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Title: Understanding catalysis in a multiphasic two-dimensional transition metal dichalcogenide.

Abstract

Establishing processing–structure–property relationships for monolayer materials is crucial for a range of applications spanning optics, catalysis, electronics and energy. Presently, for molybdenum disulfide, a promising catalyst for artificial photosynthesis, considerable debate surrounds the structure/property relationships of its various allotropes. Here we unambiguously solve the structure of molybdenum disulfide monolayers using high-resolution transmission electron microscopy supported by density functional theory and show lithium intercalation to direct a preferential transformation of the basal plane from 2H (trigonal prismatic) to 1T' (clustered Mo). These changes alter the energetics of molybdenum disulfide interactions with hydrogen (ΔGH), and, with respect to catalysis, the 1T' transformation renders the normally inert basal plane amenable towards hydrogen adsorption and hydrogen evolution. Furthermore, we show basal plane activation of 1T' molybdenum disulfide and a lowering of ΔGH from +1.6 eV for 2H to +0.18 eV for 1T', comparable to 2H molybdenum disulfide edges on Au(111), one of the most active hydrogen evolution catalysts known.

Authors:
 [1];  [2];  [1];  [1];  [1];  [3];  [1];  [4];  [4]
+ Show Author Affiliations
  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  2. Univ. of Texas, Austin, TX (United States)
  3. Univ. of New Mexico, Albuquerque, NM (United States)
  4. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Univ. of New Mexico, Albuquerque, NM (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1236234
Report Number(s):
SAND-2015-5948J
Journal ID: ISSN 2041-1723; 618380
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal Issue: 10; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; 08 HYDROGEN; chemical sciences; catalysis; materials science; physical chemistry

Citation Formats

Chou, Stanley Shihyao, Sai, Na, Lu, Ping, Coker, Eric Nicholas, Liu, Sheng, Artyushkova, Kateryna, Luk, Ting S., Kaehr, Bryan James, and Brinker, C. Jeffrey. Understanding catalysis in a multiphasic two-dimensional transition metal dichalcogenide.. United States: N. p., 2015. Web. doi:10.1038/ncomms9311.
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Chou, Stanley Shihyao, Sai, Na, Lu, Ping, Coker, Eric Nicholas, Liu, Sheng, Artyushkova, Kateryna, Luk, Ting S., Kaehr, Bryan James, & Brinker, C. Jeffrey. Understanding catalysis in a multiphasic two-dimensional transition metal dichalcogenide.. United States. https://doi.org/10.1038/ncomms9311
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Chou, Stanley Shihyao, Sai, Na, Lu, Ping, Coker, Eric Nicholas, Liu, Sheng, Artyushkova, Kateryna, Luk, Ting S., Kaehr, Bryan James, and Brinker, C. Jeffrey. Wed . "Understanding catalysis in a multiphasic two-dimensional transition metal dichalcogenide.". United States. https://doi.org/10.1038/ncomms9311. https://www.osti.gov/servlets/purl/1236234.
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@article{osti_1236234,
title = {Understanding catalysis in a multiphasic two-dimensional transition metal dichalcogenide.},
author = {Chou, Stanley Shihyao and Sai, Na and Lu, Ping and Coker, Eric Nicholas and Liu, Sheng and Artyushkova, Kateryna and Luk, Ting S. and Kaehr, Bryan James and Brinker, C. Jeffrey},
abstractNote = {Establishing processing–structure–property relationships for monolayer materials is crucial for a range of applications spanning optics, catalysis, electronics and energy. Presently, for molybdenum disulfide, a promising catalyst for artificial photosynthesis, considerable debate surrounds the structure/property relationships of its various allotropes. Here we unambiguously solve the structure of molybdenum disulfide monolayers using high-resolution transmission electron microscopy supported by density functional theory and show lithium intercalation to direct a preferential transformation of the basal plane from 2H (trigonal prismatic) to 1T' (clustered Mo). These changes alter the energetics of molybdenum disulfide interactions with hydrogen (ΔGH), and, with respect to catalysis, the 1T' transformation renders the normally inert basal plane amenable towards hydrogen adsorption and hydrogen evolution. Furthermore, we show basal plane activation of 1T' molybdenum disulfide and a lowering of ΔGH from +1.6 eV for 2H to +0.18 eV for 1T', comparable to 2H molybdenum disulfide edges on Au(111), one of the most active hydrogen evolution catalysts known.},
doi = {10.1038/ncomms9311},
journal = {Nature Communications},
number = 10,
volume = 6,
place = {United States},
year = {Wed Oct 07 00:00:00 EDT 2015},
month = {Wed Oct 07 00:00:00 EDT 2015}
}
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https://doi.org/10.1038/ncomms9311
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Biomimetic Hydrogen Evolution:  MoS 2 Nanoparticles as Catalyst for Hydrogen Evolution
journal, April 2005

