A fundamental understanding of the nature of nuclearity effects is important for the rational design of superior sub-nanocatalysts with low nuclearity, but remains a long-standing challenge. Using atomic layer deposition, we precisely synthesized Fe sub-nanocatalysts with tunable nuclearity (Fe 1 -Fe 4 ) anchored on N,O-co-doped carbon nanorods (NOC). The electronic properties and spin configuration of the Fe sub-nanocatalysts were nuclearity dependent and dominated the H 2 O 2 activation modes and adsorption strength of active O species on Fe sites toward CÀ H oxidation. The Fe 1 -NOC single atom catalyst exhibits state-of-the-art activity for benzene oxidation to phenol, which is ascribed to its unique coordination environment (Fe 1 N 2 O 3 ) and medium spin state (t 2g 4 e g 1 ); turnover frequencies of 407 h À 1 at 25 °C and 1869 h À 1 at 60 °C were obtained, which is 3.4, 5.7, and 13.6 times higher than those of Fe dimer, trimer, and tetramer catalysts, respectively.
A fundamental understanding of the nature of nuclearity effects is important for the rational design of superior sub-nanocatalysts with low nuclearity, but remains a long-standing challenge. Using atomic layer deposition, we precisely synthesized Fe sub-nanocatalysts with tunable nuclearity (Fe 1 -Fe 4 ) anchored on N,O-co-doped carbon nanorods (NOC). The electronic properties and spin configuration of the Fe sub-nanocatalysts were nuclearity dependent and dominated the H 2 O 2 activation modes and adsorption strength of active O species on Fe sites toward CÀ H oxidation. The Fe 1 -NOC single atom catalyst exhibits state-of-the-art activity for benzene oxidation to phenol, which is ascribed to its unique coordination environment (Fe 1 N 2 O 3 ) and medium spin state (t 2g 4 e g 1 ); turnover frequencies of 407 h À 1 at 25 °C and 1869 h À 1 at 60 °C were obtained, which is 3.4, 5.7, and 13.6 times higher than those of Fe dimer, trimer, and tetramer catalysts, respectively.
Graphdiyne, a sp/sp2‐cohybridized two‐dimensional all‐carbon material, has many unique and fascinating properties of alkyne‐rich structures, large π conjugated system, uniform pores, specific unevenly‐distributed surface charge, and incomplete charge transfer properties provide promising potential in practical applications including catalysis, energy conversion and storage, intelligent devices, life science, photoelectric, etc. These superior advantages have made graphdiyne one of the hottest research frontiers of chemistry and materials science, and produced a series of original and innovative research results in the fundamental and applied research of carbon materials. In recent years, considerable advances have been made toward the development of graphdiyne based multiscale catalysts for nitrogen‐fixation and ammonia synthesis at room temperatures and ambient pressures. This review aims to provide a comprehensive update in regards to the synthesis of graphdiyne‐based multiscale catalysts and their applications in the synthesis of ammonia. The unique features of graphdiyne are highlighted throughout the review. Finally, we conclude by discussing challenges and future perspectives relating to graphdiyne.
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