Pt纳米簇/富氮C3N5强富电子特征及光催化氧还原产H2O2性能

杨佳润; 郑波; 何萱瑞; 张琳; 马东; 王仲鹏

doi:10.11949/0438-1157.20260117

您当前的位置：

首页 >

文章列表页 >

Pt纳米簇/富氮C₃N₅强富电子特征及光催化氧还原产H₂O₂性能

催化、动力学与反应器 | 更新时间：2026-08-21

- Pt纳米簇/富氮C₃N₅强富电子特征及光催化氧还原产H₂O₂性能
- Pt nanoclusters/nitrogen-rich C₃N₅ with strong electron accumulation for photocatalytic oxygen reduction to produce H₂O₂
- 化工学报 2026年77卷第7期页码：3926-3935
- 作者机构：
  
  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
- 作者简介：
  
  杨佳润（2002—），男，硕士研究生，yangjr2026@163.com
  郑波（1972—），男，副教授，bo.zheng@pku-iaas.edu.cn
  马东（1981—），男，教授，madong8088@126.com
- 基金信息：
  
  国家自然科学基金项目(42077120)
- DOI：10.11949/0438-1157.20260117
  中图分类号： X 703;O 643
- 收稿：2026-01-24，
  
  修回：2026-03-13，
  
  网络首发：2026-08-20，
  
  纸质出版：2026-07-25
- 稿件说明：
移动端阅览
杨佳润, 郑波, 何萱瑞, 张琳, 马东, 王仲鹏. Pt纳米簇/富氮C₃N₅强富电子特征及光催化氧还原产H₂O₂性能[J]. 化工学报, 2026, 77(7): 3926-3935 DOI: 10.11949/0438-1157.20260117.

YANG Jiarun, ZHENG Bo, HE Xuanrui, ZHANG Lin, MA Dong, WANG Zhongpeng. Pt nanoclusters/nitrogen-rich C₃N₅ with strong electron accumulation for photocatalytic oxygen reduction to produce H₂O₂[J]. CIESC Journal, 2026, 77(7): 3926-3935 DOI: 10.11949/0438-1157.20260117.
杨佳润, 郑波, 何萱瑞, 张琳, 马东, 王仲鹏. Pt纳米簇/富氮C₃N₅强富电子特征及光催化氧还原产H₂O₂性能[J]. 化工学报, 2026, 77(7): 3926-3935 DOI: 10.11949/0438-1157.20260117. DOI：

YANG Jiarun, ZHENG Bo, HE Xuanrui, ZHANG Lin, MA Dong, WANG Zhongpeng. Pt nanoclusters/nitrogen-rich C₃N₅ with strong electron accumulation for photocatalytic oxygen reduction to produce H₂O₂[J]. CIESC Journal, 2026, 77(7): 3926-3935 DOI: 10.11949/0438-1157.20260117. DOI：

摘要

光催化氧还原生产高价值工业化合物过氧化氢（H

）是一种绿色经济的方法，但高效合成H

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

）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

活性。Pt纳米簇均匀沉积于C

片层表面，并以Pt

/Pt

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

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

复合体系60 min时H

产量可达505 μmol·g

-1

，是C

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

为主要电子还原基底，超氧自由基（·O

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=116041878&type=

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=116041865&type=

1.10066664

3.89466691

）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

。研究阐明了Pt纳米簇/富氮C

复合光催化体系高效产H

的界面电子机制，可为低贵金属、高选择性光催化体系设计提供参考。

Abstract

Photocatalytic oxygen reduction represents a sustainable and economically viable route for the production of hydrogen peroxide (H

)

yet its practical application requires the development of highly active photocatalysts and a mechanistic understanding of the reaction pathway. Highly dispersed Pt nanoclusters were constructed on the surface of nitrogen-rich carbon nitride (C

) using an

situ

reduction method

significantly improving the photocatalytic oxygen reduction activity for H

production. The Pt species are uniformly anchored on the C

nanosheets in an "island-like" nanocluster configuration and predominantly exist in Pt

/Pt

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

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

production of the Pt/C

composite system reached 505 μmol·g

-1

after 60 min

which was 4.0 times that of the C

. The Pt/C

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

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=116041880&type=

https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=116041891&type=

1.18533325

4.48733330

) identified as the key intermediate. The reaction proceeds

via

a two-electron oxygen reduction pathway

ultimately yielding H

through successive radical-mediated steps. This work elucidates the interfacial electronic mechanism underpinning the superior H

productivity of Pt/C

and offers meaningful guidance for the rational design of low-noble-metal

high-selectivity photocatalytic systems for sustainable H

production.

