Orbital coupling of hetero-diatomic nickel-iron site for bifunctional electrocatalysis of CO2 reduction and oxygen evolution

Zhiping Zeng; Li Yong Gan; Hong Bin Yang; Xiaozhi Su; Jiajian Gao; Wei Liu; Hiroaki Matsumoto; Jun Gong; Junming Zhang; Weizhen Cai; Zheye Zhang; Yibo Yan; Bin Liu; Peng Chen

doi:10.1038/s41467-021-24052-5

Orbital coupling of hetero-diatomic nickel-iron site for bifunctional electrocatalysis of CO₂ reduction and oxygen evolution

Zhiping Zeng
, Li Yong Gan
, Hong Bin Yang^*
, Xiaozhi Su
, Jiajian Gao
, Wei Liu
, Hiroaki Matsumoto
, Jun Gong
, Junming Zhang
, Weizhen Cai
, Zheye Zhang
, Yibo Yan
, Bin Liu^*
, Peng Chen^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

491 Citations (Scopus)

27 Downloads (CityUHK Scholars)

Abstract

While inheriting the exceptional merits of single atom catalysts, diatomic site catalysts (DASCs) utilize two adjacent atomic metal species for their complementary functionalities and synergistic actions. Herein, a DASC consisting of nickel-iron hetero-diatomic pairs anchored on nitrogen-doped graphene is synthesized. It exhibits extraordinary electrocatalytic activities and stability for both CO₂ reduction reaction (CO₂RR) and oxygen evolution reaction (OER). Furthermore, the rechargeable Zn-CO₂ battery equipped with such bifunctional catalyst shows high Faradaic efficiency and outstanding rechargeability. The in-depth experimental and theoretical analyses reveal the orbital coupling between the catalytic iron center and the adjacent nickel atom, which leads to alteration in orbital energy level, unique electronic states, higher oxidation state of iron, and weakened binding strength to the reaction intermediates, thus boosted CO₂RR and OER performance. This work provides critical insights to rational design, working mechanism, and application of hetero-DASCs. © 2021, The Author(s).

Original language	English
Article number	4088
Journal	Nature Communications
Volume	12
Issue number	1
Online published	2 Jul 2021
DOIs	https://doi.org/10.1038/s41467-021-24052-5
Publication status	Published - 2021
Externally published	Yes

Funding

This work was supported by AME-IRG grants (A1983c0025, A20E5c0080) from Agency for Science, Technology and Research of Singapore, AcRF tier 2 grants (MOE2017-T2-2-005, MOET2EP10120-0002) and an AcRF tier 1 grant (RG4/20) from Ministry of Education (Singapore), National Natural Science Foundation of China (NSFC, Grant Nos. 12074048 and 22075195), One-hundred Talents program of Sun Yat-sen University and Jiangsu Specially Appointed Professor program.

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 13 Climate Action

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This full text is made available under CC-BY 4.0. https://creativecommons.org/licenses/by/4.0/

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Cite this

@article{d70d9768c65940ec9dcd944ad8d2ce51,

title = "Orbital coupling of hetero-diatomic nickel-iron site for bifunctional electrocatalysis of CO2 reduction and oxygen evolution",

abstract = "While inheriting the exceptional merits of single atom catalysts, diatomic site catalysts (DASCs) utilize two adjacent atomic metal species for their complementary functionalities and synergistic actions. Herein, a DASC consisting of nickel-iron hetero-diatomic pairs anchored on nitrogen-doped graphene is synthesized. It exhibits extraordinary electrocatalytic activities and stability for both CO2 reduction reaction (CO2RR) and oxygen evolution reaction (OER). Furthermore, the rechargeable Zn-CO2 battery equipped with such bifunctional catalyst shows high Faradaic efficiency and outstanding rechargeability. The in-depth experimental and theoretical analyses reveal the orbital coupling between the catalytic iron center and the adjacent nickel atom, which leads to alteration in orbital energy level, unique electronic states, higher oxidation state of iron, and weakened binding strength to the reaction intermediates, thus boosted CO2RR and OER performance. This work provides critical insights to rational design, working mechanism, and application of hetero-DASCs. {\textcopyright} 2021, The Author(s).",

author = "Zhiping Zeng and Gan, \{Li Yong\} and \{Bin Yang\}, Hong and Xiaozhi Su and Jiajian Gao and Wei Liu and Hiroaki Matsumoto and Jun Gong and Junming Zhang and Weizhen Cai and Zheye Zhang and Yibo Yan and Bin Liu and Peng Chen",

year = "2021",

doi = "10.1038/s41467-021-24052-5",

language = "English",

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journal = "Nature Communications",

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TY - JOUR

T1 - Orbital coupling of hetero-diatomic nickel-iron site for bifunctional electrocatalysis of CO2 reduction and oxygen evolution

AU - Zeng, Zhiping

AU - Gan, Li Yong

AU - Bin Yang, Hong

AU - Su, Xiaozhi

AU - Gao, Jiajian

AU - Liu, Wei

AU - Matsumoto, Hiroaki

AU - Gong, Jun

AU - Zhang, Junming

AU - Cai, Weizhen

AU - Zhang, Zheye

AU - Yan, Yibo

AU - Liu, Bin

AU - Chen, Peng

PY - 2021

Y1 - 2021

N2 - While inheriting the exceptional merits of single atom catalysts, diatomic site catalysts (DASCs) utilize two adjacent atomic metal species for their complementary functionalities and synergistic actions. Herein, a DASC consisting of nickel-iron hetero-diatomic pairs anchored on nitrogen-doped graphene is synthesized. It exhibits extraordinary electrocatalytic activities and stability for both CO2 reduction reaction (CO2RR) and oxygen evolution reaction (OER). Furthermore, the rechargeable Zn-CO2 battery equipped with such bifunctional catalyst shows high Faradaic efficiency and outstanding rechargeability. The in-depth experimental and theoretical analyses reveal the orbital coupling between the catalytic iron center and the adjacent nickel atom, which leads to alteration in orbital energy level, unique electronic states, higher oxidation state of iron, and weakened binding strength to the reaction intermediates, thus boosted CO2RR and OER performance. This work provides critical insights to rational design, working mechanism, and application of hetero-DASCs. © 2021, The Author(s).

AB - While inheriting the exceptional merits of single atom catalysts, diatomic site catalysts (DASCs) utilize two adjacent atomic metal species for their complementary functionalities and synergistic actions. Herein, a DASC consisting of nickel-iron hetero-diatomic pairs anchored on nitrogen-doped graphene is synthesized. It exhibits extraordinary electrocatalytic activities and stability for both CO2 reduction reaction (CO2RR) and oxygen evolution reaction (OER). Furthermore, the rechargeable Zn-CO2 battery equipped with such bifunctional catalyst shows high Faradaic efficiency and outstanding rechargeability. The in-depth experimental and theoretical analyses reveal the orbital coupling between the catalytic iron center and the adjacent nickel atom, which leads to alteration in orbital energy level, unique electronic states, higher oxidation state of iron, and weakened binding strength to the reaction intermediates, thus boosted CO2RR and OER performance. This work provides critical insights to rational design, working mechanism, and application of hetero-DASCs. © 2021, The Author(s).

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U2 - 10.1038/s41467-021-24052-5

DO - 10.1038/s41467-021-24052-5

M3 - RGC 21 - Publication in refereed journal

C2 - 34215728

SN - 2041-1723

VL - 12

JO - Nature Communications

JF - Nature Communications

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