能源催化材料的电化学合成

doi:10.1016/S1872-2067(21)63940-2

催化学报 ›› 2022, Vol. 43 ›› Issue (4): 1001-1016.DOI: 10.1016/S1872-2067(21)63940-2

能源催化材料的电化学合成

高敦峰^a^,^#(), 李合肥^a^,^b, 魏鹏飞^a^,^b, 王毅^a^,^b, 汪国雄^a^,^*(), 包信和^a

^a中国科学院大连化学物理研究所, 洁净能源国家实验室(筹), 催化国家重点实验室, 辽宁大连116023
^b中国科学院大学, 北京100049

收稿日期:2021-07-29 接受日期:2021-07-29 出版日期:2022-03-05 发布日期:2022-03-01
通讯作者: 高敦峰,汪国雄
基金资助:
国家重点研发计划(2016YFB0600901);国家自然科学基金(22002155);国家自然科学基金(92045302);中科院洁净能源创新研究院合作基金(DNL180404);中科院洁净能源创新研究院合作基金(DNL201924);中国科学院战略性先导专项(XDB17020200);中科院青年创新促进会(Y201938);辽宁省自然科学基金(2021-MS-022);大连市高层次人才创新支持计划(2020RQ038)

Electrochemical synthesis of catalytic materials for energy catalysis

Dunfeng Gao^a^,^#(), Hefei Li^a^,^b, Pengfei Wei^a^,^b, Yi Wang^a^,^b, Guoxiong Wang^a^,^*(), Xinhe Bao^a

^aState Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
^bUniversity of Chinese Academy of Sciences, Beijing 100049, China

Received:2021-07-29 Accepted:2021-07-29 Online:2022-03-05 Published:2022-03-01
Contact: Dunfeng Gao, Guoxiong Wang
Supported by:
National Key R&D Program of China(2016YFB0600901);National Natural Science Foundation of China(22002155);National Natural Science Foundation of China(92045302);Dalian National Laboratory for Clean Energy(DNL180404);National Natural Science Foundation of China(DNL201924);Strategic Priority Research Program of the Chinese Academy of Sciences(XDB17020200);CAS Youth Innovation Promotion(Y201938);Natural Science Foundation of Liaoning Province(2021-MS-022);High-Level Talents Innovation Project of Dalian City(2020RQ038)

摘要/Abstract

摘要：

电催化是发展可持续洁净能源技术的基础科学, 是电化学能源转换和物质转化的关键环节. 精准合成催化活性纳米结构是制约很多电催化反应走向实际应用的重要挑战. 与湿化学合成、固相合成和气相沉积等传统方法相比, 电化学合成是一种简单、快速、廉价及可控的高效催化材料制备方法, 也是一种最为直接的一体化电极制备方法.
本文综述了近年来利用电化学合成方法制备高效能源催化材料的研究进展. 首先, 简要介绍了电沉积、阴极腐蚀、电化学去合金化、电化学置换、电化学剥离和电化学修饰等几种主要电化学合成方法的基本原理, 并讨论了电化学合成中电势、电流和电解质组成等关键合成参数的影响. 然后, 重点讨论了电化学合成的催化材料在燃料电池、电解水、二氧化碳/一氧化碳电还原、电化学合成氨、有机分子电化学转化等重要电催化反应中的应用. 这些催化材料按照形貌可分为单原子催化剂、球形纳米粒子、形貌可控的纳米粒子、二维层状/片状纳米材料和三维纳米结构等. 电化学合成在制备结构明确的单原子催化剂上具有其它合成方法不可比拟的优势. 与胶体化学方法相比, 电化学合成的尺寸和形貌可控的纳米粒子具有表面清洁、无表面附着的有机配体以及不需要焙烧等催化剂预处理的特点. 除形貌外, 电化学合成还可以制备在原子尺度上具有特定几何和电子结构的催化活性纳米结构. 电化学方法也是催化剂修饰和再生的一种重要途径, 结合特定的电化学程序, 可在连续操作条件下实现催化材料的原位再生. 通过讨论代表性的催化剂案例, 分析这些催化剂在电催化应用中的构效关系, 阐明了电化学合成方法在催化剂理性设计和制备中的独特优势. 最后, 总结了当前电化学合成催化材料方面存在的问题和研究挑战, 并展望了未来的发展方向. 电化学合成的能源催化材料在热催化、光催化等领域的应用价值仍需进一步探索. 此外, 电化学合成在金属有机框架、高熵合金等新兴功能材料的制备上也具有很好的应用前景. 如何利用电化学的特点并结合原位表征、大数据预测等先进实验和理论方法, 更加精准、可控地合成催化活性纳米结构依然是未来该领域重要的研究机遇.

