硅酸盐学报

钙钛矿复合氧化物催化剂研究进展

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王玲玲 ¹ , 邵伟 ¹^,³ , 韩飞 ² , 邹俊华 ² , 陈伟 ¹ , 胡银 ¹ , 章芬 ¹ , 施梓胜 ¹^,³

硅酸盐学报 | 综合评述 2024,52(1): 305-321

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硅酸盐学报 |综合评述 2024 , 52 (1) : 305 -321

钙钛矿复合氧化物催化剂研究进展

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王玲玲¹, 邵伟¹^,³, 韩飞², 邹俊华², 陈伟¹, 胡银¹, 章芬¹, 施梓胜¹^,³

作者信息

^1．江西省科学院应用化学研究所，南昌 330096

^2．江西省科学院能源研究所，南昌 330096

^3．南昌航空大学环境与化学工程学院，南昌 330063

通讯作者:

韩飞（1989—），男，博士，助理研究员。

作者简介:

王玲玲（1983—），女，博士，副研究员。

Research Progress on Perovskite Composite Oxide Catalysts

Lingling WANG¹, Wei SHAO¹^,³, Fei HAN², Junhua ZOU², Wei CHEN¹, Yin HU¹, Fen ZHANG¹, Zisheng SHI¹^,³

Affiliations

^1.Institute of Applied Chemistry, Jiangxi Academy of Sciences, Nanchang 330096, China

^2.Institute of Energy Research, Jiangxi Academy of Sciences, Nanchang 330096, China

^3.School of Environmental and Chemical Engineering, Nanchang Hangkong University, Nanchang 330063, China

Corresponding Author:

HAN Fei (1989-), male, Ph.D., Assistant Professor. E-mail: hanfei2031@163.com

WANG Lingling (1983-), female, Ph.D., Associate Professor. E-mail: sunnyskywang@163.com

出版时间: 2024-01-20 doi: 10.14062/j.issn.0454-5648.20230404

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摘要

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钙钛矿复合氧化物催化剂因其电子结构可调、物性丰富、组成灵活、环保等特性而备受关注。讨论了溶胶凝胶法、共沉淀法、微乳液法、水热/溶剂热法等钙钛矿复合氧化物催化剂制备方法及其优缺点，综述了钙钛矿复合氧化物在热催化、光催化、电催化以及协同催化中的应用和催化剂性能优化，重点考察了其在CO₂还原和甲烷活化等方面的催化性能及其催化机理，最后总结了钙钛矿复合氧化物催化剂在催化CO₂还原和甲烷活化等方面存在的问题，并展望了钙钛矿复合氧化物催化剂的发展前景，以期为研发更加高效、稳定的钙钛矿复合氧化物催化剂提供借鉴。

关键词

钙钛矿复合氧化物 / 催化剂 / 二氧化碳还原 / 甲烷活化

Abstract

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The catalytic conversion of greenhouse gases, such as carbon dioxide and methane, into high-value-added chemicals/fuels (i.e., formic acid, methanol, ethylene, etc.) is recognized as a cost-effective tactic for achieving the "dual-carbon" purpose. It provides an alternative to fossil fuels, and also offers novel approaches to environmental dilemmas such as global warming. Catalysts with an extensive specific surface area and plentiful surface active sites are capable of absorbing and aligning reactant molecules, including CO₂ and methane, in an orientated manner. This reduces the energy required to activate the reaction, thereby enhancing the efficiency and selectivity of CO₂ reduction and methane activation reactions. Developing novel catalysts with low cost, high catalytic activity, good long-term stability, and high product selectivity becomes popular to improve the efficiency of energy catalytic conversion. Perovskite composite oxides are a promising nanomaterial with superior redox performance, high stability, facile structural regulation, and rich active sites, offering some advantages for developed catalysts. For the advantageous properties of perovskite composite oxides in catalytic reactions, it is crucial to comprehensively investigate the catalytic mechanism of these oxides in CO₂ reduction and methane activation, promote the development of high-performance perovskite composite oxide catalysts, and accelerate global efforts towards achieving carbon peak and carbon neutrality. Therefore, there is an urgent need to summarize the research progress on perovskite composite oxides for CO₂ reduction and methane activation. This review represented the thermocatalytic, photocatalytic, electrocatalytic, and synergistic catalysis applications of perovskite composite oxides, with summarizing their catalytic performance in CO₂ reduction and methane activation.

