首页|Plasma-Assisted Dinitrogen Activation via Dual Platinum Cluster Catalysis:A Strategy for Ammonia Synthesis under Mild Conditions

Plasma-Assisted Dinitrogen Activation via Dual Platinum Cluster Catalysis:A Strategy for Ammonia Synthesis under Mild Conditions

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The activation and reduction of N2 to produce ammo-nia under mild conditions is of great interest,but challenges remain.Here,we report a breakthrough in efficient dinitrogen cleavage by employing small Ptn+(n=1-4)clusters and convenient plasma assistance.The reactivity of Pt3+is found to be substantially higher than that of other clusters,and the formed Pt3N7+shows prominent mass abundance among the odd-nitrogen products.We illustrate that a chain re-action path within dual cluster cooperation,especially via a"3+2"mode,is beneficial to N≡N triple bond dissociation,embodying efficient synergistic cataly-sis.A key intermediate containing a bridged N2 of binding with two Pt clusters facilitates N2 activation with significantly enhanced interactions between the d orbitals of Pt and the antibonding π*-orbitals of N2.Furthermore,by reacting the PtnNm+clusters with H2,we observed hydrogenation products of both even-and odd-hydrogen species,indicative of ammonia release.The in situ synthesized platinum nitride clus-ters,typically Pt3N7+,induce a highly active N site for hydrogen anchoring,enabling a cost-effective hydro-treating process for ammonia synthesis.

dual-metal clusternitrogen activationammonia synthesisplatinum nitride clustersplasma-assistance

Chaonan Cui、Yuhan Jia、Hanyu Zhang、Lijun Geng、Zhixun Luo

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Beijing National Laboratory for Molecular Sciences(BNLMS),State Key Laboratory for Structural Chemistry of Unstable and Stable Species,Institute of Chemistry Chinese Academy of Sciences,Beijing 100190

University of Chinese Academy of Sciences,Beijing 100049

国家自然科学基金国家自然科学基金CAS Key Research Project of Frontier Science(CAS)Frontier Cross Project of national laboratory for molecular sciences

2180214621722308QYZDB-SSW-SLH024051Z011BZ3

2023

10.31635/ccschem.022.202201879

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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