关键词: 催化材料, 电化学合成, 电催化反应, 电沉积, 阴极腐蚀, 纳米结构

Abstract:

Electrocatalysis is a process dealing with electrochemical reactions in the interconversion of chemical energy and electrical energy. Precise synthesis of catalytically active nanostructures is one of the key challenges that hinder the practical application of many important energy-related electrocatalytic reactions. Compared with conventional wet-chemical, solid-state and vapor deposition synthesis, electrochemical synthesis is a simple, fast, cost-effective and precisely controllable method for the preparation of highly efficient catalytic materials. In this review, we summarize recent progress in the electrochemical synthesis of catalytic materials such as single atoms, spherical and shaped nanoparticles, nanosheets, nanowires, core-shell nanostructures, layered nanomaterials, dendritic nanostructures, hierarchically porous nanostructures as well as composite nanostructures. Fundamental aspects of electrochemical synthesis and several main electrochemical synthesis methods are discussed. Structure-performance correlations between electrochemically synthesized catalysts and their unique electrocatalytic properties are exemplified using selected examples. We offer the reader with a basic guide to the synthesis of highly efficient catalysts using electrochemical methods, and we propose some research challenges and future opportunities in this field.

Key words: Catalytic material, Electrochemical synthesis, Electrocatalytic reaction, Electrodeposition, Cathodic corrosion, Nanostructure

高敦峰, 李合肥, 魏鹏飞, 王毅, 汪国雄, 包信和. 能源催化材料的电化学合成[J]. 催化学报, 2022, 43(4): 1001-1016.

Dunfeng Gao, Hefei Li, Pengfei Wei, Yi Wang, Guoxiong Wang, Xinhe Bao. Electrochemical synthesis of catalytic materials for energy catalysis[J]. Chinese Journal of Catalysis, 2022, 43(4): 1001-1016.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(21)63940-2

https://www.cjcatal.com/CN/Y2022/V43/I4/1001

图/表 11

Table 1 Comparison of various synthesis methods for the preparation of catalytic materials.

Method	Impregnation	Precipitation	Hydrothermal synthesis	Colloidal synthesis	Electrochemical synthesis
Temperature	RT‒100 °C	RT‒100 °C	100‒200 °C	RT‒350 °C	RT
Solvent	Water	Water	Water	Organic solvents	Water
Setup and operation	Simple	Simple	Complicated	Complicated	Simple
Organic ligand	No	No	No	Yes	No
Post-treatment	Yes	Yes	Yes	Yes	No
Tunability in morphology & compositions	Difficult	Difficult	Difficult	Easy	Easy
Suitability for integrated electrodes	No	No	No	No	Yes

Fig. 1. Electrochemical synthesis of catalytic materials for energy catalysis.

Fig. 2. Electrochemical procedures of applying currents and potentials for electrochemical synthesis of catalytic materials. (a) Galvanostatic mode; (b) Potentiostatic mode; (c) Cyclic voltammetry; (d) Square-wave potential pulse; (e) Coupled cyclic voltammetry and square-wave potential pulse.