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journal, June 2006

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Enhanced Hydrogen Evolution Catalysis from Chemically Exfoliated Metallic MoS 2 Nanosheets
journal, May 2013

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journal, March 2013

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journal, December 2011

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journal, February 2013

  • Kong, Desheng; Wang, Haotian; Cha, Judy J.
  • Nano Letters, Vol. 13, Issue 3, p. 1341-1347
  • DOI: 10.1021/nl400258t

Low-Temperature Solution Processing of Graphene−Carbon Nanotube Hybrid Materials for High-Performance Transparent Conductors
journal, May 2009

  • Tung, Vincent C.; Chen, Li-Min; Allen, Matthew J.
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Atomic Structure of Reduced Graphene Oxide
journal, April 2010

  • Gómez-Navarro, Cristina; Meyer, Jannik C.; Sundaram, Ravi S.
  • Nano Letters, Vol. 10, Issue 4
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Coherent Atomic and Electronic Heterostructures of Single-Layer MoS2
journal, July 2012

  • Eda, Goki; Fujita, Takeshi; Yamaguchi, Hisato
  • ACS Nano, Vol. 6, Issue 8, p. 7311-7317
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Biological Interactions of Graphene-Family Nanomaterials: An Interdisciplinary Review
journal, October 2011

  • Sanchez, Vanesa C.; Jachak, Ashish; Hurt, Robert H.
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Building an appropriate active-site motif into a hydrogen-evolution catalyst with thiomolybdate [Mo3S13]2− clusters
journal, January 2014

  • Kibsgaard, Jakob; Jaramillo, Thomas F.; Besenbacher, Flemming
  • Nature Chemistry, Vol. 6, Issue 3
  • DOI: 10.1038/nchem.1853

Robust carbon dioxide reduction on molybdenum disulphide edges
journal, July 2014

  • Asadi, Mohammad; Kumar, Bijandra; Behranginia, Amirhossein
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5470

Engineering the surface structure of MoS2 to preferentially expose active edge sites for electrocatalysis
journal, October 2012

  • Kibsgaard, Jakob; Chen, Zhebo; Reinecke, Benjamin N.
  • Nature Materials, Vol. 11, Issue 11, p. 963-969
  • DOI: 10.1038/nmat3439

High-throughput solution processing of large-scale graphene
journal, November 2008

  • Tung, Vincent C.; Allen, Matthew J.; Yang, Yang
  • Nature Nanotechnology, Vol. 4, Issue 1
  • DOI: 10.1038/nnano.2008.329

Powering the planet: Chemical challenges in solar energy utilization
journal, October 2006

  • Lewis, N. S.; Nocera, D. G.
  • Proceedings of the National Academy of Sciences, Vol. 103, Issue 43, p. 15729-15735
  • DOI: 10.1073/pnas.0603395103

Sustainable Hydrogen Production
journal, August 2004

Identification of Active Edge Sites for Electrochemical H2 Evolution from MoS2 Nanocatalysts
journal, July 2007

  • Jaramillo, T. F.; Jorgensen, K. P.; Bonde, J.
  • Science, Vol. 317, Issue 5834, p. 100-102
  • DOI: 10.1126/science.1141483

Structural destabilization induced by lithium intercalation in MoS 2 and related compounds
journal, January 1983

  • Py, M. A.; Haering, R. R.
  • Canadian Journal of Physics, Vol. 61, Issue 1
  • DOI: 10.1139/p83-013
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    • Zhang, Xiao; Lai, Zhuangchai; Tan, Chaoliang
    • Angewandte Chemie International Edition, Vol. 55, Issue 31
    • DOI: 10.1002/anie.201509933

