Negative Pressure Pyrolysis Induced Highly Accessible Single Sites Dispersed on 3D Graphene Frameworks for Enhanced Oxygen Reduction

Huang Zhou; Tong Yang; Zongkui Kou; Lei Shen; Yafei Zhao; Zhiyuan Wang; Xiaoqian Wang; Zhenkun Yang; Junyi Du; Jie Xu; Min Chen; Lin Tian; Wenxin Guo; Qiuping Wang; Hongwei Lv; Wenxing Chen; Xun Hong; Jun Luo; Daping He; Yuen Wu

doi:10.1002/anie.202009700

Negative Pressure Pyrolysis Induced Highly Accessible Single Sites Dispersed on 3D Graphene Frameworks for Enhanced Oxygen Reduction

Huang Zhou, Tong Yang, Zongkui Kou, Lei Shen, Yafei Zhao, Zhiyuan Wang, Xiaoqian Wang, Zhenkun Yang, Junyi Du, Jie Xu, Min Chen, Lin Tian, Wenxin Guo, Qiuping Wang, Hongwei Lv, Wenxing Chen, Xun Hong, Jun Luo, Daping He^*, Yuen Wu^*

^*Corresponding author for this work

School of Material Science and Engineering

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

119 Citations (Scopus)

Abstract

Herein, we report a negative pressure pyrolysis to access dense single metal sites (Co, Fe, Ni etc.) with high accessibility dispersed on three-dimensional (3D) graphene frameworks (GFs), during which the differential pressure between inside and outside of metal–organic frameworks (MOFs) promotes the cleavage of the derived carbon layers and gradual expansion of mesopores. In situ transmission electron microscopy and Brunauer–Emmett–Teller tests reveal that the formed 3D GFs possess an enhanced mesoporosity and external surface area, which greatly favor the mass transport and utilization of metal sites. This contributes to an excellent oxygen reduction reaction (ORR) activity (half-wave potential of 0.901 V vs. RHE). Theoretical calculations verify that selective carbon cleavage near Co centers can efficiently lower the overall ORR theoretical overpotential in comparison with intact atomic configuration.

Original language	English
Pages (from-to)	20465-20469
Number of pages	5
Journal	Angewandte Chemie - International Edition
Volume	59
Issue number	46
DOIs	https://doi.org/10.1002/anie.202009700
Publication status	Published - 9 Nov 2020

Keywords

3D graphene frameworks
metal–organic frameworks
negative pressure
oxygen reduction reaction
single sites

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Zhou, H., Yang, T., Kou, Z., Shen, L., Zhao, Y., Wang, Z., Wang, X., Yang, Z., Du, J., Xu, J., Chen, M., Tian, L., Guo, W., Wang, Q., Lv, H., Chen, W., Hong, X., Luo, J., He, D., & Wu, Y. (2020). Negative Pressure Pyrolysis Induced Highly Accessible Single Sites Dispersed on 3D Graphene Frameworks for Enhanced Oxygen Reduction. Angewandte Chemie - International Edition, 59(46), 20465-20469. https://doi.org/10.1002/anie.202009700

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title = "Negative Pressure Pyrolysis Induced Highly Accessible Single Sites Dispersed on 3D Graphene Frameworks for Enhanced Oxygen Reduction",

abstract = "Herein, we report a negative pressure pyrolysis to access dense single metal sites (Co, Fe, Ni etc.) with high accessibility dispersed on three-dimensional (3D) graphene frameworks (GFs), during which the differential pressure between inside and outside of metal–organic frameworks (MOFs) promotes the cleavage of the derived carbon layers and gradual expansion of mesopores. In situ transmission electron microscopy and Brunauer–Emmett–Teller tests reveal that the formed 3D GFs possess an enhanced mesoporosity and external surface area, which greatly favor the mass transport and utilization of metal sites. This contributes to an excellent oxygen reduction reaction (ORR) activity (half-wave potential of 0.901 V vs. RHE). Theoretical calculations verify that selective carbon cleavage near Co centers can efficiently lower the overall ORR theoretical overpotential in comparison with intact atomic configuration.",

keywords = "3D graphene frameworks, metal–organic frameworks, negative pressure, oxygen reduction reaction, single sites",

author = "Huang Zhou and Tong Yang and Zongkui Kou and Lei Shen and Yafei Zhao and Zhiyuan Wang and Xiaoqian Wang and Zhenkun Yang and Junyi Du and Jie Xu and Min Chen and Lin Tian and Wenxin Guo and Qiuping Wang and Hongwei Lv and Wenxing Chen and Xun Hong and Jun Luo and Daping He and Yuen Wu",