Fig. 3. Electrochemical deposition for synthesizing single atom catalysts. Schematic of cathodic (a) and anodic (b) deposition of Ir species over Co(OH)2 nanosheets loaded on glassy carbon in a standard three-electrode cell; HAADF-STEM images of cathodically (c) and anodically (d) deposited metal single atoms on Co(OH)2 nanosheets. Reproduced with permission from Ref. [88]. Copyright 2020, Springer Nature.

Fig. 4. Synthesis of single atom catalysts under high voltage. Schematic of plasma arc formed by a 20 kV direct current (DC) supply (a), spark pulse generated by a multistage Marx circuit (b) and synthesis of Co single atom catalysts using PA and SP methods (c). Reproduced with permission from Ref. [69]. Copyright 2021, Wiley-VCH.

Fig. 5. Electrochemical synthesis of spherical nanoparticles. (a) Cathodic corrosion for growing nanoparticles over a Pt wire at a direct current of -10 V in 10 mol·L-1NaOH. Reproduced with permission from Ref. [49]. Copyright 2011, Wiley-VCH. (b) Pd nanoparticles electrodeposited potentiostatically on an Au substrate. Reproduced with permission from Ref. [106]. Copyright 2018, Wiley-VCH. (c) Synthesis procedure of carbon-supported Pt nanoparticles by applying an alternating sinusoidal potential to a Pt counter electrode. Reproduced with permission from Ref. [104]. Copyright 2020, American Chemical Society. (d) HADDF-STEM images of as-prepared and electrochemically dealloyed Cu3Pt intermetallic nanoparticles. Reproduced with permission from Ref. [80]. Copyright 2015, American Chemical Society.

Fig. 6. Electrochemical synthesis of shape-controlled Pt nanoparticles. (a) Scheme of electrochemical synthesis of THH Pt nanocrystals from nanospheres; (b) SEM images and size distributions of THH Pt nanocrystals grown for 10, 30, 40 and 50 min. Scale bars, 200 nm. (c) In situ transmission electron microscopy (TEM) observation on the thermal stability of THH Pt nanocrystals. Reproduced with permission from Ref. [116]. Copyright 2007, American Association for the Advancement of Science.

Fig. 7. Electrochemical synthesis of Cu nanocubes. (a) Electrochemical deposition of Cu nanocubes, revealed by liquid cell TEM technique. Reproduced with permission from Ref. [132]. Copyright 2020, Springer Nature. (b) Support effects on the CO2RR selectivity over Cu nanocubes. Reproduced with permission from Ref. [37]. Copyright 2018, Wiley-VCH. (c) CO2RR performance over shaped nanostructures grown on Cu foils via electrolyte-driven nanostructuring. (c,d) Reproduced with permission from Ref. [71]. Copyright 2019, Wiley-VCH.

Fig. 8. Morphology, structure and performance of electrochemically in situ generated ultrathin Ni nanosheets. (a) SEM images; (b) Ni K-edge EXAFS; (c) HER performance. Reproduced with permission from Ref. [142]. Copyright 2017, Cell Press.

Fig. 9. Electrochemical synthesis of three-dimensional nanostructures. (a) Electrodeposition using graphite substrate and nitrate precursors; (b) Cross-sectional SEM images of as-prepared NiCeOxHy deposited on graphite with (left) and without (right) nitrate ion insertion; (c) OER stability of NiCeOxHy/graphite electrode at a current density of 1 A·cm?2. Reproduced with permission from Ref. [160]. Copyright 2018, Springer Nature.

Fig. 10. Catalyst modification and regeneration via electrochemical methods. (a) Cyclic voltammogram of Pb UPD on electropolished Cu foils; (b) Ratio of HCOO-/H2 production rate for bare Cu foil, 0.78 ML Pb/Cu and Pb foil. Reproduced with permission from Ref. [78]. Copyright 2019, American Chemical Society.

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能源催化材料的电化学合成

Electrochemical synthesis of catalytic materials for energy catalysis

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