首页|Nitrogen Reduction to Ammonia by a Phosphorus-Nitrogen PN3P-Mo(Ⅴ)Nitride Complex:Significant Enhancement via Ligand Postmodification

Nitrogen Reduction to Ammonia by a Phosphorus-Nitrogen PN3P-Mo(Ⅴ)Nitride Complex:Significant Enhancement via Ligand Postmodification

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Efforts to develop organometallic complexes for cat-alytic nitrogen reduction have seen significant prog-ress in recent years.However,the strategies for improving the activity of the homogenous catalysts have mainly focused on alternating ligands and metals.Herein,we report that the activity and stability of a PN3P-Mo pincer complex(2)toward dinitrogen(N2)reduction were greatly enhanced through post-modification of the PN3P pincer framework of its parent complex(1).A high ratio of NH3/Mo(3525)was achieved in the presence of Sml2 as a reductant.In sharp contrast,1 only afforded an NH3/Mo ratio of 21.Moreover,when supported by an anionic pincer ligand,2 furnished a high oxidation state Mo(Ⅴ)-nitride complex via N2 cleavage as a plausible key intermediate in the catalytic process,suggesting a catalytic cycle that may involve different oxidation states(Ⅱ/Ⅴ)from those with 10-n electron configura-tion in the literature.

molybdenumPN3Psamarium(Ⅱ)iodidenitrogen reductionligand postmodification

Delong Han、Priyanka Chakraborty、Mei-Hui Huang、Li Yang、Hao Huang、Théo P.Gon?alves、Abdul Hamid Emwas、Zhiping Lai、Jr-Hau He、Aleksander Shkurenko、Mohamed Eddaoudi、Kuo-Wei Huang

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Division of Physical Science and Engineering,King Abdullah University of Science and Technology,Thuwal 23955

KAUST Catalysis Center,King Abdullah University of Science and Technology,Thuwal 23955

Core Lab,King Abdullah University of Science and Technology,Thuwal 23955

Advanced Membranes and Porous Materials Research Center,King Abdullah University of Science and Technology,Thuwal 23955

Department of Materials Science and Engineering,City University of Hong Kong,Kowloon 999077

Agency for Science,Technology,and Research,Institute of Materials Research and Engineering and Institute of Sustainability for Chemicals,Energy and Environment,Singapore 138634

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King Abdullah University of Science and Technology(KAUST)

2023

10.31635/ccschem.022.202202385

中国化学会会刊(英文)

中国化学会会刊(英文)

CSCD
ISSN：
年,卷(期)：2023.5(3)
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