法选择性地沉积在AuPd改性的单晶BiVO₄光催化剂的（110）面上，从而制备了AuPd/BiVO₄/MnOOH光催化剂。光催化实验表明，所制备的AuPd/BiVO₄/MnOOH （0.5%）光催化剂的H₂O₂产生速率达到214μmol·L^-1，并表现出良好的稳定性和重现性。密度泛函理论计算和X射线光电子能谱表征表明，MnOOH的自由电子可以有效地转移到BiVO₄上，诱导缺电子Mn位（Mn^（3+δ）+）的产生，从而自发地促进H₂O及其中间体的吸附，增强四电子WOR反应，导致H₂O₂的高效生成。本文关于助催化剂与主体催化剂之间强相互作用的工作为其它高效催化材料的合理设计提供了一种新的思路。

关键词:

English

Spontaneously Improved Adsorption of H₂O and Its Intermediates on Electron-Deficient Mn^(3+δ)+ for Efficient Photocatalytic H₂O₂ Production

Xinyu Yin ^1, ,
Haiyang Shi ^1, ,
Yu Wang ^1, ,
Xuefei Wang ^{1,
,} ,
Ping Wang ^1, ,
Huogen Yu ^{2,
,}

1.
School of Materials Science and Engineering, and School of Chemistry, Chemical Engineering and Life Sciences, Wuhan University of Technology, Wuhan 430070, China;
2.
Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, China

Corresponding author: Xuefei Wang, ; Huogen Yu,

Received Date: 06 December 2023
Accepted Date: 10 January 2024
Revised Date: 10 January 2024
Available Online: 15 January 2024
Fund Project:
This work was supported by the National Natural Science Foundation of China (22178276, U22A20147, 52073263) and the Natural Science Foundation of Hubei Province of China (2022CFA001).

Abstract: Transitional metal oxyhydroxides have been demonstrated to be the reliable cocatalysts for water oxidation reaction. However, their insufficient adsorption ability for H₂O and its intermediate products during water oxidation greatly restricts the improvement of water oxidation rate. In this study, a spontaneously improved adsorption of H₂O and its intermediates on the electron-deficient Mn^(3+δ)+ of MnOOH cocatalyst can greatly promote the rapid water oxidation to realize the efficient photocatalytic H₂O₂ production in a pure water system. In this case, amorphous MnOOH is selectively deposited on the (110) facet of AuPd-modified single-crystal BiVO₄ photocatalyst via the directionally photoinduced oxidation approach to produce AuPd/BiVO₄/MnOOH photocatalyst. Photocatalytic experiments exhibit that the as-prepared AuPd/BiVO₄/MnOOH (0.5%) photocatalyst obtains the boosted H₂O₂-evolution rate of 214 μmol·L^-1 as well as exhibits an outstanding stability and reproducibility. Density functional theory calculations and X-ray photoelectron spectroscopy (XPS) characterization reveal that the free electrons of MnOOH can effectively transfer to BiVO₄ to induce the generation of electron-deficient Mn sites (Mn^(3+δ)+), which spontaneously promotes the adsorption of H₂O and its intermediates for enhancing 4-electron water oxidation reaction, resulting in an efficient H₂O₂ production. The present work about the strong interaction between cocatalyst and bulk catalyst provides a fresh idea for the rational design of highly efficient catalytic materials.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

H₂O及其中间体在缺电子Mn^{(3+^δ)+}位的自发增强吸附及其促进光催化产H₂O₂性能

通讯作者: 王雪飞,Email:xuefei@whut.edu.cn; 余火根,Email:yuhuogen@cug.edu.cn

English

Spontaneously Improved Adsorption of H₂O and Its Intermediates on Electron-Deficient Mn^(3+δ)+ for Efficient Photocatalytic H₂O₂ Production

Corresponding author: Xuefei Wang, ; Huogen Yu,

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