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材料导报  2023, Vol. 37 Issue (12): 21070195-15    https://doi.org/10.11896/cldb.21070195
  高分子与聚合物基复合材料 |
尿素分解制氢催化剂研究进展
王留留1,†, 任洁1,†, 卢星宇1, 邹力1, 谢佳乐1,2,*
1 西南石油大学新能源与材料学院,成都 610500
2 西南石油大学油气藏地质及开发工程国家重点实验室,成都 610500
Research Progress of Urea Splitting Catalysts for Hydrogen Generation
WANG Liuliu1,†, REN Jie1,†, LU Xingyu1, ZOU Li1, XIE Jiale1,2,*
1 School of New Energy and Materials, Southwest Petroleum University, Chengdu 610500, China
2 State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu 610500, China
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摘要 氢能既是零碳燃料,又是化石能源和可再生能源之间过渡和转换的桥梁。相对于水分解制氢,尿素分解制氢可以实现节能,以及解决尿素环境污染的问题。尿素具有储量丰富、安全性高和低成本等优点,且其理论上分解制氢性能远优于水分解制氢,是未来氢气获取的重要来源之一。尿素氧化反应(UOR)是尿素分解制氢技术的重要半反应,决定了尿素电解池或尿素燃料电池的工作效率。催化剂在UOR反应中起着关键作用,其本征物化性质以及表面性质会显著影响UOR反应动力学,目前大体发展出无基底材料支撑的镍基催化剂、有基底材料支撑的镍基催化剂和非镍基催化剂三类。
然而,UOR反应的过电位很高,高于理论值约1 000 mV。UOR反应是一种涉及多质子耦合电子转移步骤的复杂反应过程,其具体的反应机理远非简单的C-N键断裂。贵金属基催化剂具有良好的UOR催化性能,但存在价格昂贵和储量不足的缺点。非贵过渡金属基催化剂则成为研究的焦点,其催化性能可能与贵金属基催化剂相当或超过贵金属基催化剂性能。镍基催化剂成为催化UOR反应的明星材料,目前已发展出金属镍、氢氧化镍、氧化镍、磷化镍、镍金属有机框架材料等大量含镍催化剂。进一步,也发展出Ni-Zn-Co、MoO2/Ni2P等含镍复合催化剂。新型UOR催化剂发展的同时,也形成了缺陷工程、结构工程、界面工程等先进的催化剂设计与调控方法。
以镍元素为主要活性成分的UOR催化剂是电催化或光电催化UOR反应的研究焦点,按照催化剂生长基底可以分为无基底材料支撑和有基底材料支撑两类催化剂。近年来,以金属、氧化物、氢氧化物、磷化物和金属有机框架材料等形式存在的非贵金属、高效镍基电催化剂因能降低成本和加速反应动力学而受到广泛关注。另一方面,由钴基、铜基、钼基、锰基和铁基等过渡金属和镍元素复合形成的双金属或者三金属催化剂用于UOR反应也被大量研究。为了解决常见镍基催化剂电导率低的问题,人们在使用泡沫镍、碳基材料、钛网等高导电率基底材料与含镍催化剂形成复合材料方面也进行了不断的尝试。此外,一些新型的非镍基材料也被用作UOR反应的催化剂。
本文归纳了尿素分解制氢催化剂的研究进展,分别对尿素分解制氢原理、电催化尿素氧化催化剂、光电催化尿素氧化催化剂、催化剂设计与合成等进行介绍,分析了尿素分解制氢催化剂面临的问题并展望其前景,以期为制备高效的尿素分解制氢催化剂提供参考。
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王留留
任洁
卢星宇
邹力
谢佳乐
关键词:  氢能  尿素分解  催化剂  电催化  光电催化    
Abstract: Hydrogen energy is both a zero-carbon fuel and a bridge for the transition and conversion between fossil fuels and renewable energy. Compared to water splitting for hydrogen production, urea splitting is an energy-saving strategy, which can also solve the problem of urea pollution. Urea has the merits of vast reserves, safety, and low cost, and its theoretical potential for urea splitting is far lower than water splitting, which is one of the important sources of hydrogen in the future. Urea oxidation reaction (UOR)is an important half-reaction of the urea splitting for hydrogen production, which determines the efficiency of the urea electrolysis cells or the urea fuel cells. Catalyst plays a key role in UOR reaction, and its physicochemical and surface properties will significantly affect the kinetics of UOR reaction. At present, nickel-based catalysts can be classified into three subsidiary sets:unsupported nickel-based catalysts, supported nickel-based catalysts, and non-nickel-based catalysts.
