三聚氰胺泡沫支撑的S型硫铟锌镉/硫掺杂氮化碳异质结的绿色H<sub>2</sub>O<sub>2</sub>合成：协同界面电荷转移调控与局域光热效应

引用本文: 王伟康, 吴亚栋, 张建军, 孟凯, 李金河, 王乐乐, 刘芹芹. 三聚氰胺泡沫支撑的S型硫铟锌镉/硫掺杂氮化碳异质结的绿色H₂O₂合成：协同界面电荷转移调控与局域光热效应[J]. 物理化学学报, 2025, 41(8): 100093. doi: 10.1016/j.actphy.2025.100093 shu

Citation: Weikang Wang, Yadong Wu, Jianjun Zhang, Kai Meng, Jinhe Li, Lele Wang, Qinqin Liu. Green H₂O₂ synthesis via melamine-foam supported S-scheme Cd_0.5Zn_0.5In₂S₄/S-doped carbon nitride heterojunction: synergistic interfacial charge transfer and local photothermal effect[J]. Acta Physico-Chimica Sinica, 2025, 41(8): 100093. doi: 10.1016/j.actphy.2025.100093 shu

三聚氰胺泡沫支撑的S型硫铟锌镉/硫掺杂氮化碳异质结的绿色H₂O₂合成：协同界面电荷转移调控与局域光热效应

王伟康 ^1, ,
吴亚栋 ^1, ,
张建军 ^{2,
,} ,
孟凯 ^3, ,
李金河 ^1, ,
王乐乐 ^1, ,
刘芹芹 ^{1,
,}

1.
江苏大学, 材料科学与工程学院, 江苏镇江 212013
2.
中国地质大学(武汉), 材料与化学学院, 太阳燃料实验室, 湖北武汉 430078
3.
武汉理工大学, 材料复合新技术国家重点实验室, 湖北武汉 430070

通讯作者: 张建军, zhangjianjun@cug.edu.com; 刘芹芹, qqliu@ujs.edu.cn

基金项目:
国家自然科学基金 22472069

国家自然科学基金 22102064

国家自然科学基金 22302080

纳米材料与技术安徽省重点实验室 202305a12020006

摘要: 绿色光催化合成过氧化氢(H₂O₂)是替代高能耗蒽醌工艺的理想途径，但其在无牺牲剂体系中受限于快速载流子复合与氧化还原能力不足。本研究报道了一种原位化学浴-水热法制备的三聚氰胺泡沫(MF)负载的硫掺杂氮化碳(SCN)/硫空位修饰硫铟锌镉(CZIS)S型异质结(CZIS/SCN/MF)，用于无牺牲剂H₂O₂光合成。通过原位辐照X射线光电子能谱(XPS)、自由基捕获电子顺磁共振(EPR)、飞秒瞬态吸收光谱(fs-TA)及理论计算，证实了其S型电荷转移机制。具体而言，硫掺杂可调控氮化碳骨架的局域电荷分布，强化SCN/CZIS异质结界面内建电场；同时，CZIS中煅烧引入的硫空位作为光电子陷阱促进电荷分离，并保留光生空穴用于H₂O氧化，从而实现无牺牲剂H₂O₂合成。结合MF三维多孔框架的光热效应，优化S掺杂浓度和SCN用量的CZIS/SCN/MF催化剂在纯水中H₂O₂产率达3.46 mmol·g⁻¹·h⁻¹，显著优于多数无牺牲剂体系。该研究为无牺牲剂光催化体系中的界面电荷协同调控与能量转换强化提供了新策略。

关键词:

English

Green H₂O₂ synthesis via melamine-foam supported S-scheme Cd_0.5Zn_0.5In₂S₄/S-doped carbon nitride heterojunction: synergistic interfacial charge transfer and local photothermal effect

Weikang Wang ^1, ,
Yadong Wu ^1, ,
Jianjun Zhang ^{2,
,} ,
Kai Meng ^3, ,
Jinhe Li ^1, ,
Lele Wang ^1, ,
Qinqin Liu ^{1,
,}

1.
School of Materials Science and Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu Province, China
2.
Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, Wuhan 430078, Hubei Province, China
3.
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, Hubei Province, China

