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

引用本文: 王玉, 石海洋, 陈子涵, 陈峰, 王苹, 王雪飞. 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]. 物理化学学报, 2025, 41(7): 100081. doi: 10.1016/j.actphy.2025.100081 shu

Citation: Yu Wang, Haiyang Shi, Zihan Chen, Feng Chen, Ping Wang, Xuefei Wang. Hollow AgPt@Pt core-shell cocatalyst with electron-rich Pt^δ^- shell for boosting selectivity of photocatalytic H₂O₂ production for faceted BiVO₄[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

王玉 ^1, ,
石海洋 ^2, ,
陈子涵 ^1, ,
陈峰 ^1, ,
王苹 ^1, ,
王雪飞 ^1,

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, 湖北武汉 430070;
2.
三峡大学水利与环境学院, 湖北宜昌 443002
基金项目:
国家自然科学基金(22178276),国家资助博士后研究人员计划(GZC20240888)和武汉理工大学国家大学生创新创业训练计划(S202410497023)资助

摘要: 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。

关键词:

English

Hollow AgPt@Pt core-shell cocatalyst with electron-rich Pt^δ^- shell for boosting selectivity of photocatalytic H₂O₂ production for faceted BiVO₄

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
Accepted Date: 17 March 2025
Revised Date: 08 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).

Abstract: Platinum (Pt) is an excellent oxygen reduction cocatalyst with great potential for the photocatalytic production of H₂O₂. However, its catalytic efficiency is limited by the strong adsorption of O₂, which facilitates O―O bond cleavage and reduces selectivity for the 2-electron oxygen reduction reaction (ORR). Fortunately, the strength of the Pt―O bond can be weakened by adjusting the structure of the cocatalyst to modify the electronic structure of Pt. In this paper, Pt and Ag cocatalysts are successively modified on the (010) facet of BiVO₄ through a two-step photodeposition method. Due to the occurrence of a displacement reaction during the process, a synergistic catalyst with a hollow AgPt alloy core and an electron-rich Pt^δ^- shell (AgPt@Pt) structure is ultimately synthesized. Photocatalytic experiments demonstrated that the H₂O₂ production from BiVO₄ modified with hollow AgPt@Pt reached an impressive 1021.5 μmol·L^-1. This corresponds to an AQE of 5.1%, which is 28.6 times higher than that of the Pt/BiVO₄ photocatalyst with only 35.7 μmol·L^-1. Furthermore, research results show that AgPt can transfer electrons to the Pt shell to generate electron-rich Pt^δ^- active sites, thus increasing the antibonding orbital occupancy of Pt―O_ads in AgPt@Pt catalysts. This electron redistribution weakens the adsorption strength of O₂ on Pt, promoting the 2-electron ORR and facilitating the efficient generation of H₂O₂. This synthesis strategy offers a versatile approach for preparing other Pt-based nano-alloy cocatalysts with improved activity for the selective reduction of O₂ to H₂O₂.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

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

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Hollow AgPt@Pt core-shell cocatalyst with electron-rich Pt^δ^- shell for boosting selectivity of photocatalytic H₂O₂ production for faceted BiVO₄

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