    Structure Re-determination and Superconductivity Observation of Bulk 1T MoS 2
    journal, January 2018

    • Fang, Yuqiang; Pan, Jie; He, Jianqiao
    • Angewandte Chemie International Edition, Vol. 57, Issue 5
    • DOI: 10.1002/anie.201710512

    Strong Charge Transfer at 2H–1T Phase Boundary of MoS 2 for Superb High‐Performance Energy Storage
    journal, April 2019

    Wafer‐Scale and Low‐Temperature Growth of 1T‐WS 2 Film for Efficient and Stable Hydrogen Evolution Reaction
    journal, January 2020

    Recent progress in MoS2 for solar energy conversion applications
    journal, May 2019

    High-metallic-phase-concentration Mo1–xWxS2 nanosheets with expanded interlayers as efficient electrocatalysts
    journal, February 2018

    Interface confined hydrogen evolution reaction in zero valent metal nanoparticles-intercalated molybdenum disulfide
    journal, February 2017

    • Chen, Zhongxin; Leng, Kai; Zhao, Xiaoxu
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms14548

    High phase-purity 1T′-MoS2- and 1T′-MoSe2-layered crystals
    journal, April 2018

    Stable and scalable 1T MoS2 with low temperature-coefficient of resistance
    journal, August 2018

    Phase engineering of a multiphasic 1T/2H MoS 2 catalyst for highly efficient hydrogen evolution
    journal, January 2017

    • Wang, Dezhi; Zhang, Xiangyong; Bao, Siyuan
    • Journal of Materials Chemistry A, Vol. 5, Issue 6
    • DOI: 10.1039/c6ta09409k

    Direct deposition of MoSe 2 nanocrystals onto conducting substrates: towards ultra-efficient electrocatalysts for hydrogen evolution
    journal, January 2017

    • Damien, Dijo; Anil, Athira; Chatterjee, Dipanwita
    • Journal of Materials Chemistry A, Vol. 5, Issue 26
    • DOI: 10.1039/c6ta09645j

    Observation of superconductivity in 1T′-MoS 2 nanosheets
    journal, January 2017

    • Guo, Chenguang; Pan, Jie; Li, Hui
    • J. Mater. Chem. C, Vol. 5, Issue 41
    • DOI: 10.1039/c7tc03749j

    A new phase of the two-dimensional ReS 2 sheet with tunable magnetism
    journal, January 2018

    • Sun, Zhongti; Lv, Haifeng; Zhuo, Zhiwen
    • Journal of Materials Chemistry C, Vol. 6, Issue 5
    • DOI: 10.1039/c7tc05303g

    Novel structured transition metal dichalcogenide nanosheets
    journal, January 2018

    • Zhang, Xiao; Lai, Zhuangchai; Ma, Qinglang
    • Chemical Society Reviews, Vol. 47, Issue 9
    • DOI: 10.1039/c8cs00094h

    Stable 1T-phase MoS 2 as an effective electron mediator promoting photocatalytic hydrogen production
    journal, January 2018

    • Shi, Jian-Wen; Zou, Yajun; Ma, Dandan
    • Nanoscale, Vol. 10, Issue 19
    • DOI: 10.1039/c8nr00017d

    Oxygen incorporated WS 2 nanoclusters with superior electrocatalytic properties for hydrogen evolution reaction
    journal, January 2018

    • Sarma, Prasad V.; Tiwary, Chandra Sekhar; Radhakrishnan, Sruthi
    • Nanoscale, Vol. 10, Issue 20
    • DOI: 10.1039/c8nr00253c

    Nitrogen-rich 1T′-MoS 2 layered nanostructures using alkyl amines for high catalytic performance toward hydrogen evolution
    journal, January 2018

    • Kwak, In Hye; Kwon, Ik Seon; Abbas, Hafiz Ghulam
    • Nanoscale, Vol. 10, Issue 30
    • DOI: 10.1039/c8nr03661f

    Simultaneous edge and electronic control of MoS 2 nanosheets through Fe doping for an efficient oxygen evolution reaction
    journal, January 2018

    • Tang, Baoshan; Yu, Zhi Gen; Seng, Hwee Leng
    • Nanoscale, Vol. 10, Issue 43
    • DOI: 10.1039/c8nr06659k

