Synthesis of cobalt single atom catalyst by a solid-state transformation strategy for direct C-C cross-coupling of primary and secondary alcohols

Li, Zhijun; Chen, Yuying; Lü, Xin; Li, Honghong; Leng, Leipeng; Zhang, Tinglei; Horton, J. Hugh

doi:10.1007/s12274-022-4196-7

Cited by 20 publications

(7 citation statements)

References 61 publications

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“…[25][26][27] The strong interaction between metal atoms and carrier materials is very signicant for keeping the atomic dispersion of metal active centers and preventing agglomeration into particles. [28][29][30][31] Carbon materials have been proven to be ideal carrier materials because of their adjustable structure, excellent conductivity, stable physical and chemical properties. [32][33][34] The uniformly distributed defects on the surface of carbon materials also provide a basis for anchoring isolated active metal atoms.…”

Section: Introductionmentioning

confidence: 99%

Rational design, application and dynamic evolution of Cu–N–C single-atom catalysts

Dou

Sun

et al. 2022

J. Mater. Chem. A

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Section: Introductionmentioning

confidence: 99%

Rational design, application and dynamic evolution of Cu–N–C single-atom catalysts

Dou

Sun

et al. 2022

J. Mater. Chem. A

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“…The development of advanced energy conversion and storage technologies is important to fulfill the purpose of clean energy Single-atom catalysts (SACs), by virtue of their well-defined atomic structure, maximal metal utilization, unique electronic/ geometric properties, and excellent activity and selectivity, have attracted considerable research attention. [17][18][19][20][21][22][23][24][25][26] Nitrogen-doped carbon (NC) supported transition metal-based SACs, which exhibit the merits of good electrical conductivity, low cost, environmental friendliness, and comparable catalytic activity with precious-metal counterparts, have been regarded as one of the potentially feasible alternatives to precious-metal-based electrocatalysts in ORR and OER. [27][28][29][30] For example, Chen et al reported a polymerization-pyrolysis-evaporation strategy to synthesize N-doped porous carbon with atomically dispersed Fe 1 -N 4 sites.…”

Section: Introductionmentioning

confidence: 99%

Engineering the Electronic Structure of Single‐Atom Iron Sites with Boosted Oxygen Bifunctional Activity for Zinc–Air Batteries

et al. 2022

Advanced Materials

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Rechargeable zinc–air batteries typically require efficient, durable, and inexpensive bifunctional electrocatalysts to support oxygen reduction/evolution reactions (ORR/OER). However, sluggish kinetics and mass transportation challenges must be addressed if the performance of these catalysts is to be enhanced. Herein, a strategy to fabricate a catalyst comprising atomically dispersed iron atoms supported on a mesoporous nitrogen‐doped carbon support (Fe SAs/NC) with accessible metal sites and optimized electronic metal–support interactions is developed. Both the experimental results and theoretical calculations reveal that the engineered electronic structures of the metal active sites can regulate the charge distribution of Fe centers to optimize the adsorption/desorption of oxygenated intermediates. The Fe SAs/NC containing Fe1N4O1 sites achieves remarkable ORR activity over the entire pH range, with half‐wave potentials of 0.93, 0.83, and 0.75 V (vs reversible hydrogen electrode) in alkaline, acidic, and neutral electrolytes, respectively. In addition, it demonstrates a promising low overpotential of 320 mV at 10 mA cm−2 for OER in alkaline conditions. The zinc–air battery assembled with Fe SAs/NC exhibits superior performance than that of Pt/C+RuO2 counterpart in terms of peak power density, specific capacity, and cycling stability. These findings demonstrate the importance of the electronic structure engineering of metal sites in directing catalytic activity.

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“…[11][12][13][14][15][16] Single-atom catalysts (SACs) demonstrate great promise for rational use of metal precursors and maximized atom utilization efficiency in a variety of chemical reactions. [17][18][19] SACs offer atomically dispersed metal active sites by coordinating with neighboring atoms on support materials, thus delivering excellent activity and selectivity that are comparable with homogeneous catalysts. [19][20][21][22][23][24] The catalytic performance of SACs is highly dependent on the number and coordination environment of active sites, which are largely determined by such variables as preparation methods, metal precursors, or types of supports.…”

Section: Introductionmentioning

confidence: 99%

A Heterogeneous Single Atom Cobalt Catalyst for Highly Efficient Acceptorless Dehydrogenative Coupling Reactions

Lü

Zhao

et al. 2023

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A fundamental understanding of metal active sites in single‐atom catalysts (SACs) is important and challenging in the development of high‐performance catalyst systems. Here, a highly efficient and straightforward molten‐salt‐assisted approach is reported to create atomically dispersed cobalt atoms supported over vanadium pentoxide layered material, with each cobalt atom coordinated with four neighboring oxygen atoms. The liquid environment and the strong polarizing force of the molten salt at high temperatures potentially favor the weakening of VO bonding and the formation of CoO bonding on the vanadium oxide surface. This cobalt SAC achieves extraordinary catalytic efficiency in acceptorless dehydrogenative coupling of alcohols with amines to give imines, with more than 99% selectivity under almost 100% conversion within 3 h, along with a high turnover frequency (TOF) of 5882 h−1, exceeding those of previously reported benchmarking catalysts. Moreover, it delivers excellent recyclability, reaction scalability, and substrate tolerance. Density functional theory (DFT) calculations further confirm that the optimized coordination environment and strong electronic metal‐support interaction contribute significantly to the activation of reactants. The findings provide a feasible route to construct SACs at the atomic level for use in organic transformations.

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Synthesis of cobalt single atom catalyst by a solid-state transformation strategy for direct C-C cross-coupling of primary and secondary alcohols

Cited by 20 publications

References 61 publications

Rational design, application and dynamic evolution of Cu–N–C single-atom catalysts

Rational design, application and dynamic evolution of Cu–N–C single-atom catalysts

Engineering the Electronic Structure of Single‐Atom Iron Sites with Boosted Oxygen Bifunctional Activity for Zinc–Air Batteries

A Heterogeneous Single Atom Cobalt Catalyst for Highly Efficient Acceptorless Dehydrogenative Coupling Reactions

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