However, the overpotential of the UOR reaction is high, which is about 1 000 mV higher than the theoretical value. The UOR reaction is a complex reaction process involving several proton-coupled electron transfer steps, whose deep mechanism is much more complex than the simple C-N bond cleavage. Precious metal-based catalysts are frequently applied as benchmarks for UOR catalysis. However, the drawbacks of expensiveness and scarcities are the major reasons for their limiting roles in current scientific research and future commercialization of urea-based technologies. Nonprecious transition metal-based catalysts have become the focus of research, whose catalytic performance may match or even surpass those of the precious metal catalysts. Nickel-based catalyst has become a class of star materials to catalyze UOR reaction, and many nickel-containing catalysts such as nickel metal, nickel hydroxide, nickel phosphate, and nickel metal organic framework materials. Further, nickel-containing composite catalysts such as Ni-Zn-Co, MoO2/Ni2P are also developed recently. The newly controllable methods of UOR catalysts such as the defect engineering, structural engineering and interface engineering are also developed.
The UOR catalysts with nickel as the main active component are the focus of electrocatalytic or photoelectrocatalytic UOR reaction. According to the growth substrate of catalysts, it can be divided into two types of unsupported nickel-based catalysts and supported nickel-based catalysts. In recent years, non-precious metal and high-efficiency nickel-based electrocatalysts in the form of metals, oxides, hydrogen oxides, phosphorides, and metal-organic framework materials have been attracting wide attention for their cost reduction and accelerated reaction kinetics. On the other hand, a bimetal-catalyst or trimetal-catalyst formed by the hybridization of transition metals and nickel elements, including cobalt, copper, molybdenum, manganese, and iron, has also been extensively studied for UOR reactions. To solve the common problem of low conductivity of nickel-based catalyst, continuous attempts have been made to use nickel foam, carbon material, titanium mesh, and other high conductivity substrates with nickel-containing catalysts. In addition, some new non-nickel-based materials are also used as catalysts for the UOR reaction.
This review offers a retrospection of the research efforts with respect to the urea splitting catalysts, and provides elaborate descriptions about the principle of urea splitting, the electrocatalysts for urea splitting, the photoelectrocatalysts for urea splitting, and the rational design/synthesis of UOR catalysts. We then pay attention to the problems confronting the current state-of-the-art UOR catalysts. This review can be used as a refe-rence for the preparation of high-efficient catalysts for hydrogen production from urea splitting.
Key words:  hydrogen energy    urea splitting    catalyst    electrocatalysis    photoelectrocatalysis
出版日期:  2023-06-25      发布日期:  2023-06-20
ZTFLH:  O64  
基金资助: 四川省高层次人才引进计划项目;国家自然科学基金青年科学基金项目(21703150);四川省科技计划项目(2020YJ0123);西南石油大学校级青年科研创新团队项目(2019CXTD10);西南石油大学自然科学“揭榜挂帅”项目(2021JBGS08)和启动基金
通讯作者:  * 谢佳乐,博士,四川省高层次人才引进计划入选者,副研究员,硕士研究生导师。曾于2009年和2014年获得西南大学学士和博士学位;此后在西南大学和德国伊尔梅瑙工业大学以博士后和访问学者身份开展研究工作,现任教于西南石油大学。长期从事低维纳米材料和光伏制氢等相关领域的研究,并取得了一系列研究成果,以第一或通信作者身份在Energy & Environmental Science、Nano Energy、Journal of Materials Chemistry A、ACS Sustainable Chemistry & Engineering等在内的专业期刊上发表学术论文46篇,获授权或公开美国和中国发明专利9项,参与编著出版4部学术专著。jialexie@swpu.edu.cn   
作者简介:  王留留,2018年6月毕业于长春工业大学,获得工学学士学位。现为西南石油大学新能源与材料学院硕士研究生,在谢佳乐副研究员的指导下进行研究。目前主要研究领域为光电催化制氢。
任洁,2019年6月毕业于西安石油大学,获得工学学士学位。现为西南石油大学新能源与材料学院硕士研究生,在谢佳乐副研究员的指导下进行研究。目前主要研究领域为光电催化制氢。
引用本文:    
王留留, 任洁, 卢星宇, 邹力, 谢佳乐. 尿素分解制氢催化剂研究进展[J]. 材料导报, 2023, 37(12): 21070195-15.
WANG Liuliu, REN Jie, LU Xingyu, ZOU Li, XIE Jiale. Research Progress of Urea Splitting Catalysts for Hydrogen Generation. Materials Reports, 2023, 37(12): 21070195-15.
链接本文:  
http://www.mater-rep.com/CN/10.11896/cldb.21070195  或          http://www.mater-rep.com/CN/Y2023/V37/I12/21070195
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