Engineering the surface structure of MoS2 to preferentially expose active edge sites for electrocatalysis

Kibsgaard, Jakob; Chen, Zhebo; Reinecke, Benjamin N.; Jaramillo, Thomas F.

doi:10.1038/nmat3439

Cited by 3,234Electrocatalysts for Energy Conversion2D Materials and ApplicationsSupercapacitor Materials and Fabrication

Engineering the surface structure of MoS2 to preferentially expose active edge sites for electrocatalysis

Kibsgaard, Jakob, Chen, Zhebo, Reinecke, Benjamin N., Jaramillo, Thomas F.·2012·Nature Materials

DOI 10.1038/nmat3439

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Abstract

Controlling surface structure at the atomic scale is paramount to developing effective catalysts. For example, the edge sites of MoS(2) are highly catalytically active and are thus preferred at the catalyst surface over MoS(2) basal planes, which are inert. However, thermodynamics favours the presence of the basal plane, limiting the number of active sites at the surface. Herein, we engineer the surface structure of MoS(2) to preferentially expose edge sites to effect improved catalysis by successfully synthesizing contiguous large-area thin films of a highly ordered double-gyroid MoS(2) bicontinuous network with nanoscaled pores. The high surface curvature of this catalyst mesostructure exposes a large fraction of edge sites, which, along with its high surface area, leads to excellent activity for electrocatalytic hydrogen evolution. This work elucidates how morphological control of materials at the nanoscale can significantly impact the surface structure at the atomic scale, enabling new opportunities for enhancing surface properties for catalysis and other important technological applications.

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TMDs as co-catalysts can improve photocatalytic activity because active S atoms on exposed edges of 2D MoS2 can strongly bond with H+ in solution, enabling H+ reduction to H2.
“Numerous reports have demonstrated that TMDs as co-catalysts can improve the photocatalytic activity for two main reasons: i) the active S atoms on the exposed edges of 2D MoS 2 can strongly bond with H + in solution, enabling the H + reduction to H 2 . [ 20,24,40,50,111,112 ] In this way, the photocatalytic activity for HER can be greatly enhanced.”
From 2D Transition‐Metal‐Dichalcogenide‐Nanosheet‐Based Composites for Photocatalytic and Electrocatalytic Hydrogen Evolution Reactions (2016) · cites this paper as [112]
The Tafel slope (46 mV per decade) of the single-layer MoS2 nanosheet was comparable with that of the excellent MoS2-based catalyst.
“The Tafel slope (46 mV per decade) of the singlelayer MoS 2 nanosheet was also comparable with that of the excellent MoS 2 -based catalyst (Figure 7 g). [ 112 ]”
From 2D Transition‐Metal‐Dichalcogenide‐Nanosheet‐Based Composites for Photocatalytic and Electrocatalytic Hydrogen Evolution Reactions (2016) · cites this paper as [112]
The overpotential and Tafel slope of MoS2QD-aerogel-100 constitute the best catalytic activity reported for pure semiconducting-type MoS2 electrocatalysts up to the present.
“which is the best result for pure semiconducting type MoS2 electrocatalysts up until the present.”
From Highly Efficient Hydrogen Evolution from Seawater by Biofunctionalized Exfoliated MoS2 Quantum Dot Aerogel Electrocatalysts That Is Superior to Pt (2019) · cites this paper as [29]
Bimetal alloys and their derivatives (e.g., sulphides and phosphides) usually have better catalytic performance for the HER than for the OER.
“In contrast, bimetal alloys and their derivatives (e.g., sulphides and phosphides) usually have better catalytic performance for the HER than for the OER.21–23”
From Tunable CoFe-based active sites on 3D heteroatom doped graphene aerogel electrocatalysts via annealing gas regulation for efficient water splitting (2018) · cites this paper as [23]
Ultrathin architecture of TMD is favorable for exposing edge active sites to catalyze HER.
“The ultrathin architecture of TMD is favorable for exposing those active sites located on edges to catalyze HER.”
From Carbon-Nanotube-Incorporated Graphene Scroll-Sheet Conjoined Aerogels for Efficient Hydrogen Evolution Reaction (2017) · cites this paper as [7]

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Authors: Kibsgaard, J., Chen, Z., Reinecke, B. N., & Jaramillo, T. F.
Affiliations: Stanford University (US)
Corresponding author: Jaramillo, Thomas F.
ORCID: Kibsgaard, Jakob
Chen, Zhebo
Jaramillo, Thomas F.
Venue: Nature Materials
Publisher: Springer Science and Business Media LLC
Published: 2012-10-07
Volume: 11
Issue: 11
Pages: 963-969
ISSN: 1476-1122 (ISSN-L)
1476-4660
DOI: 10.1038/nmat3439
OpenAlex: W1981539053
Cited by: 3,234
References: 2
Citations by year: 2026: 109 · 2025: 130 · 2024: 133 · 2023: 181 · 2022: 211 · 2021: 251 · 2020: 293 · 2019: 336 · 2018: 401 · 2017: 378 · 2016: 304 · 2015: 245 · 2014: 188 · 2013: 70
FWCI: 61.61
Type: journal article
Language: en
Open access: closed
Licence: www.springer.com/tdm (tdm)
www.springer.com/tdm (vor)
Locations: Nature Materials (publishedVersion)
PubMed (publishedVersion)
Funders: U.S. Department of Energy (DESC0001060)
Topics: Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
Physical Sciences › Materials Science › Materials Chemistry › 2D Materials and Applications
Physical Sciences › Materials Science › Electronic, Optical and Magnetic Materials › Supercapacitor Materials and Fabrication
Keywords: MoS2, edge sites, surface structure engineering, electrocatalytic hydrogen evolution, nanoscale pores, surface curvature, basal plane

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Engineering the surface structure of MoS2 to preferentially expose active edge sites for electrocatalysis

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