催化学报 ›› 2020, Vol. 41 ›› Issue (12): 1791-1811.DOI: 10.1016/S1872-2067(20)63652-X

• 综述 • 上一篇    下一篇

负载型金属纳米催化剂的可持续构筑及其电催化析氢应用

陈倩a, 聂瑶b, 明媚a,c, 樊光银a, 张云a, 胡劲松c   

  1. a 四川师范大学化学与材料科学学院, 四川成都 610068;
    b 重庆师范大学化学学院, 重庆 410033;
    c 中国科学院化学研究所, 中国科学院分子纳米结构与纳米技术重点实验室, 北京分子科学研究中心, 北京 100190
  • 收稿日期:2020-02-07 修回日期:2020-03-30 出版日期:2020-12-18 发布日期:2020-08-14
  • 通讯作者: 张云, 樊光银
  • 基金资助:
    国家自然科学基金(21905187,21777109);绿色催化四川省高等学校重点实验室(LZJ1802);重庆师范大学拔尖青年人才工程(02030307-0075).

Sustainable synthesis of supported metal nanocatalysts for electrochemical hydrogen evolution

Qian Chena, Yao Nieb, Mei Minga,c, Guangyin Fana, Yun Zhanga, Jin-Song Huc   

  1. a College of Chemistry and Materials Science, Sichuan Normal University, Chengdu 610068, Sichuan, China;
    b College of Chemistry, Chongqing Normal University, Chongqing 410033, China;
    c Beijing National Laboratory for Molecular Sciences(BNLMS), CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, Institute of Chemistry, Chinese Academy of Sciences(CAS), Beijing 100190, China
  • Received:2020-02-07 Revised:2020-03-30 Online:2020-12-18 Published:2020-08-14
  • Supported by:
    This work was supported by the National Natural Science Foundation of China (21905187, 21777109), Key Laboratory of Green Catalysis of Higher Education Institutes of Sichuan (LZJ1802), and Top-notch youth Talent project of Chongqing Normal University (02030307-0075).

摘要: 在众多非均相催化剂中,负载型金属纳米催化剂(SMNCs)因具有高效、稳定、可循环使用等特性而广泛应用于多相催化反应领域.近几十年来,研究者们致力于合理设计和优化载体和颗粒等来提高SMNCs催化性能.其中,通过传统方法(如沉淀法、溶胶-凝胶法、溶剂热法、高温热解法等)成功开发了种类繁多的SMNCs,然而这些传统方法通常会涉及大量的有机试剂、复杂的制备步骤以及昂贵的专用设备,极大地限制了SMNCs的规模化生产.因此,发展简便、高效的绿色可持续的SMNCs生成方法意义重大.本文总结了绿色、可持续化生产SMNCs的几种方法,包括固态合成法、低温热解法、无表面活性剂和还原剂合成法及离子液体辅助合成法.与传统合成技术相比,这些方法在可持续性方面、原子利用率方面、产物选择性方面及规模化生产方面表现出明显的优势.此外,本文还对SMNCs的经典应用-电催化产氢(HER)技术的研究进展进行了详细评述.尽管SMNCs的可持续化合成及其大规模应用已取得较大进展,但目前仍存在几个关键问题需不断改进:如何进一步提高绿色、可持续化生产效率?如何调控金属纳米颗粒的载量及粒径尺寸?如何调节金属纳米颗粒的表面状态?如何探究催化剂结构与活性之间的构效关系?探究上述问题对实现SMNCs的规模化生产及实际应用有着十分重要的现实意义.此外,SMNCs在设计时应遵循协同构建大量的有效活性位和快速的电子传输通道,协同调控金属纳米颗粒的表面状态、颗粒大小和晶面以及载体和助催化剂的组成和结构.目前报道的大多数SMNCs仅局限于负载型贵金属(Ru,Rh,Ir,Pt等)类,对此,我们未来的研究工作应在降低成本、保护环境、规模化生产的基础上将SMNCs拓宽至非贵金属类.此外,结合理论计算和原位表征技术从本质上揭示SMNCs的构效关系、应用反应机理以及真正活性中心,拓展其更广的催化应用领域.

关键词: 负载型金属纳米催化剂, 可持续化制备, 绿色合成, 电催化, 析氢反应

Abstract: Among the various types of heterogeneous catalysts, supported metal nanocatalysts (SMNCs) have attracted widespread interest in chemistry and materials science, due to their advantageous features, such as high efficiency, stability, and reusability for catalytic reactions. However, to obtain well-defined SMNCs and inhibit nanoparticle aggregation, traditional approaches generally involve numerous organic reagents, complex steps, and specialized equipment, thus hindering the practical and large-scale synthesis of SMNCs. In this review, we summarize green and sustainable synthetic methodologies for the assembly of SMNCs, including low temperature pyrolysis and solid-state, surfactant- and reductant-free, and ionic liquid assisted syntheses. The conventional application of SMNCs for electrochemical hydrogen evolution and the corresponding achievements are subsequently discussed. Finally, future perspectives toward the sustainable production of SMNCs are presented.

Key words: Supported metal nanocrystals, Sustainable production, Green synthesis, Electrocatalysis, Hydrogen evolution reaction