Catalysis of dinitrogen activation and reduction by a single Fe13 cluster and its doped systems

文献情報

出版日 2022-12-05

DOI 10.1039/D2CP04619A

インパクトファクター 3.676

著者

Chaonan Cui

原文を見る

要旨

Catalyzing N2 reduction to ammonia under ambient conditions is known to be significant both in the fertilizer industry and life sciences. To unveil the synergy of multiple sites, here, we have studied the catalysis of ammonia synthesis using a typical Fe13 cluster and its doped systems, Fe12X (X = V, Cr, Mn, Co, Ni, Cu, Zn, Nb, Mo, Ru, and Rh). The energetics analysis showed that center substitution (X@Fe12) was favored while doping single V, Cr, Co, and Mo atoms, whereas Mn, Ni, Cu, Zn, Nb, Ru, and Rh tended to form shell-doped structures (Fe12X). Among all the 13 clusters, Fe12Nb exhibited the lowest activation energy for N2 dissociation; moreover, in the hydrogenation process, Fe12Nb could convert N2 to ammonia efficiently. We have fully illustrated the reaction dynamics and structural chemistry essence of these diverse 13-atom systems and propose Fe12Nb as an ideal candidate for catalytic ammonia synthesis.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.