Perovskite composite oxide catalysts have a potential in facilitating thermally catalyzed CO₂ reduction and methane activation reactions. In particular, some rare-earth-based perovskite composite oxide catalysts serve a crucial function in this regard. The morphology, compositional structure, and surface adsorption properties of perovskite composite oxide catalysts are modulated via optimizing the preparation method and doping/substitution of metal elements. This leads to an increase in the oxygen vacancies and active sites of the catalysts, thereby improving their catalytic performance in thermocatalytic reactions. Compared to the photocatalytic and electrocatalytic materials, thermaocatalytic material yields a faster reaction rate, but the catalyst is susceptible to coking and carbon deposition at elevated temperatures. In addition, perovskite composite oxide catalysts demonstrate the superior effectiveness in the processes of photocatalytic reduction of CO₂ and activation of methane. The energy band structure of the perovskite composite oxide photocatalyst are adjusted via doping with transition and rare-earth metals, optimizing morphology, regulating oxygen vacancy, loading cocatalysts, and constructing heterogeneous structures, etc.. This can broaden the light absorption range, reduce the reaction activation energy, promote the photogenerated carrier separation, inhibite the electron-hole pair recombination, and improve the reactant adsorption on the photocatalyst surface. This leads to the improved production rate, yield, and selectivity of the product. Photocatalysis offers environmentally friendly and controllable processes, yet it is limited due to its low reaction rate and selectivity for product formation. Also, perovskite composite oxide catalysts demonstrate a significant potential for electrocatalytic CO₂ reduction and methane activation reactions. Perovskite composite oxides constitute a commendable class of electrocatalytic cathode materials showcasing exceptional ionic conductivity and redox properties. Scientists further enhance the conductivity of the materials by elemental doping at A/B sites and constructing oxygen vacancy to facilitate electron transfer, thereby improving the electrocatalytic performance of perovskite composite oxides. The electrocatalytic reaction offers some advantages like efficiency, cleanliness, and high product selectivity. Nonetheless, the reaction performance is extensively impacted underits reaction conditions (i.e., electrodes, electrolyte solution, etc.). In recent years, the combination of two or more catalytic technologies through synergistic catalysis has attracted much attention alongside the progress of catalytic research. Synergistic catalysis incorporates the benefits of individual catalytic technologies, while overcoming their inherent drawbacks, leading to the more effective and stable catalytic reactions. Synergistic catalytic techniques also allow catalysts that are not suitable for an individual catalytic reaction to be applied to a synergistic catalytic reaction under appropriate imposed conditions. Currently, perovskite composite oxide catalysts are still in their infancy for synergistic catalysis reactions, and researchers have not thoroughly examined the reaction conditions, basic principles, and interactions of various catalytic methods involved in synergistic catalysis reactions yet. The further exploration is required to generate more stable and efficient catalysts for synergistic catalysis reactions.

Summary and prospects

Perovskite composite oxides have some advantages of adjustable structure, excellent stability, and high catalytic activity, which make them a promising catalyst. They have undergone a significant growth since the initial simple CaTiO₃, with dozens of varieties now available and in widespread use in energy conversion, chemical production, and environmental protection. This review represented recent research progress on catalytic CO₂ reduction and methane activation by perovskite composite oxide catalysts. The objective was to offer a reference for research on perovskite composite oxide catalysts for catalytic energy conversion and related fields. In future research, we proposed the following perspectives: 1) new methods (e.g., high-pressure, high-temperature synthesis techniques and in-situ dipole source electrostatic field modulation strategies, etc.) and novelprocesses (e.g., supercritical fluid deposition and atomic layer deposition, etc.) are necessary to produce perovskite composite oxide catalysts with improved structural stability and diversity to enhance their performance; 2) The catalytic principles and reaction pathways of perovskite composite oxide catalysts are further investigated via theoretical calculations (e.g. first-principles calculations, molecular thermodynamics, and kinetic simulations, etc.) as well as characterization techniques (e.g. In-situ Fourier IR spectroscopy and in-situ electron paramagnetic/spin resonance, etc.) to provide a theoretical guidance for the design of perovskite composite oxide catalysts for a novel system; 3) The benefits of perovskite composite oxides should be maximized to extend their application in photothermocatalytic, photoelectrocatalytic, thermoelectrocatalytic, and photoelectrothermal synergistic catalytic as well.

Key words

perovskite composite oxide / catalyst / carbondioxide reduction / methane activation

引用本文

王玲玲, 邵伟, 韩飞, 邹俊华, 陈伟, 胡银, 章芬, 施梓胜. 钙钛矿复合氧化物催化剂研究进展. 硅酸盐学报, 2024 , 52 (1) : 305 -321 . DOI: 10.14062/j.issn.0454-5648.20230404

Lingling WANG, Wei SHAO, Fei HAN, Junhua ZOU, Wei CHEN, Yin HU, Fen ZHANG, Zisheng SHI. Research Progress on Perovskite Composite Oxide Catalysts[J]. Journal of the Chinese Ceramic Society, 2024 , 52 (1) : 305 -321 . DOI: 10.14062/j.issn.0454-5648.20230404

基金

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江西省自然科学基金项目(20232BAB202036; 20232BAB213014; 20212BAB203038)
江西省科学院省级科技计划项目(2022YJC1002; 2023YJC2020; 2023YSBG21008)

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2024年第52卷第1期

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文章信息

doi: 10.14062/j.issn.0454-5648.20230404

接收时间：2023-06-12
首发时间：2026-10-22
出版时间：2024-01-20

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出版历史

收稿日期：2023-06-12
修回日期：2023-08-30

基金

江西省自然科学基金项目(20232BAB202036; 20232BAB213014; 20212BAB203038)

江西省科学院省级科技计划项目(2022YJC1002; 2023YJC2020; 2023YSBG21008)

作者信息

^1．江西省科学院应用化学研究所，南昌 330096

^2．江西省科学院能源研究所，南昌 330096

^3．南昌航空大学环境与化学工程学院，南昌 330063

通讯作者:

韩飞（1989—），男，博士，助理研究员。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20230404

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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