    Two dimensional MoS 2 meets porphyrins via intercalation to enhance the electrocatalytic activity toward hydrogen evolution
    journal, January 2019

    • Kwon, Ik Seon; Kwak, In Hye; Abbas, Hafiz Ghulam
    • Nanoscale, Vol. 11, Issue 9
    • DOI: 10.1039/c8nr10165e

    Identifying the high activity of the basal plane in 1T′-phase MoS 2 towards electrochemical hydrogen evolution
    journal, January 2018

    • Shi, Yanmei; Zhang, Bin
    • Inorganic Chemistry Frontiers, Vol. 5, Issue 7
    • DOI: 10.1039/c8qi00317c

    Dynamic tungsten diselenide nanomaterials: supramolecular assembly-induced structural transition over exfoliated two-dimensional nanosheets
    journal, January 2018

    • Muhabie, Adem Ali; Ho, Ching-Hwa; Gebeyehu, Belete Tewabe
    • Chemical Science, Vol. 9, Issue 24
    • DOI: 10.1039/c8sc01778f

    Stable methylammonium-intercalated 1T′-MoS 2 for efficient electrocatalytic hydrogen evolution
    journal, January 2018

    • Kwak, In Hye; Kwon, Ik Seon; Abbas, Hafiz Ghulam
    • Journal of Materials Chemistry A, Vol. 6, Issue 14
    • DOI: 10.1039/c8ta00700d

    Intercalated complexes of 1T′-MoS 2 nanosheets with alkylated phenylenediamines as excellent catalysts for electrochemical hydrogen evolution
    journal, January 2019

    • Kwak, In Hye; Kwon, Ik Seon; Abbas, Hafiz Ghulam
    • Journal of Materials Chemistry A, Vol. 7, Issue 5
    • DOI: 10.1039/c8ta11085a

    Superhydrophobic states of 2D nanomaterials controlled by atomic defects can modulate cell adhesion
    journal, January 2019

    • Jaiswal, Manish K.; Singh, Kanwar Abhay; Lokhande, Giriraj
    • Chemical Communications, Vol. 55, Issue 60
    • DOI: 10.1039/c9cc00547a

    Enhancing the electrocatalytic activity of 2H-WS 2 for hydrogen evolution via defect engineering
    journal, January 2019

    • Wu, Longfei; van Hoof, Arno J. F.; Dzade, Nelson Y.
    • Physical Chemistry Chemical Physics, Vol. 21, Issue 11
    • DOI: 10.1039/c9cp00722a

    Ligand induced structure and property changes of 1T-MoS 2
    journal, January 2019

    • Linghu, Yaoyao; Li, Na; Du, Yaping
    • Physical Chemistry Chemical Physics, Vol. 21, Issue 18
    • DOI: 10.1039/c9cp00917e

    Two-dimensional transition metal dichalcogenides as promising anodes for potassium ion batteries from first-principles prediction
    journal, January 2019

    • Zhang, Zixiang; Yang, Mingye; Zhao, Ni
    • Physical Chemistry Chemical Physics, Vol. 21, Issue 42
    • DOI: 10.1039/c9cp03948a

    Recent progress of TMD nanomaterials: phase transitions and applications
    journal, January 2020

    • Huang, H. H.; Fan, Xiaofeng; Singh, David J.
    • Nanoscale, Vol. 12, Issue 3
    • DOI: 10.1039/c9nr08313h

    Metal–organic framework-derived hierarchical MoS 2 /CoS 2 nanotube arrays as pH-universal electrocatalysts for efficient hydrogen evolution
    journal, January 2019

    • Tang, Baoshan; Yu, Zhi Gen; Zhang, Yaoxin
    • Journal of Materials Chemistry A, Vol. 7, Issue 21
    • DOI: 10.1039/c9ta00545e

    A highly efficient alkaline HER Co–Mo bimetallic carbide catalyst with an optimized Mo d-orbital electronic state
    journal, January 2019

    • Liu, Gejun; Bai, Haipeng; Ji, Yujin
    • Journal of Materials Chemistry A, Vol. 7, Issue 20
    • DOI: 10.1039/c9ta02886b

    C 3 N 4 -digested 3D construction of hierarchical metallic phase MoS 2 nanostructures
    journal, January 2019

