Citation: Yu Wang, Haiyang Shi, Zihan Chen, Feng Chen, Ping Wang, Xuefei Wang. 具有富电子Pt^δ^-壳层的空心AgPt@Pt核壳催化剂：提升光催化H₂O₂生成选择性与活性[J]. Acta Physico-Chimica Sinica, ;2025, 41(7): 100081. doi: 10.1016/j.actphy.2025.100081 shu

具有富电子Pt^δ^-壳层的空心AgPt@Pt核壳催化剂：提升光催化H₂O₂生成选择性与活性

Yu Wang ¹ ,
Haiyang Shi ² ,
Zihan Chen ¹ ,
Feng Chen ¹ ,
Ping Wang ¹ ,
Xuefei Wang ¹

1.
School of Materials Science and Engineering, and School of Chemistry, Chemical Engineering and Life Sciences, Wuhan University of Technology, Wuhan 430070, Hubei Province, China;
2.
College of Hydraulic and Environmental Engineering, China Three Gorges University, Yichang 443002, Hubei Province, China

Received Date: 12 February 2025
Revised Date: 8 March 2025
Accepted Date: 17 March 2025

Fund Project: This work was supported by the National Natural Science Foundation of China (22178276), the Postdoctoral Fellowship Program of CPSF (GZC20240888), the National College Students’ Innovation and Entrepreneurship Training Program at Wuhan University of Technology (S202410497023).

铂(Pt)作为优异的氧还原助催化剂，在光催化产H₂O₂方面具有巨大潜力。然而，Pt对O₂的吸附能力过强，易使O―O键裂解，从而降低2电子氧还原反应(ORR)生成H₂O₂的选择性。在本研究中，通过调节助剂结构改变Pt的电子结构，从而削弱Pt―O键的强度。本文通过两步光沉积法在BiVO₄的(010)面上连续修饰了铂和银助催化剂。由于在此过程中存在置换反应，最终合成了一种具有中空AgPt合金核和富电子Pt^δ^-壳(AgPt@Pt)结构的协同催化剂。光催化实验结果表明：修饰空心结构AgPt@Pt助剂的BiVO₄产生H₂O₂的速率达到了1021.5 μmol·L^-1，且其对应的量子效率(AQE)为5.07%，是Pt/BiVO₄光催化剂(35.7 μmol·L^-1)的28.6倍。此外，密度泛函理论计算和X射线光电子能谱表征表明：AgPt合金向Pt壳转移电子，生成富电子的Pt^δ^-活性位点，进而增加了AgPt@Pt助催化剂中Pt―O_ads反键轨道的占有率。这种电子再分布削弱了O₂在Pt上的吸附强度，促进了2电子ORR反应，并显著提高了H₂O₂的生成效率。这一合成策略为制备具有更高H₂O₂选择性的铂基纳米助催化剂提供了可靠的方法。
- Photocatalysis,
- Electron-rich Pt^δ^-,
- O₂-adsorption,
- H₂O₂,
- BiVO₄
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具有富电子Ptδ-壳层的空心AgPt@Pt核壳催化剂：提升光催化H2O2生成选择性与活性

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通讯作者: 陈斌, bchen63@163.com

具有富电子Pt^δ^-壳层的空心AgPt@Pt核壳催化剂：提升光催化H₂O₂生成选择性与活性