Boosting alkaline hydrogen evolution: The dominating role of interior modification in surface electrocatalysis

Zhao Li; Wenhan Niu; Zhenzhong Yang; Abdelkader Kara; Qi Wang; Maoyu Wang; Meng Gu; Zhenxing Feng; Yingge Du; Yang Yang

doi:10.1039/d0ee01750g

Boosting alkaline hydrogen evolution: The dominating role of interior modification in surface electrocatalysis

Zhao Li (Co-first Author)
, Wenhan Niu (Co-first Author)
, Zhenzhong Yang (Co-first Author)
, Abdelkader Kara
, Qi Wang
, Maoyu Wang
, Meng Gu^*
, Zhenxing Feng^*
, Yingge Du^*
, Yang Yang^*

^*Corresponding author for this work

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

114 Citations (Scopus)

Abstract

The alkaline hydrogen evolution reaction (A-HER) holds great promise for clean hydrogen fuel generation but its practical utilization is severely hindered by the sluggish kinetics for water dissociation in alkaline solutions. Traditional ways to improve the electrochemical kinetics for A-HER catalysts have been focusing on surface modification, which still can not meet the demanding requirements for practical water electrolysis because of catalyst surface deactivation. Herein, we report an interior modification strategy to significantly boost the A-HER performance. Specifically, a trace amount of Pt was doped in the interior Co₂P (Pt-Co₂P) to introduce a stronger dopant-host interaction than that of the surface-modified catalyst. Consequently, the local chemical state and electronic structure of the catalysts were adjusted to improve the electron mobility and reduce the energy barriers for hydrogen adsorption and H-H bond formation. As a proof-of-concept, the interior-modified Pt-Co₂P shows a reduced onset potential at near-zero volts for the A-HER, low overpotentials of 2 mV and 58 mV to achieve 10 and 100 mA cm^-2, and excellent durability for long-term utilization. The interior-modified Pt-Co₂P delivers superior A-HER performance to Pt/C and other state-of-the-art electrocatalysts. This work will open a new avenue for A-HER catalyst design. © The Royal Society of Chemistry 2020

Original language	English
Pages (from-to)	3110-3118
Journal	Energy and Environmental Science
Volume	13
Issue number	9
Online published	31 Jul 2020
DOIs	https://doi.org/10.1039/d0ee01750g
Publication status	Published - 1 Sept 2020
Externally published	Yes

Funding

This work was supported by the National Science Foundation under Grant No. CMMI-1851674 and the startup grant from the University of Central Florida. The XPS test was supported by the NSF MRI XPS: ECCS: 1726636, hosted in the MCF-AMPAC facility, MSE, CECS, UCF. TEM and data analysis were supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Early Career Research Program under award # 68278. A portion of the research was performed using EMSL, a DOE User Facility sponsored by the Office of Biological and Environmental Research and located at the Pacific Northwest National Laboratory. Part of the microscopy work of MG was supported by the National Natural Science Foundation of China (No. 21802065). The computational work of AK is supported by the U.S. Department of Energy Basic Energy Science under Contract No DE-FG02-11ER16243. Resources of the National Energy Research Scientific Computing Center (NERSC) were used for the computational part of this paper. This research used resources of the beamline 5-BM-D, of DND-CAT at the Advanced Photon Source (APS), a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract DE-AC02-06CH11357. DND-CAT is supported through E. I. duPont de Nemours & Co., Northwestern University, and The Dow Chemical Company.

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SDG 7 Affordable and Clean Energy

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title = "Boosting alkaline hydrogen evolution: The dominating role of interior modification in surface electrocatalysis",

abstract = "The alkaline hydrogen evolution reaction (A-HER) holds great promise for clean hydrogen fuel generation but its practical utilization is severely hindered by the sluggish kinetics for water dissociation in alkaline solutions. Traditional ways to improve the electrochemical kinetics for A-HER catalysts have been focusing on surface modification, which still can not meet the demanding requirements for practical water electrolysis because of catalyst surface deactivation. Herein, we report an interior modification strategy to significantly boost the A-HER performance. Specifically, a trace amount of Pt was doped in the interior Co2P (Pt-Co2P) to introduce a stronger dopant-host interaction than that of the surface-modified catalyst. Consequently, the local chemical state and electronic structure of the catalysts were adjusted to improve the electron mobility and reduce the energy barriers for hydrogen adsorption and H-H bond formation. As a proof-of-concept, the interior-modified Pt-Co2P shows a reduced onset potential at near-zero volts for the A-HER, low overpotentials of 2 mV and 58 mV to achieve 10 and 100 mA cm-2, and excellent durability for long-term utilization. The interior-modified Pt-Co2P delivers superior A-HER performance to Pt/C and other state-of-the-art electrocatalysts. This work will open a new avenue for A-HER catalyst design. {\textcopyright} The Royal Society of Chemistry 2020",