关键词

Keywords

references

Yong Z J , Ma T Y . Solar-to-H 2 O 2 catalyzed by covalent organic frameworks [J ] . Angewandte Chemie International Edition , 2023 , 62 ( 49 ): e202308980 .

Shi X J , Back S , Gill T M , et al . Electrochemical synthesis of H 2 O 2 by two-electron water oxidation reaction [J ] . Chem , 2021 , 7 ( 1 ): 38 - 63 .

Ingle A A , Ansari S Z , Shende D Z , et al . Progress and prospective of heterogeneous catalysts for H 2 O 2 production via anthraquinone process [J ] . Environmental Science and Pollution Research , 2022 , 29 ( 57 ): 86468 - 86484 .

Qu S Y , Wu H , Ng Y H . Clean production of hydrogen peroxide: a heterogeneous solar-driven redox process [J ] . Advanced Energy Materials , 2023 , 13 ( 36 ): 2301047 .

Wang C H , Zhang X T , Liu Y C . Promotion of multi-electron transfer for enhanced photocatalysis: a review focused on oxygen reduction reaction [J ] . Applied Surface Science , 2015 , 358 : 28 - 45 .

Sun X , Yang J D , Zeng X K , et al . Pairing oxygen reduction and water oxidation for dual-pathway H 2 O 2 production [J ] . Angewandte Chemie International Edition , 2024 , 63 ( 52 ): e202414417 .

Liu Y , Hao X Q , Hu H Q , et al . High efficiency electron transfer realized over NiS 2 /MoSe 2 S-scheme heterojunction in photocatalytic hydrogen evolution [J ] . Acta Physico Chimica Sinica , 2021 , 37 ( 6 ): 2008030

Liu J H , Xie S Y , Geng Z B , et al . Carbon nitride supramolecular hybrid material enabled high-efficiency photocatalytic water treatments [J ] . Nano Letters , 2016 , 16 ( 10 ): 6568 - 6575 .

Li K , Cai W , Zhang Z C , et al . Boron doped C 3 N 5 for photocatalytic nitrogen fixation to ammonia: the key role of boron in nitrogen activation and mechanism [J ] . Chemical Engineering Journal , 2022 , 435 : 135017 .

Deng Y C , Li L , Zeng H , et al . Unveiling the origin of high-efficiency charge transport effect of C 3 N 5 /C 3 N 4 homojunction for activating peroxymonosulfate to degrade atrazine under visible light [J ] . Chemical Engineering Journal , 2023 , 457 : 141261 .

Cheng Q , Li J P , Huang Y X , et al . Verifying the unique charge migration pathway in polymeric homojunctions for artificial photosynthesis of hydrogen peroxide [J ] . Advanced Science , 2025 , 12 ( 16 ): 2500218 .

Zhang J K , Yu Z B , Gao Z , et al . Porous TiO 2 nanotubes with spatially separated platinum and CoO x cocatalysts produced by atomic layer deposition for photocatalytic hydrogen production [J ] . Angewandte Chemie International Edition , 2017 , 56 ( 3 ): 816 - 820 .

Zhang N , Wang B Z , Hu P C , et al . Achieve high-efficiency photocatalytic hydrogen production of MCNTs-CdS/Pt/ZnFe 2 O 4 heterojunction owing to building charge transport bridge [J ] . Journal of Environmental Chemical Engineering , 2025 , 13 ( 2 ): 115800 .

Cheng X , Wang Y S , Lu Y , et al . Single-atom alloy with Pt-Co dual sites as an efficient electrocatalyst for oxygen reduction reaction [J ] . Applied Catalysis B: Environmental , 2022 , 306 : 121112 .

Zhang L , Doyle-Davis K , Sun X L . Pt-based electrocatalysts with high atom utilization efficiency: from nanostructures to single atoms [J ] . Energy & Environmental Science , 2019 , 12 ( 2 ): 492 - 517 .

Cheng C , He B W , Fan J J , et al . An inorganic/organic S-scheme heteroj unction H 2 -production photocatalyst and its charge transfer mechanism [J ] . Advanced Materials , 2021 , 33 ( 22 ): 2100317 .

