摘要
随着经济的发展,当今社会对能源的需求不断增加.然而,传统的化石燃料,如煤和石油,虽然能够提供大量的能源,但其资源有限,不可再生,并且燃烧产物对环境有害,不符合绿色低碳的发展理念,亟需开发新型、高效的清洁能源.氨(NH3)因具有氢含量高、燃烧产物(完全燃烧时产物为N_(2)和H2O)无害、可规模化生产、压缩性好、易于储存和运输等优点,被认为是直接氨燃料电池(DAFCs)的理想候选燃料.同时,氨也是常见的含氮污染物,广泛存在于人类生产和工农业活动中.因此,氨氧化反应(AOR)在清洁能源生产和含氨废水处理领域都起着重要作用.本文首先系统总结了AOR在不同领域的研究进展,强调了其在清洁能源领域(如DAFCs)的巨大应用潜力,突出了AOR与水电解反应中的阴极氢析出过程耦合制取氢气在能源转化领域的研究价值,以及AOR在含氨废水处理领域的重要性.然后,讨论了AOR机制:AOR反应过程中存在竞争,并可生成多种含氮产物(如N_(2),NO,NO_(2),NO_(2)^(–)和NO_(3)^(–)等),进而影响产物的选择性和反应效率等.再后,讨论了原位表征技术(如采用原位拉曼光谱对催化剂重构行为跟踪和采用原位傅里叶变换红外光谱对反应中间体实时监测)和构建理论计算模型的重要性,这些方法为揭示AOR机制和反应路径提供有力的支持.同时,对AOR催化剂的设计策略和反应条件的筛选提出建议,如反应环境pH值会影响活性位点的质子化状态,从而改变吸附行为,影响催化性能.还探讨了AOR过程耦合电解水氢析反应对低能耗、高效率制取氢气的意义,并概述了在含氨废水处理中提高氮气产物选择性的必要性.最后,讨论了AOR研究中面临的挑战和可采用的策略,包括进一步增加活性位点的暴露、增强催化活性、精准识别活性位点、最大程度地利用催化中心、提高催化剂抗中毒能力、提高目标产物的选择性以及提高催化剂使用寿命等.综上,本文系统地总结了AOR的研究进展、反应机制以及未来的发展策略等,为进一步推动AOR在洁净能源和环境保护领域的应用,为进一步开发更绿色环保的能源体系以及高效的污水处理方法提供新思路.
In recent decades,the advancement of clean energy technologies and sewage purification has emerged as a focal point of research.This review focuses on the ammonia oxidation reaction(AOR)and summarizes its multifaceted applications,including its use in direct ammonia fuel cells(DAFCs),its coupling with the hydrogen evolution reaction(HER),and its significance in ammonia-containing sewage purification.We discuss how the combination of in‐situ characterization techniques and theoretical models has emerged as a powerful tool for exploring the AOR mechanism.The interplay of operational parameters such as temperature and pH,along with catalyst design,is emphasized in the context of DAFCs,highlighting the need for precise optimization to enhance efficiency.The importance of selectivity in the nitrogen gas product in ammonia-containing wastewater is also discussed.Furthermore,the review addresses the challenges and opportunities in AOR research,including strategies to enhance catalytic activity,identify active centers,maximize the utilization of catalyst atoms,and improve selectivity while ensuring catalyst durability.Ultimately,this review serves as a comprehensive guide for researchers and practitioners interested in harnessing the potential of AOR to bridge the gap between clean energy generation and sustainable wastewater treatment,offering insights into a greener and more environmentally responsible future.
作者
张颖贞
黄剑莹
赖跃坤
Yingzhen Zhang;Jianying Huang;Yuekun Lai(National Engineering Research Center of Chemical Fertilizer Catalyst(NERC‐CFC),College of Chemical Engineering,Fuzhou University,Fuzhou 350116,Fujian,China;Qingyuan Innovation Laboratory,Quanzhou 362801,Fujian,China)
基金
国家自然科学基金(22075046,51972063)
国家重点研发计划(2022YFB3804905,2022YFB3804900,2019YFE0111200)
福建省杰出青年自然科学基金(2020J06038)
福建省杰出青年自然科学基金(2019J01256)
111工程(D17005).
关键词
氨氧化反应
直接氨燃料电池
氢气
污水处理
清洁能源
电催化
Ammonia oxidation reaction
Direct ammonia fuel cells
Hydrogen
Sewage purification
Clean energy
Electrocatalysis