author = "Zhao Li and Wenhan Niu and Zhenzhong Yang and Abdelkader Kara and Qi Wang and Maoyu Wang and Meng Gu and Zhenxing Feng and Yingge Du and Yang Yang",

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Boosting alkaline hydrogen evolution: The dominating role of interior modification in surface electrocatalysis. / Li, Zhao (Co-first Author); Niu, Wenhan (Co-first Author); Yang, Zhenzhong (Co-first Author) et al.
In: Energy and Environmental Science, Vol. 13, No. 9, 01.09.2020, p. 3110-3118.

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

TY - JOUR

T1 - Boosting alkaline hydrogen evolution

T2 - The dominating role of interior modification in surface electrocatalysis

AU - Li, Zhao

AU - Niu, Wenhan

AU - Yang, Zhenzhong

AU - Kara, Abdelkader

AU - Wang, Qi

AU - Wang, Maoyu

AU - Gu, Meng

AU - Feng, Zhenxing

AU - Du, Yingge

AU - Yang, Yang

PY - 2020/9/1

Y1 - 2020/9/1

N2 - The alkaline hydrogen evolution reaction (A-HER) holds great promise for clean hydrogen fuel generation but its practical utilization is severely hindered by the sluggish kinetics for water dissociation in alkaline solutions. Traditional ways to improve the electrochemical kinetics for A-HER catalysts have been focusing on surface modification, which still can not meet the demanding requirements for practical water electrolysis because of catalyst surface deactivation. Herein, we report an interior modification strategy to significantly boost the A-HER performance. Specifically, a trace amount of Pt was doped in the interior Co2P (Pt-Co2P) to introduce a stronger dopant-host interaction than that of the surface-modified catalyst. Consequently, the local chemical state and electronic structure of the catalysts were adjusted to improve the electron mobility and reduce the energy barriers for hydrogen adsorption and H-H bond formation. As a proof-of-concept, the interior-modified Pt-Co2P shows a reduced onset potential at near-zero volts for the A-HER, low overpotentials of 2 mV and 58 mV to achieve 10 and 100 mA cm-2, and excellent durability for long-term utilization. The interior-modified Pt-Co2P delivers superior A-HER performance to Pt/C and other state-of-the-art electrocatalysts. This work will open a new avenue for A-HER catalyst design. © The Royal Society of Chemistry 2020

AB - The alkaline hydrogen evolution reaction (A-HER) holds great promise for clean hydrogen fuel generation but its practical utilization is severely hindered by the sluggish kinetics for water dissociation in alkaline solutions. Traditional ways to improve the electrochemical kinetics for A-HER catalysts have been focusing on surface modification, which still can not meet the demanding requirements for practical water electrolysis because of catalyst surface deactivation. Herein, we report an interior modification strategy to significantly boost the A-HER performance. Specifically, a trace amount of Pt was doped in the interior Co2P (Pt-Co2P) to introduce a stronger dopant-host interaction than that of the surface-modified catalyst. Consequently, the local chemical state and electronic structure of the catalysts were adjusted to improve the electron mobility and reduce the energy barriers for hydrogen adsorption and H-H bond formation. As a proof-of-concept, the interior-modified Pt-Co2P shows a reduced onset potential at near-zero volts for the A-HER, low overpotentials of 2 mV and 58 mV to achieve 10 and 100 mA cm-2, and excellent durability for long-term utilization. The interior-modified Pt-Co2P delivers superior A-HER performance to Pt/C and other state-of-the-art electrocatalysts. This work will open a new avenue for A-HER catalyst design. © The Royal Society of Chemistry 2020

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DO - 10.1039/d0ee01750g

M3 - RGC 21 - Publication in refereed journal

SN - 1754-5692

VL - 13

SP - 3110

EP - 3118

JO - Energy and Environmental Science

JF - Energy and Environmental Science

IS - 9

ER -

Boosting alkaline hydrogen evolution: The dominating role of interior modification in surface electrocatalysis

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