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Cascade anchoring strategy for general mass production of high-loading single-atomic metal-nitrogen catalysts.

ABSTRACT: Although single-atomically dispersed metal-N_x on carbon support (M-NC) has great potential in heterogeneous catalysis, the scalable synthesis of such single-atom catalysts (SACs) with high-loading metal-N_x is greatly challenging since the loading and single-atomic dispersion have to be balanced at high temperature for forming metal-N_x. Herein, we develop a general cascade anchoring strategy for the mass production of a series of M-NC SACs with a metal loading up to 12.1 wt%. Systematic investigation reveals that the chelation of metal ions, physical isolation of chelate complex upon high loading, and the binding with N-species at elevated temperature are essential to achieving high-loading M-NC SACs. As a demonstration, high-loading Fe-NC SAC shows superior electrocatalytic performance for O₂ reduction and Ni-NC SAC exhibits high electrocatalytic activity for CO₂ reduction. The strategy paves a universal way to produce stable M-NC SAC with high-density metal-N_x sites for diverse high-performance applications.

SUBMITTER: Zhao L

PROVIDER: S-EPMC6426845 | biostudies-literature | 2019 Mar

REPOSITORIES: biostudies-literature

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Cascade anchoring strategy for general mass production of high-loading single-atomic metal-nitrogen catalysts.

Zhao Lu L Zhang Yun Y Huang Lin-Bo LB Liu Xiao-Zhi XZ Zhang Qing-Hua QH He Chao C Wu Ze-Yuan ZY Zhang Lin-Juan LJ Wu Jinpeng J Yang Wanli W Gu Lin L Hu Jin-Song JS Wan Li-Jun LJ

Nature communications 20190320 1

Although single-atomically dispersed metal-Nx on carbon support (M-NC) has great potential in heterogeneous catalysis, the scalable synthesis of such single-atom catalysts (SACs) with high-loading metal-Nx is greatly challenging since the loading and single-atomic dispersion have to be balanced at high temperature for forming metal-Nx. Herein, we develop a general cascade anchoring strategy for the mass production of a series of M-NC SACs with a metal loading up ...[more]

PMID: 30894539

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Project description:ABSTRACT Thermally activated ultrafast diffusion, collision and combination of metal atoms comprise the fundamental processes of synthesizing burgeoning subnanometer metal clusters for diverse applications. However, so far, no method has allowed the kinetically controllable synthesis of subnanometer metal clusters without compromising metal loading. Herein, we have developed, for the first time, a graphene-confined ultrafast radiant heating (GCURH) method for the synthesis of high-loading metal cluster catalysts in microseconds, where the impermeable and flexible graphene acts as a diffusion-constrained nanoreactor for high-temperature reactions. Originating from graphene-mediated ultrafast and efficient laser-to-thermal conversion, the GCURH method is capable of providing a record-high heating and cooling rate of ∼109°C/s and a peak temperature above 2000°C, and the diffusion of thermally activated atoms is spatially limited within the confinement of the graphene nanoreactor. As a result, due to the kinetics-dominant and diffusion-constrained condition provided by GCURH, subnanometer Co cluster catalysts with high metal loading up to 27.1 wt% have been synthesized by pyrolyzing a Co-based metal-organic framework (MOF) in microseconds, representing one of the highest size-loading combinations and the quickest rate for MOF pyrolysis in the reported literature. The obtained Co cluster catalyst not only exhibits an extraordinary activity similar to that of most modern multicomponent noble metal counterparts in the electrocatalytic oxygen evolution reaction, but is also highly convenient for catalyst recycling and refining due to its single metal component. Such a novel GCURH technique paves the way for the kinetically regulated, limited diffusion distance of thermally activated atoms, which in turn provides enormous opportunities for the development of sophisticated and environmentally sustainable metal cluster catalysts. In order to overcome the trade-off between ultrasmall size and high loading in synthesizing high-performance metal cluster catalysts, a novel graphene-confined ultrafast radiant heating (GCURH) method is developed.

Dataset Information

Cascade anchoring strategy for general mass production of high-loading single-atomic metal-nitrogen catalysts.

Publications

Cascade anchoring strategy for general mass production of high-loading single-atomic metal-nitrogen catalysts.

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