摘要
氢能是一种高效、清洁的新能源,有望在未来的能源领域占据重要地位。开发安全、高效的储氢材料是实现氢能大规模实际应用的关键。水合肼(N2H4·H2O)的储氢含量高(8%)且便于运输和储存,是一种具有良好应用前景的储氢材料。研究表明,使用合适的催化剂可以有效降低水合肼分解制氢反应能垒,显著提高水合肼脱氢速率。因此,开发温和条件下高效脱氢催化剂已成为水合肼作为储氢材料规模化应用的研究热点。简要介绍水合肼分解脱氢机制,并阐述水合肼脱氢催化剂体系近年的研究进展,并对提高催化剂的催化性能的策略进行分析。归纳总结改善水合肼脱氢催化剂的催化活性和制氢选择性的方法(如构筑合金结构等),添加助剂创造适宜的外部化学环境,调控金属-载体强相互作用,优化合成方法增加金属催化剂表面积和活性位点等,并对该领域未来的发展进行了展望。
Hydrogen is an efficient and clean new energy,and it is expected to occupy an important position in the future energy field.Developing safe and efficient hydrogen storage materials is the key to realize large-scale practical application of hydrogen energy.Hydrous hydrazine(N2H4·H2O)is a promising hydrogen storage material because of its high hydrogen storage content(8%)and convenient transportation and storage.The research show that the appropriate metal catalyst can effectively reduce the reaction energy barrier of hydrous hydrazine decomposition and hydrogen production,and significantly increase the dehydrogenation rate of hydrous hydrazine.Therefore,the development of efficient dehydrogenation catalyst under mild conditions has become a research hotspot of hydrous hydrazine as a hydrogen storage material.In this paper,the decomposition and dehydrogenation mechanism of hydrous hydrazine were briefly introduced,and the research progress of hydrous hydrazine dehydrogenation catalyst system in recent years was systematically expounded,and the strategies to improve the catalytic performance of the catalyst were analyzed.Essentially,the catalytic decomposition reaction path of N2H4 mainly depended on the cleavage sequence of N-N bond and N-H bond.The purpose of the prepared catalyst was to promote the cleavage of N-H bond.In recent years,the research on dehydrogenation catalysts of hydrous hydrazine had experienced metal nanoparticles,composite oxides and metal-supported catalysts.Metal nanoparticles were usually synthesized by co-reduction method,some of which could selectively decompose hydrous hydrazine,but the overall catalytic performance was poor.This was because the free metal nanoparticles were easy to agglomerate,which reduced the specific surface area and active sites of the catalyst,resulting in the decline of catalytic performance.Although the addition of surfactant could avoid the aggregation of metal nanoparticles,it would cover the active sites on the surface of the particles,which could not fundamentally improve the catalytic performance.Relatively speaking,as a catalyst in strong alkaline environment,composite oxide could achieve 100%selectivity of hydrogen production,and its catalytic performance was considerable,but there were some problems such as low strength and easy change of metal valence.Supported catalyst was to load metal nanoparticles on the carrier/carrier surface,which not only ensured the good dispersion of active metal nanoparticles,but also provided excellent catalytic performance stability for nano-catalyst.In addition,the carrier would have a synergistic effect with metal nanoparticles,and sometimes the carrier could provide a suitable chemical environment for the reaction,which was conducive to improving the catalytic activity and hydrogen production selectivity of the catalyst.With the deepening of scholars'research and understanding on the mechanism of hydrogen production by catalytic decomposition,the nano-catalyst developed showed extremely high catalytic activity for hydrogen production by catalytic decomposition of hydrous hydrazine.After continuous exploration,the researchers summarized the following design strategies that affect the catalytic performance of the catalyst:building alloy structure,create a suitable chemical environment for nano-catalyst,introducing strong metal-carrier interaction(SMSI)and optimizing the synthesis method to increase the surface area and active sites.
作者
孔军
李蓉
刘勇
许立信
叶明富
万超
Kong Jun;Li Rong;LiuYong;Xu Lixin;Ye Mingfu;Wan Chao(Engineering Research Institute,School of Chemistry and Chemical Engineering,Anhui University of Technology,Ma’anshan 243000,China;College of Chemical and Biological Engineering,Zhejiang University,Hangzhou 310027,China;Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Nankai Uni-versity,Tianjin 300071,China;Anhui Provincial Key Laboratory of Optical Functional Materials,Anhui Key Laboratory of Optical Functional Complexes and Nano Complexes,Anqing Normal University,Anqing 246011,China;Jiangxi Province Engineering Research Center of Ecological Chemical Industry,Jiujiang University,Jiujiang 332005,China)
出处
《稀有金属》
EI
CAS
CSCD
北大核心
2024年第8期1177-1190,共14页
Chinese Journal of Rare Metals
基金
国家自然科学基金青年项目(22108238)和联合项目(U22A20408)
安徽省自然科学基金青年项目(1908085QB68)
安徽省科技重大专项(201903a05020055)
中国博士后面上项目(2019M662060)、派出项目(PC2022046)和特别资助站中项目(2020T130580)
安徽省光电磁性功能材料重点实验室开放基金项目(ZD2021007)
江西省生态化工工程研究中心开放基金项目(STKF2109)资助。
关键词
氢能
储氢材料
水合肼
金属催化剂
hydrogen energy
hydrogen storage materials
hydrous hydrazine
metal catalysts
作者简介
孔军(1996-),男,安徽合肥人,硕士研究生,研究方向:液体储氢材料及其脱氢催化剂开发,E-mail:1514055254@qq.com;通信作者:万超,副教授,电话:15655560636,E-mail:wanchao@zju.edu.cn。