化工学报 ›› 2023, Vol. 74 ›› Issue (6): 2458-2467.DOI: 10.11949/0438-1157.20230323

• 催化、动力学与反应器 • 上一篇    下一篇

Ni@C@TiO2核壳双重异质结的构筑及光热催化分解水产氢

李勇1(), 高佳琦1, 杜超1, 赵亚丽1(), 李伯琼1, 申倩倩2, 贾虎生2, 薛晋波2()   

  1. 1.晋中学院材料科学与工程系,轻质材料改性应用山西省协同创新中心,山西 晋中 030619
    2.太原理工大学新材料界面科学与工程教育部重点实验室,山西 太原 030024
  • 收稿日期:2023-04-04 修回日期:2023-06-10 出版日期:2023-06-05 发布日期:2023-07-27
  • 通讯作者: 赵亚丽,薛晋波
  • 作者简介:李勇(1987—),男,博士,讲师,lytyut@126.com
  • 基金资助:
    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)

Construction of Ni@C@TiO2 core-shell dual-heterojunctions for advanced photo-thermal catalytic hydrogen generation

Yong LI1(), Jiaqi GAO1, Chao DU1, Yali ZHAO1(), Boqiong LI1, Qianqian SHEN2, Husheng JIA2, Jinbo XUE2()   

  1. 1.Department of Materials Science and Engineering, Shanxi Province Collaborative Innovation Center for Light Materials Modification and Application, Jinzhong University, Jinzhong 030619, Shanxi, China
    2.Key Laboratory of Interface Science and Engineering in Advanced Materials (Taiyuan University of Technology), Ministry of Education, Taiyuan 030024, Shanxi, China
  • Received:2023-04-04 Revised:2023-06-10 Online:2023-06-05 Published:2023-07-27
  • Contact: Yali ZHAO, Jinbo XUE

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@TiO2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TiO2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/TiO2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1538 μmol·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。

关键词: 催化剂, 制氢, 纳米粒子, 异质结, 等离激元, 核壳结构

Abstract:

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@TiO2 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/TiO2 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 (1538 μmol·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.

Key words: catalyst, hydrogen production, nanoparticles, heterojunction, plasmonic, core-shell

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