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Active site manipulation in MoS2 cluster electrocatalysts by transition metal doping

Jo J. L. Humphrey, Rasmus Kronberg, Rongsheng Cai Orcid Logo, Kari Laasonen, Richard Palmer Orcid Logo, Andrew J. Wain

Nanoscale, Volume: 12, Pages: 4459 - 4472

Swansea University Authors: Rongsheng Cai Orcid Logo, Richard Palmer Orcid Logo

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DOI (Published version): 10.1039/c9nr10702a

Abstract

The development of non-platinum group metal catalysts for the hydrogen evolution reaction (HER) in water electrolyser devices is essential for their widespread and sustainable deployment. In recent years, molybdenum disulfide (MoS2) catalysts have received significant attention as they not only exhi...

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Published in: Nanoscale
ISSN: 2040-3364 2040-3372
Published: Royal Society of Chemistry (RSC) 2020
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URI: https://cronfa.swan.ac.uk/Record/cronfa53484
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spelling 2020-02-10T12:49:03.5819985 v2 53484 2020-02-10 Active site manipulation in MoS2 cluster electrocatalysts by transition metal doping c2d38332a07bde5ce1ce66d8750f652e 0000-0002-2148-0563 Rongsheng Cai Rongsheng Cai true false 6ae369618efc7424d9774377536ea519 0000-0001-8728-8083 Richard Palmer Richard Palmer true false 2020-02-10 EEN The development of non-platinum group metal catalysts for the hydrogen evolution reaction (HER) in water electrolyser devices is essential for their widespread and sustainable deployment. In recent years, molybdenum disulfide (MoS2) catalysts have received significant attention as they not only exhibit good electrocatalytic HER activity but also, crucially, acid-stability. However, further performance enhancement is required for these materials to be competitive with Pt and to that end transition metal doping of MoS2 has been explored as a route to further increasing its catalytic activity. In this work, cluster beam deposition was employed to produce controlled cobalt-doped MoS2 clusters (MoS2–Co). We demonstrate that, in contrast to previous observations of performance enhancement in MoS2 resulting from nickel doping (MoS2–Ni), the introduction of Co has a detrimental effect on HER activity. The contrasting behaviours of Ni and Co doping are rationalized by density functional theory (DFT) calculations, which suggest that HER-active surface vacancies are deactivated by combination with Co dopant atoms, whilst their activity is retained, or even partially enhanced, by combination with Ni dopant atoms. Furthermore, the adatom dopant–vacancy combination kinetics appear to be more than three orders of magnitude faster in MoS2–Co than for MoS2–Ni. These findings highlight a fundamental difference in the influence of transition metal dopants on the HER performance of MoS2 electrocatalysts and stress the importance of considering surface atomic defects when predicting their behaviour. Journal Article Nanoscale 12 4459 4472 Royal Society of Chemistry (RSC) 2040-3364 2040-3372 21 2 2020 2020-02-21 10.1039/c9nr10702a COLLEGE NANME Engineering COLLEGE CODE EEN Swansea University 2020-02-10T12:49:03.5819985 2020-02-10T12:49:03.5819985 Jo J. L. Humphrey 1 Rasmus Kronberg 2 Rongsheng Cai 0000-0002-2148-0563 3 Kari Laasonen 4 Richard Palmer 0000-0001-8728-8083 5 Andrew J. Wain 6 53484__16681__2777fb333cc84b228950dd71cfb1995f.pdf 53484.pdf 2020-02-24T17:15:01.0702194 Output 1099609 application/pdf Accepted Manuscript true 2021-02-07T00:00:00.0000000 true eng
title Active site manipulation in MoS2 cluster electrocatalysts by transition metal doping
spellingShingle Active site manipulation in MoS2 cluster electrocatalysts by transition metal doping
Rongsheng Cai
Richard Palmer
title_short Active site manipulation in MoS2 cluster electrocatalysts by transition metal doping
title_full Active site manipulation in MoS2 cluster electrocatalysts by transition metal doping
title_fullStr Active site manipulation in MoS2 cluster electrocatalysts by transition metal doping
title_full_unstemmed Active site manipulation in MoS2 cluster electrocatalysts by transition metal doping
title_sort Active site manipulation in MoS2 cluster electrocatalysts by transition metal doping
author_id_str_mv c2d38332a07bde5ce1ce66d8750f652e
6ae369618efc7424d9774377536ea519
author_id_fullname_str_mv c2d38332a07bde5ce1ce66d8750f652e_***_Rongsheng Cai
6ae369618efc7424d9774377536ea519_***_Richard Palmer
author Rongsheng Cai
Richard Palmer
author2 Jo J. L. Humphrey
Rasmus Kronberg
Rongsheng Cai
Kari Laasonen
Richard Palmer
Andrew J. Wain
format Journal article
container_title Nanoscale
container_volume 12
container_start_page 4459
publishDate 2020
institution Swansea University
issn 2040-3364
2040-3372
doi_str_mv 10.1039/c9nr10702a
publisher Royal Society of Chemistry (RSC)
document_store_str 1
active_str 0
description The development of non-platinum group metal catalysts for the hydrogen evolution reaction (HER) in water electrolyser devices is essential for their widespread and sustainable deployment. In recent years, molybdenum disulfide (MoS2) catalysts have received significant attention as they not only exhibit good electrocatalytic HER activity but also, crucially, acid-stability. However, further performance enhancement is required for these materials to be competitive with Pt and to that end transition metal doping of MoS2 has been explored as a route to further increasing its catalytic activity. In this work, cluster beam deposition was employed to produce controlled cobalt-doped MoS2 clusters (MoS2–Co). We demonstrate that, in contrast to previous observations of performance enhancement in MoS2 resulting from nickel doping (MoS2–Ni), the introduction of Co has a detrimental effect on HER activity. The contrasting behaviours of Ni and Co doping are rationalized by density functional theory (DFT) calculations, which suggest that HER-active surface vacancies are deactivated by combination with Co dopant atoms, whilst their activity is retained, or even partially enhanced, by combination with Ni dopant atoms. Furthermore, the adatom dopant–vacancy combination kinetics appear to be more than three orders of magnitude faster in MoS2–Co than for MoS2–Ni. These findings highlight a fundamental difference in the influence of transition metal dopants on the HER performance of MoS2 electrocatalysts and stress the importance of considering surface atomic defects when predicting their behaviour.
published_date 2020-02-21T04:06:25Z
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score 11.012678

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