General synthesis of single-atom catalysts with high metal loading using graphene quantum dots

Chuan Xia; Yunrui Qiu; Yang Xia; Peng Zhu; Graham King; Xiao Zhang; Zhenyu Wu; Jung Yoon Kim; David A. Cullen; Dongxing Zheng; Peng Li; Mohsen Shakouri; Emilio Heredia; Peixin Cui; Husam N. Alshareef; Yongfeng Hu; Haotian Wang

doi:10.1038/s41557-021-00734-x

General synthesis of single-atom catalysts with high metal loading using graphene quantum dots

Chuan Xia, Yunrui Qiu, Yang Xia, Peng Zhu, Graham King, Xiao Zhang, Zhenyu Wu, Jung Yoon Kim, David A. Cullen, Dongxing Zheng, Peng Li, Mohsen Shakouri, Emilio Heredia, Peixin Cui, Husam N. Alshareef, Yongfeng Hu, Haotian Wang

Research output: Contribution to journal › Article › peer-review

422 Scopus citations

Abstract

Transition-metal single-atom catalysts present extraordinary activity per metal atomic site, but suffer from low metal-atom densities (typically less than 5 wt% or 1 at.%), which limits their overall catalytic performance. Here we report a general method for the synthesis of single-atom catalysts with high transition-metal-atom loadings of up to 40 wt% or 3.8 at.%, representing several-fold improvements compared to benchmarks in the literature. Graphene quantum dots, later interweaved into a carbon matrix, were used as a support, providing numerous anchoring sites and thus facilitating the generation of high densities of transition-metal atoms with sufficient spacing between the metal atoms to avoid aggregation. A significant increase in activity in electrochemical CO2 reduction (used as a representative reaction) was demonstrated on a Ni single-atom catalyst with increased Ni loading.

Original language	English (US)
Journal	Nature Chemistry
DOIs	https://doi.org/10.1038/s41557-021-00734-x
State	Published - Jun 24 2021

Bibliographical note

KAUST Repository Item: Exported on 2021-06-28
Acknowledgements: This work was supported by Rice University and the Welch Foundation Research Grant C-2051-20200401. H.W. is a CIFAR Azrieli Global Scholar in the Bio-inspired Solar Energy Program. C.X. acknowledges support from a J. Evans Attwell-Welch Postdoctoral Fellowship. C.X. acknowledges the University of Electronic Science and Technology of China for startup funding (A1098531023601264). This work was performed in part at the Shared Equipment Authority at Rice University. H.N.A. acknowledges support from King Abdullah University of Science and Technology. XAS and PDF measurements were conducted at the Canadian Light Source, which is supported by the Natural Sciences and Engineering Research Council of Canada (NSERC), National Research Council Canada (NRC) and University of Saskatchewan. Electron microscopy was conducted at the Center for Nanophase Materials Sciences, which is a U.S. Department of Energy Office of Science User Facility.

ASJC Scopus subject areas

General Chemical Engineering
General Chemistry

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title = "General synthesis of single-atom catalysts with high metal loading using graphene quantum dots",

abstract = "Transition-metal single-atom catalysts present extraordinary activity per metal atomic site, but suffer from low metal-atom densities (typically less than 5 wt% or 1 at.%), which limits their overall catalytic performance. Here we report a general method for the synthesis of single-atom catalysts with high transition-metal-atom loadings of up to 40 wt% or 3.8 at.%, representing several-fold improvements compared to benchmarks in the literature. Graphene quantum dots, later interweaved into a carbon matrix, were used as a support, providing numerous anchoring sites and thus facilitating the generation of high densities of transition-metal atoms with sufficient spacing between the metal atoms to avoid aggregation. A significant increase in activity in electrochemical CO2 reduction (used as a representative reaction) was demonstrated on a Ni single-atom catalyst with increased Ni loading.",

author = "Chuan Xia and Yunrui Qiu and Yang Xia and Peng Zhu and Graham King and Xiao Zhang and Zhenyu Wu and Kim, {Jung Yoon} and Cullen, {David A.} and Dongxing Zheng and Peng Li and Mohsen Shakouri and Emilio Heredia and Peixin Cui and Alshareef, {Husam N.} and Yongfeng Hu and Haotian Wang",