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year = "2020",

month = nov,

day = "9",

doi = "10.1002/anie.202009700",

language = "English",

volume = "59",

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Zhou, H, Yang, T, Kou, Z, Shen, L, Zhao, Y, Wang, Z, Wang, X, Yang, Z, Du, J, Xu, J, Chen, M, Tian, L, Guo, W, Wang, Q, Lv, H, Chen, W, Hong, X, Luo, J, He, D & Wu, Y 2020, 'Negative Pressure Pyrolysis Induced Highly Accessible Single Sites Dispersed on 3D Graphene Frameworks for Enhanced Oxygen Reduction', Angewandte Chemie - International Edition, vol. 59, no. 46, pp. 20465-20469. https://doi.org/10.1002/anie.202009700

TY - JOUR

T1 - Negative Pressure Pyrolysis Induced Highly Accessible Single Sites Dispersed on 3D Graphene Frameworks for Enhanced Oxygen Reduction

AU - Zhou, Huang

AU - Yang, Tong

AU - Kou, Zongkui

AU - Shen, Lei

AU - Zhao, Yafei

AU - Wang, Zhiyuan

AU - Wang, Xiaoqian

AU - Yang, Zhenkun

AU - Du, Junyi

AU - Xu, Jie

AU - Chen, Min

AU - Tian, Lin

AU - Guo, Wenxin

AU - Wang, Qiuping

AU - Lv, Hongwei

AU - Chen, Wenxing

AU - Hong, Xun

AU - Luo, Jun

AU - He, Daping

AU - Wu, Yuen

PY - 2020/11/9

Y1 - 2020/11/9

N2 - Herein, we report a negative pressure pyrolysis to access dense single metal sites (Co, Fe, Ni etc.) with high accessibility dispersed on three-dimensional (3D) graphene frameworks (GFs), during which the differential pressure between inside and outside of metal–organic frameworks (MOFs) promotes the cleavage of the derived carbon layers and gradual expansion of mesopores. In situ transmission electron microscopy and Brunauer–Emmett–Teller tests reveal that the formed 3D GFs possess an enhanced mesoporosity and external surface area, which greatly favor the mass transport and utilization of metal sites. This contributes to an excellent oxygen reduction reaction (ORR) activity (half-wave potential of 0.901 V vs. RHE). Theoretical calculations verify that selective carbon cleavage near Co centers can efficiently lower the overall ORR theoretical overpotential in comparison with intact atomic configuration.

AB - Herein, we report a negative pressure pyrolysis to access dense single metal sites (Co, Fe, Ni etc.) with high accessibility dispersed on three-dimensional (3D) graphene frameworks (GFs), during which the differential pressure between inside and outside of metal–organic frameworks (MOFs) promotes the cleavage of the derived carbon layers and gradual expansion of mesopores. In situ transmission electron microscopy and Brunauer–Emmett–Teller tests reveal that the formed 3D GFs possess an enhanced mesoporosity and external surface area, which greatly favor the mass transport and utilization of metal sites. This contributes to an excellent oxygen reduction reaction (ORR) activity (half-wave potential of 0.901 V vs. RHE). Theoretical calculations verify that selective carbon cleavage near Co centers can efficiently lower the overall ORR theoretical overpotential in comparison with intact atomic configuration.

KW - 3D graphene frameworks

KW - metal–organic frameworks

KW - negative pressure

KW - oxygen reduction reaction

KW - single sites

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U2 - 10.1002/anie.202009700

DO - 10.1002/anie.202009700

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AN - SCOPUS:85090142573

SN - 1433-7851

VL - 59

SP - 20465

EP - 20469

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 46

ER -

Negative Pressure Pyrolysis Induced Highly Accessible Single Sites Dispersed on 3D Graphene Frameworks for Enhanced Oxygen Reduction

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Keywords

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