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1.济南大学水利与环境学院,山东 济南 250022
2.潍坊市科技创新促进中心,山东 潍坊 261061
3.山东省黄河三角洲生态环境重点实验室,山东 滨州 256603
Received:24 January 2026,
Revised:2026-04-28,
Accepted:29 April 2026,
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YANG Jiarun, ZHENG Bo, HE Xuanrui, et al. Pt nanoclusters/rich-nitrogen C3N5 with strong electron accumulation for photocatalytic oxygen reduction to produce H2O2[J/OL]. CIESC Journal, 2026.
YANG Jiarun, ZHENG Bo, HE Xuanrui, et al. Pt nanoclusters/rich-nitrogen C3N5 with strong electron accumulation for photocatalytic oxygen reduction to produce H2O2[J/OL]. CIESC Journal, 2026. DOI: 10.11949/0438-1157.20260117.
光催化氧还原生产高价值工业化合物过氧化氢(H
2
O
2
)是一种绿色经济的方法,但高效合成H
2
O
2
需要设计高活性光催化剂,并深入了解氧还原反应机理。通过原位还原法在富氮型氮化碳(C
3
N
5
)表面构筑高度分散Pt纳米簇,显著提高了光催化氧还原生成H
2
O
2
活性。Pt纳米簇均匀沉积于C
3
N
5
片层表面,并以Pt
2+
/Pt
4+
氧化态存在,具备强电子富集特征和表面拉曼增强效应。Pt的引入导致体系的能带收缩,带隙宽度从2.55 eV降至2.39 eV,Pt与C
3
N
5
间形成以内建电场为基础的肖特基结,有效促进光生电子在Pt纳米簇表面富集并阻断其复合途径。可见光照射下Pt/C
3
N
5
复合体系60 min时H
2
O
2
产量可达505 μmol·g⁻
1
,是单独C
3
N
5
的4.0倍,且循环稳定性良好。机制研究表明,催化剂表面吸附O
2
为主要电子还原基底,超氧自由基(·O
2
⁻)为关键中间体,反应按照两电子路径经过氧自由基最终生成H
2
O
2
。研究阐明了Pt纳米簇/富氮C
3
N
5
复合光催化体系高效产H
2
O
2
的界面电子机制,为低贵金属、高选择性光催化体系设计提供重要参考。
Photocatalytic oxygen reduction represents a sustainable and economically viable route for the production of hydrogen peroxide (H
2
O
2
)
yet its practical application requires the development of highly active photocatalysts and a mechanistic understanding of the reaction pathway. Herein
highly dispersed Pt nanoclusters on nitrogen-rich C
3
N
5
have been constructed via an in-situ reduction strategy
achieving a pronounced enhancement in photocatalytic H
2
O
2
generation. The Pt species are uniformly anchored on the C
3
N
5
nanosheets in an “island-like” nanocluster configuration and predominantly exist in Pt
2+
/Pt
4+
oxidation states
exhibiting strong electron-enrichment behavior and evident surface-enhanced Raman characteristics. The introduction of Pt leads to the contraction of the energy band in the system
and the band gap width decreases from 2.55 eV to 2.39 eV. The intimate Pt/C
3
N
5
interface gives rise to a Schottky junction with a built-in electric field
which facilitates the rapid accumulation and directional transfer of photogenerated electrons toward Pt nanoclusters while effectively suppressing electron–hole recombination. Under visible light irradiation
the H
2
O
2
production of the Pt/C
3
N
5
composite system reached 505 μmol·g⁻
1
after 60 minutes
which was 4.0 times that of the C
3
N
5
alone. The Pt/C
3
N
5
composite maintains excellent cycling stability. Mechanistic investigations reveal that molecular oxygen adsorbed on the catalyst surface acts as the primary electron acceptor
with superoxide radical (·O
2
⁻) identified as the key intermediate. The reaction proceeds via a two-electron oxygen reduction pathway
ultimately yielding H
2
O
2
through successive radical-mediated steps. This work elucidates the interfacial electronic mechanism underpinning the superior H
2
O
2
productivity of Pt/C
3
N
5
and offers meaningful guidance for the rational design of low–noble–metal
high-selectivity photocatalytic systems for sustainable H
2
O
2
production.
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