物理化学学报2025，Vol.41Issue(8)：137-148,12.DOI:10.1016/j.actphy.2025.100093
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 Cd0.5Zn0.5In2S4/S-doped carbon nitride heterojunction:synergistic interfacial charge transfer and local photothermal effect
摘要
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 Cd0.5Zn0.5In2S4(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.关键词
S型异质结/过氧化氢合成/光热效应/三聚氰胺泡沫/无牺牲试剂Key words
S-scheme heterojunction/H2O2 production/Photothermal effect/Melamine foam/Sacrificial-Agent-Free分类
化学化工引用本文复制引用
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):137-148,12.基金项目
This work was supported by the Natural Science Foundation of China(22472069,22102064,22302080)and Anhui Key Laboratory of Nanomaterials and Nanotechnology,the Major Science and Technology Projects in Anhui Province(202305a12020006).国家自然科学基金(22472069,22102064,22302080),纳米材料与技术安徽省重点实验室资助(202305a12020006) （22472069,22102064,22302080）