Wu Y C , Wei W , Yu R H , et al . Anchoring sub-nanometer Pt clusters on crumpled paper-like MXene enables high hydrogen evolution mass activity [J ] . Advanced Functional Materials , 2022 , 32 ( 17 ): 2110910 .

Wang Y , Liu X H , Wang Q K , et al . Insights into charge transfer at an atomically precise nanocluster/semiconductor interface [J ] . Angewandte Chemie International Edition , 2020 , 59 ( 20 ): 7748 - 7754 .

Cui E T , Lu Y L , Li Z X , et al . Unveiling the charge transfer dynamics regulated by bonding evolution in single-atom Pt/C 3 N 5 for boosting hydrogen evolution [J ] . Applied Catalysis B: Environment and Energy , 2024 , 347 : 123806 .

Zhong W , Meng A Y , Su Y R , et al . Achieving free-electron transfer reversal and <math id="M14"><msub><mrow><mi>d</mi></mrow><mrow><msup><mrow><mi>z</mi></mrow><mrow><mn mathvariant="normal">2</mn></mrow></msup></mrow></msub></math> https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=116041983&type= https://html.publish.founderss.cn/rc-pub/api/common/picture?pictureId=116041962&type= 2.79399991 2.96333337 -orbital occupancy modulation on core-shell NiS@Au cocatalysts for highly selective H 2 O 2 photosynthesis [J ] . Angewandte Chemie International Edition , 2025 , 64 ( 20 ): e202425038 .

Zhu Q , Su J J , Lin G A , et al . Surface indium vacancies promote photocatalytic H 2 O 2 production over In 2 S 3 [J ] . Nature Communications , 2025 , 16 : 10501 .

Dong C Y , Lian C , Hu S C , et al . Size-dependent activity and selectivity of carbon dioxide photocatalytic reduction over platinum nanoparticles [J ] . Nature Communications , 2018 , 9 : 1252 .

Jeon Y J , Kang S J , Joo S H , et al . Pyridinic-to-graphitic conformational change of nitrogen in graphitic carbon nitride by lithium coordination during lithium plating [J ] . Energy Storage Materials , 2020 , 31 : 505 - 514 .

Mueller N S , Pfitzner E , Okamura Y , et al . Surface-enhanced Raman scattering and surface-enhanced infrared absorption by plasmon polaritons in three-dimensional nanoparticle supercrystals [J ] . ACS Nano , 2021 , 15 ( 3 ): 5523 - 5533 .

Wei J H , Huang M F , Yu K , et al . Water-mediated recycling of gold, palladium and platinum using semimetallic TiS 2 and TaS 2 nanosheets [J ] . National Science Review , 2026 , 13 ( 1 ): nwaf522 .

Hu J M , Fan Y J , Li S J , et al . Ultrathin porous carbon nitride anchored with Pt nanoclusters for synergistic enhancement of hydrogen production in alkaline photocatalytic polyester reforming [J ] . Small , 2024 , 20 ( 49 ): 2403573 .

Kwon H , Choi H , Yoon Y , et al . Electronic switching between hot electrons and hot holes via Schottky junctions during chemical reactions [J ] . ACS Nano , 2025 , 19 ( 11 ): 11450 - 11462 .

Sridhar V , Podjaski F , Kröger J , et al . Carbon nitride-based light-driven microswimmers with intrinsic photocharging ability [J ] . Proceedings of the National Academy of Sciences of the United States of America , 2020 , 117 ( 40 ): 24748 - 24756 .

Bai C W , Liu L L , Chen J J , et al . Circumventing bottlenecks in H 2 O 2 photosynthesis over carbon nitride with iodine redox chemistry and electric field effects [J ] . Nature Communications , 2024 , 15 : 4718 .

浏览量

下载量

CSCD

文章被引用时，请邮件提醒。

提交

工具集

关联资源

多孔TiO2/g-C3N4异质结的制备及其光催化辅酶再生性能研究

C元素修饰g-C3N4对TiO2的调控及复合材料光催化产氢性能研究

BiOBr的形貌调控及其光催化CO2还原性能的研究

直接Z型异质结体系光催化还原二氧化碳研究进展

制备方法对硅藻土负载镍钇双金属催化剂加氢性能的影响