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所属单位：材料科学与工程学院

发表刊物：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

关键字：Chemistry, Multidisciplinary

摘要：Metal nitride complexes have recently been proposed as an efficient noble-metal-free catalyst for ammonia synthesis utilizing a dual active site concept. However, their high sensitivity to air and moisture has restricted potential applications. We report that their chemical sensitivity can be improved by introducing Al into the LaN lattice, thereby forming La−Al metallic bonds (La−Al−N). The catalytic activity and mechanism of the resulting TM/La−Al−N (TM=Ni, Co) are comparable to the previously reported TM/LaN catalyst. Notably, the catalytic activity did not degrade after exposure to air and moisture. Kinetic analysis and isotopic experiment showed that La−Al−N is responsible for N2 absorption and activation despite substantial Al being introduced into its lattice because the local coordination of the lattice N remained largely unchanged. These findings show the effectiveness of metallic bond formation, which can support the chemical stability of rare-earth nitrides with retention of catalytic functionality.

合写作者：Tian-Nan Ye(外),Jiang Li(外),Zichuang Li(外),关浩天(学),Masato Sasase(外),Yasuhiro Niwa(外),Hitoshi Abe(外),李谦,Fushen Pan

论文类型：期刊论文

通讯作者：鲁杨帆,Masaaki Kitano,Hideo Hosono

论文编号：242325

卷号：61

页面范围：e202211759

ISSN号：1433-7851

是否译文：否

发表时间：2022-01-01