note = "KAUST Repository Item: Exported on 2021-06-28 Acknowledgements: This work was supported by Rice University and the Welch Foundation Research Grant C-2051-20200401. H.W. is a CIFAR Azrieli Global Scholar in the Bio-inspired Solar Energy Program. C.X. acknowledges support from a J. Evans Attwell-Welch Postdoctoral Fellowship. C.X. acknowledges the University of Electronic Science and Technology of China for startup funding (A1098531023601264). This work was performed in part at the Shared Equipment Authority at Rice University. H.N.A. acknowledges support from King Abdullah University of Science and Technology. XAS and PDF measurements were conducted at the Canadian Light Source, which is supported by the Natural Sciences and Engineering Research Council of Canada (NSERC), National Research Council Canada (NRC) and University of Saskatchewan. Electron microscopy was conducted at the Center for Nanophase Materials Sciences, which is a U.S. Department of Energy Office of Science User Facility.",

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AU - Xia, Chuan

AU - Qiu, Yunrui

AU - Xia, Yang

AU - Zhu, Peng

AU - King, Graham

AU - Zhang, Xiao

AU - Wu, Zhenyu

AU - Kim, Jung Yoon

AU - Cullen, David A.

AU - Zheng, Dongxing

AU - Li, Peng

AU - Shakouri, Mohsen

AU - Heredia, Emilio

AU - Cui, Peixin

AU - Alshareef, Husam N.

AU - Hu, Yongfeng

AU - Wang, Haotian

N1 - KAUST Repository Item: Exported on 2021-06-28 Acknowledgements: This work was supported by Rice University and the Welch Foundation Research Grant C-2051-20200401. H.W. is a CIFAR Azrieli Global Scholar in the Bio-inspired Solar Energy Program. C.X. acknowledges support from a J. Evans Attwell-Welch Postdoctoral Fellowship. C.X. acknowledges the University of Electronic Science and Technology of China for startup funding (A1098531023601264). This work was performed in part at the Shared Equipment Authority at Rice University. H.N.A. acknowledges support from King Abdullah University of Science and Technology. XAS and PDF measurements were conducted at the Canadian Light Source, which is supported by the Natural Sciences and Engineering Research Council of Canada (NSERC), National Research Council Canada (NRC) and University of Saskatchewan. Electron microscopy was conducted at the Center for Nanophase Materials Sciences, which is a U.S. Department of Energy Office of Science User Facility.

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N2 - Transition-metal single-atom catalysts present extraordinary activity per metal atomic site, but suffer from low metal-atom densities (typically less than 5 wt% or 1 at.%), which limits their overall catalytic performance. Here we report a general method for the synthesis of single-atom catalysts with high transition-metal-atom loadings of up to 40 wt% or 3.8 at.%, representing several-fold improvements compared to benchmarks in the literature. Graphene quantum dots, later interweaved into a carbon matrix, were used as a support, providing numerous anchoring sites and thus facilitating the generation of high densities of transition-metal atoms with sufficient spacing between the metal atoms to avoid aggregation. A significant increase in activity in electrochemical CO2 reduction (used as a representative reaction) was demonstrated on a Ni single-atom catalyst with increased Ni loading.

AB - Transition-metal single-atom catalysts present extraordinary activity per metal atomic site, but suffer from low metal-atom densities (typically less than 5 wt% or 1 at.%), which limits their overall catalytic performance. Here we report a general method for the synthesis of single-atom catalysts with high transition-metal-atom loadings of up to 40 wt% or 3.8 at.%, representing several-fold improvements compared to benchmarks in the literature. Graphene quantum dots, later interweaved into a carbon matrix, were used as a support, providing numerous anchoring sites and thus facilitating the generation of high densities of transition-metal atoms with sufficient spacing between the metal atoms to avoid aggregation. A significant increase in activity in electrochemical CO2 reduction (used as a representative reaction) was demonstrated on a Ni single-atom catalyst with increased Ni loading.

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SN - 1755-4330

JO - Nature Chemistry

JF - Nature Chemistry

ER -

General synthesis of single-atom catalysts with high metal loading using graphene quantum dots

Abstract

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