摘要
合理设计具有出色光吸收和电荷分离与转移能力的纳米催化剂,实现高效的光催化制氢仍然是一个挑战。借助间苯二酚-甲醛树脂(RF)模板和Ar气氛煅烧工艺构建了三元Ni@C@TiO_(2)核壳双重异质结纳米催化剂,实现了高效热积聚和高通量电荷转移。该体系充分结合了碳层的宽带吸收、Ni纳米粒子(NPs)的等离激元特性以及TiO_(2)的保护和催化功能。在双重异质结中建立了较大的内部电场,使电荷分离效率提高了2.4倍。得益于Ni@C芯光热效应与Ni/C-C/TiO_(2)双重异质结的协同效应,从而实现有效的电荷分离和传输,提高了电荷转移速率;核壳结构的构建降低了体系热量损耗,最终实现高效的太阳能光热转换(光热效率78.0%)和光热催化分解水产氢性能(析氢速率为1538μmol·g^(-1)·h^(-1))的提升。稳健的核壳纳米颗粒可以应用到其他光热催化系统的设计中,为开发更高效的全光谱利用型光催化剂提供思路。
Photo-thermal synergistic catalysis coupling photo-chemical and thermo-chemical conversions integrates the benefits of both high driving force of photocatalysis and high selectivity of thermocatalysis.It is one of the most promising methods to enhance its catalytic efficiency.Unfortunately,rapid heat loss and fast charge carrier recombination seriously affect its solar energy utilization and conversion efficiency.Herein,a hierarchical Ni@C@TiO_(2)core-shell dual-heterojunctions is prepared by resorcinol formaldehyde(RF)template and Ar calcination process to realize efficient heat accumulation and high-flux charge transfer for achieving advanced photo-thermal catalytic hydrogen performance.This system fully combines the broadband absorption of carbon layer and plasmonic property of Ni core.A giant internal electric field(IEF)in the dual-heterojunctions is built,enabling the charge transfer efficiency to be enhanced by 2.4 times.Benefiting from the synergistic effect between Ni@C core photo-thermal effect and Ni/C and C/TiO_(2)dual-heterojunctions,an excellent photo-thermal efficiency of 78.0%and the performance of photo-thermal catalytic water splitting for hydrogen production hydrogen evolution rate is(1538μmol·g-1·h-1)are eventually improved.Robust core-shell nanoparticles can be applied to the design of other photo-thermal catalytic systems,providing ideas for the development of more efficient full-spectrum utilization photocatalysts.
作者
李勇
高佳琦
杜超
赵亚丽
李伯琼
申倩倩
贾虎生
薛晋波
LI Yong;GAO Jiaqi;DU Chao;ZHAO Yali;LI Boqiong;SHEN Qianqian;JIA Husheng;XUE Jinbo(Department of Materials Science and Engineering,Shanxi Province Collaborative Innovation Center for Light Materials Modification and Application,Jinzhong University,Jinzhong 030619,Shanxi,China;Key Laboratory of Interface Science and Engineering in Advanced Materials(Taiyuan University of Technology),Ministry of Education,Taiyuan 030024,Shanxi,China)
出处
《化工学报》
EI
CSCD
北大核心
2023年第6期2458-2467,共10页
CIESC Journal
基金
国家自然科学基金项目(62105131)
山西省自然科学基金项目(202203021212508)
山西省科技创新青年人才团队项目(202204051001005)
晋中市科技重点研发项目(Y201027)
山西省高等学校科技创新项目(2022L491,2022L492)。
关键词
催化剂
制氢
纳米粒子
异质结
等离激元
核壳结构
catalyst
hydrogen production
nanoparticles
heterojunction
plasmonic
core-shell
作者简介
第一作者:李勇(1987-),男,博士,讲师,lytyut@126.com;通信作者:薛晋波(1982-),男,博士,副教授,xuejinbo@tyut.edu.cn;通信作者:赵亚丽(1981-),女,博士,教授,yaliz12@163.com。
