Chem Catalysis ( IF 11.5 ) Pub Date : 2023-12-20 , DOI: 10.1016/j.checat.2023.100840 Xia Zhang , Solmaz Feizpoor , Muhammad Humayun , Chundong Wang
The urea oxidation reaction (UOR) holds tremendous applications in various catalysis processes. Given the general unsatisfied urea degradation (<100%), exploration of highly selective and efficient catalysts for the UOR is highly desirable. Metal-organic frameworks (MOFs) with tailorable metal nodes, organic ligands, homogeneous microenvironments, and structurally identifiable features represent an ideal platform for understanding the relationship between structure, activity, and product selectivity. This review summarizes the UOR mechanisms of nickel-based catalysts, including Ni3+/Ni4+-mediated mechanisms (adsorbate evolution mechanism and lattice oxygen mechanism), the dual-step mechanism associated with Ni2+ (urea decomposition reaction + UOR), and the three pathways of urea dissociation (i.e., the final products of NO2−, N2, and NH3). Additionally, we also review the modulation strategies (metal node, organic ligands, and morphology) in Ni-MOFs, along with urea product analysis and in situ detection methods. This work provides useful insights into the relationships between structure, activity, and product selectivity for the UOR.
中文翻译:
尿素氧化反应电催化剂:结构、活性和选择性的相关性
尿素氧化反应 (UOR) 在各种催化过程中有着巨大的应用。考虑到尿素降解率普遍不理想(<100%),非常需要探索高选择性和高效的UOR催化剂。具有可定制金属节点、有机配体、均匀微环境和结构可识别特征的金属有机框架(MOF)代表了理解结构、活性和产物选择性之间关系的理想平台。本综述总结了镍基催化剂的UOR机理,包括Ni3+/Ni4+检测方法。这项工作为 UOR 的结构、活性和产品选择性之间的关系提供了有用的见解。原位)。此外,我们还回顾了 Ni-MOF 中的调制策略(金属节点、有机配体和形态),以及尿素产物分析和3 和 NH2, N−2(尿素分解反应+UOR),以及尿素解离的三种途径(即NO的最终产物2+介导机制(吸附质演化机制和晶格氧机制),与Ni相关的双步机制