Corresponding author: Email: zhangjianjun@cug.edu.com; Tel.: +86-13921581597 (J. Zhang); Email: qqliu@ujs.edu.cn (Q. Liu)

Received Date: 13 March 2025
Accepted Date: 10 April 2025
Revised Date: 01 April 2025
Available Online: 15 August 2025
Fund Project:
the Natural Science Foundation of China

the Natural Science Foundation of China

the Natural Science Foundation of China

Anhui Key Laboratory of Nanomaterials and Nanotechnology, the Major Science and Technology Projects in Anhui Province

Abstract: Green photocatalytic synthesis of hydrogen peroxide (H₂O₂) represents a promising alternative to the energy-intensive anthraquinone process, yet it is hindered by rapid carrier recombination and insufficient redox capacity in sacrificial-agent-free systems. This work reports a melamine foam (MF)-supported sulfur (S)-doped carbon nitride (SCN)/S vacancy-modified Cd_0.5Zn_0.5In₂S₄ (CZIS) S-scheme heterojunction (CZIS/SCN/MF) via an in situ chemical bath-hydrothermal method for sacrificial-agent-free H₂O₂ photosynthesis. The S-scheme charge transfer mechanism was confirmed by in situ irradiated X-ray photoelectron spectroscopy, free-radical trapping electron paramagnetic resonance, femtosecond transient absorption spectra and theoretical calculations. Specifically, the sulfur doping could modulate the local charge distribution of the carbon nitride framework to reinforce the interfacial built-in electric field for the CZIS/SCN S-scheme heterojunction. Meanwhile, the calcination-induced S-vacancies in CZIS could serve as photoelectron traps, promoting charge separation, and reserving photoinduced holes for H₂O oxidation, thereby achieving sacrificial-agent-free H₂O₂ synthesis. Coupled with the photothermal effect of MF's three-dimensional porous framework, the CZIS/SCN/MF catalyst with optimized S-doping density and SCN dosage delivers an H₂O₂ production rate of 3.46 mmol·g⁻¹·h⁻¹ in pure water, surpassing most of the sacrificial-agent-free systems. This study proposes a novel strategy for synergistic interfacial charge regulation and energy conversion enhancement in sacrificial-agent-free photocatalytic systems.

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沈阳化工大学材料科学与工程学院沈阳 110142

三聚氰胺泡沫支撑的S型硫铟锌镉/硫掺杂氮化碳异质结的绿色H₂O₂合成：协同界面电荷转移调控与局域光热效应

通讯作者: 张建军, zhangjianjun@cug.edu.com; 刘芹芹, qqliu@ujs.edu.cn

English

Green H₂O₂ synthesis via melamine-foam supported S-scheme Cd_0.5Zn_0.5In₂S₄/S-doped carbon nitride heterojunction: synergistic interfacial charge transfer and local photothermal effect

Corresponding author: Email: zhangjianjun@cug.edu.com; Tel.: +86-13921581597 (J. Zhang); Email: qqliu@ujs.edu.cn (Q. Liu)

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

三聚氰胺泡沫支撑的S型硫铟锌镉/硫掺杂氮化碳异质结的绿色H2O2合成：协同界面电荷转移调控与局域光热效应

通讯作者: 张建军, zhangjianjun@cug.edu.com; 刘芹芹, qqliu@ujs.edu.cn

English

Green H2O2 synthesis via melamine-foam supported S-scheme Cd0.5Zn0.5In2S4/S-doped carbon nitride heterojunction: synergistic interfacial charge transfer and local photothermal effect

Corresponding author: Email: zhangjianjun@cug.edu.com; Tel.: +86-13921581597 (J. Zhang); Email: qqliu@ujs.edu.cn (Q. Liu)

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

文章相关

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

三聚氰胺泡沫支撑的S型硫铟锌镉/硫掺杂氮化碳异质结的绿色H₂O₂合成：协同界面电荷转移调控与局域光热效应

Green H₂O₂ synthesis via melamine-foam supported S-scheme Cd_0.5Zn_0.5In₂S₄/S-doped carbon nitride heterojunction: synergistic interfacial charge transfer and local photothermal effect

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs