Dinitrogen cleavage and hydrogenation to ammonia with a uranium complex
作者机构：State Key Laboratory of Coordination Chemistry Jiangsu Key Laboratory of Advanced Organic Materials School of Chemistry and Chemical EngineeringNanjing University School of Medicine and Holistic Integrative MedicineNanjing University of Chinese Medicine LPCNO CNRS and INSA Université Paul Sabatier State Key Laboratory of Radiation Medicine and Protection School for Radiological and Interdisciplinary Sciences (RAD-X) and Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education InstitutionsSoochow University
出 版 物：《National Science Review》 (国家科学评论(英文版))
年 卷 期：2023年第10卷第2期
页 面：165-173页
核心收录：
学科分类：081702[工学-化学工艺] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 080502[工学-材料学] 0805[工学-材料科学与工程（可授工学、理学学位）]
基 金：supported by the National Key R&D Program of China (2021YFA1502500) the National Natural Science Foundation of China (91961116) Fundamental Research Funds for the Central Universities and the Programs for High-Level Entrepreneurial and Innovative Talents Introduction of Jiangsu Province (group programs) The Humboldt Foundation the Chinese Academy of Sciences are acknowledged for their support
主 题：N_2 activation NH_3 formation depleted uranium uranium azide actinide coordination chemistry
摘 要：The Haber-Bosch process produces ammonia(NH3) from dinitrogen(N2) and dihydrogen(H2),but re quires high temperature and *** iron-based catalysts were exploited in the current industrial Haber-Bosch process,uranium-based materials served as effective catalysts for production of NH3from *** some molecular uranium complexes are known to be capable of combining with N2,further hydrogenation with H2forming NH3has not been reported to ***,we describe the first example of N2cleavage and hydrogenation with H2to NH3with a molecular uranium *** N2cleavage product contains three uranium centers that are bridged by three imido μ2-NH ligands and one nitridoμ3-N *** experiments with15N demonstrate that the nitrido ligand in the product originates from *** of the N2-cleaved complex with H2or H+forms NH3under mild conditions.A synthetic cycle has been established by the reaction of the N2-cleaved complex with trimethylsilyl *** isolation of this trinuclear imido-nitrido product implies that a multi-metallic uranium assembly plays an important role in the activation of N2.
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