In situ formation of molecular Ni-Fe active sites on heteroatom-doped graphene as a heterogeneous electrocatalyst toward oxygen evolution

Jiong Wang; Liyong Gan; Wenyu Zhang; Yuecheng Peng; Hong Yu; Qingyu Yan; Xinghua Xia; Xin Wang

doi:10.1126/sciadv.aap7970

In situ formation of molecular Ni-Fe active sites on heteroatom-doped graphene as a heterogeneous electrocatalyst toward oxygen evolution

Jiong Wang
, Liyong Gan
, Wenyu Zhang
, Yuecheng Peng
, Hong Yu
, Qingyu Yan
, Xinghua Xia
, Xin Wang^*

^*Corresponding author for this work

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

274 Citations (Scopus)

26 Downloads (CityUHK Scholars)

Abstract

Molecularly well-defined Ni sites at heterogeneous interfaces were derived from the incorporation of Ni³⁺ ions into heteroatom-doped graphene. The molecular Ni sites on graphene were redox-Active. However, they showed poor activity toward oxygen evolution reaction (OER) in KOH aqueous solution. We demonstrated for the first time that the presence of Fe³⁺ ions in the solution could bond at the vicinity of the Ni sites with a distance of 2.7 A, generating molecularly sized and heterogeneous Ni-Fe sites anchored on doped graphene. These Ni-Fe sites exhibited markedly improved OER activity. The Pourbaix diagram confirmed the formation of the Ni-Fe sites and revealed that the Ni-Fe sites adsorbed HO- ions with a bridge geometry, which facilitated the OER electrocatalysis. © 2018 American Association for the Advancement of Science. All rights reserved.

Original language	English
Article number	eaap7970
Journal	Science Advances
Volume	4
Issue number	3
DOIs	https://doi.org/10.1126/sciadv.aap7970
Publication status	Published - 9 Mar 2018
Externally published	Yes

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Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to [email protected].

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title = "In situ formation of molecular Ni-Fe active sites on heteroatom-doped graphene as a heterogeneous electrocatalyst toward oxygen evolution",

abstract = "Molecularly well-defined Ni sites at heterogeneous interfaces were derived from the incorporation of Ni3+ ions into heteroatom-doped graphene. The molecular Ni sites on graphene were redox-Active. However, they showed poor activity toward oxygen evolution reaction (OER) in KOH aqueous solution. We demonstrated for the first time that the presence of Fe3+ ions in the solution could bond at the vicinity of the Ni sites with a distance of 2.7 A, generating molecularly sized and heterogeneous Ni-Fe sites anchored on doped graphene. These Ni-Fe sites exhibited markedly improved OER activity. The Pourbaix diagram confirmed the formation of the Ni-Fe sites and revealed that the Ni-Fe sites adsorbed HO- ions with a bridge geometry, which facilitated the OER electrocatalysis. {\textcopyright} 2018 American Association for the Advancement of Science. All rights reserved.",

author = "Jiong Wang and Liyong Gan and Wenyu Zhang and Yuecheng Peng and Hong Yu and Qingyu Yan and Xinghua Xia and Xin Wang",

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T1 - In situ formation of molecular Ni-Fe active sites on heteroatom-doped graphene as a heterogeneous electrocatalyst toward oxygen evolution

AU - Wang, Jiong

AU - Gan, Liyong

AU - Zhang, Wenyu

AU - Peng, Yuecheng

AU - Yu, Hong

AU - Yan, Qingyu

AU - Xia, Xinghua

AU - Wang, Xin

N1 - Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to [email protected].

PY - 2018/3/9

Y1 - 2018/3/9

N2 - Molecularly well-defined Ni sites at heterogeneous interfaces were derived from the incorporation of Ni3+ ions into heteroatom-doped graphene. The molecular Ni sites on graphene were redox-Active. However, they showed poor activity toward oxygen evolution reaction (OER) in KOH aqueous solution. We demonstrated for the first time that the presence of Fe3+ ions in the solution could bond at the vicinity of the Ni sites with a distance of 2.7 A, generating molecularly sized and heterogeneous Ni-Fe sites anchored on doped graphene. These Ni-Fe sites exhibited markedly improved OER activity. The Pourbaix diagram confirmed the formation of the Ni-Fe sites and revealed that the Ni-Fe sites adsorbed HO- ions with a bridge geometry, which facilitated the OER electrocatalysis. © 2018 American Association for the Advancement of Science. All rights reserved.

AB - Molecularly well-defined Ni sites at heterogeneous interfaces were derived from the incorporation of Ni3+ ions into heteroatom-doped graphene. The molecular Ni sites on graphene were redox-Active. However, they showed poor activity toward oxygen evolution reaction (OER) in KOH aqueous solution. We demonstrated for the first time that the presence of Fe3+ ions in the solution could bond at the vicinity of the Ni sites with a distance of 2.7 A, generating molecularly sized and heterogeneous Ni-Fe sites anchored on doped graphene. These Ni-Fe sites exhibited markedly improved OER activity. The Pourbaix diagram confirmed the formation of the Ni-Fe sites and revealed that the Ni-Fe sites adsorbed HO- ions with a bridge geometry, which facilitated the OER electrocatalysis. © 2018 American Association for the Advancement of Science. All rights reserved.

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U2 - 10.1126/sciadv.aap7970

DO - 10.1126/sciadv.aap7970

M3 - RGC 21 - Publication in refereed journal

C2 - 29536041

SN - 2375-2548

VL - 4

JO - Science Advances

JF - Science Advances

IS - 3

M1 - eaap7970

ER -

In situ formation of molecular Ni-Fe active sites on heteroatom-doped graphene as a heterogeneous electrocatalyst toward oxygen evolution

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