    • Wang, Jiayu; Tang, Jing; Guo, Tong
    • Journal of Materials Chemistry A, Vol. 7, Issue 31
    • DOI: 10.1039/c9ta06115k

    Two-dimensional MoS 2 –melamine hybrid nanostructures for enhanced catalytic hydrogen evolution reaction
    journal, January 2019

    • Kwak, In Hye; Kwon, Ik Seon; Debela, Tekalign Terfa
    • Journal of Materials Chemistry A, Vol. 7, Issue 39
    • DOI: 10.1039/c9ta07802a

    A phosphorene-like InP 3 monolayer: structure, stability, and catalytic properties toward the hydrogen evolution reaction
    journal, January 2020

    • Jalil, Abdul; Zhuo, Zhiwen; Sun, Zhongti
    • Journal of Materials Chemistry A, Vol. 8, Issue 3
    • DOI: 10.1039/c9ta08612a

    Proximity exchange induced gap opening and topological feature in graphene/1T′-MX 2 (M  =  Mo,W; X  =  S,Se,Te) Dirac heterostructures
    journal, June 2018

    • Song, Changsheng; Xiao, Wen; Lin, Ping
    • Journal of Physics: Condensed Matter, Vol. 30, Issue 27
    • DOI: 10.1088/1361-648x/aac7f8

    Structural stability of coplanar 1T-2H superlattice MoS 2 under high energy electron beam
    journal, March 2018

    Structural phase transition barrier of N-doped MoS 2 with charge injection
    journal, October 2018

    Phase Engineering from 2H to 1T-MoS 2 for Efficient Ammonia PL Sensor and Electrocatalyst for Hydrogen Evolution Reaction
    journal, January 2019

    • Chacko, Levna; Rastogi, Pankaj Kumar; Aneesh, P. M.
    • Journal of The Electrochemical Society, Vol. 166, Issue 8
    • DOI: 10.1149/2.0071908jes

    Sulfur‐Mastery: Precise Synthesis of 2D Transition Metal Dichalcogenides
    journal, May 2019

    Unraveling High‐Yield Phase‐Transition Dynamics in Transition Metal Dichalcogenides on Metallic Substrates
    journal, January 2019

    Engineering MoS 2 Basal Planes for Hydrogen Evolution via Synergistic Ruthenium Doping and Nanocarbon Hybridization
    journal, March 2019

    2DMatPedia, an open computational database of two-dimensional materials from top-down and bottom-up approaches
    journal, June 2019

    A vacancy-driven phase transition in MoX 2 (X: S, Se and Te) nanoscrolls
    journal, January 2018

    • Hwang, Da Young; Choi, Kyoung Hwan; Suh, Dong Hack
    • Nanoscale, Vol. 10, Issue 17
    • DOI: 10.1039/c7nr08634b

    High-quality single-layer nanosheets of MS 2 (M = Mo, Nb, Ta, Ti) directly exfoliated from AMS 2 (A = Li, Na, K) crystals
    journal, January 2017

    • Guo, Chenguang; Li, Hui; Zhao, Wei
    • Journal of Materials Chemistry C, Vol. 5, Issue 24
    • DOI: 10.1039/c7tc00838d

    Intercalation of aromatic amine for the 2H–1T′ phase transition of MoS 2 by experiments and calculations
    journal, January 2018

    • Kwon, Ik Seon; Kwak, In Hye; Abbas, Hafiz Ghulam
    • Nanoscale, Vol. 10, Issue 24
    • DOI: 10.1039/c8nr02365d

    Tuning the catalytic activity of heterogeneous two-dimensional transition metal dichalcogenides for hydrogen evolution
    journal, January 2018

    • Noh, Seung Hyo; Hwang, Jeemin; Kang, Joonhee
    • Journal of Materials Chemistry A, Vol. 6, Issue 41
    • DOI: 10.1039/c8ta07141a

    Tuning the phase stability of Mo-based TMD monolayers through coupled vacancy defects and lattice strain
    journal, January 2018

    Revealing the role of the 1T phase on the adsorption of organic dyes on MoS 2 nanosheets
    journal, January 2019

    • Omar, Asmaa M.; Metwalli, Ossama I.; Saber, Mohamed R.
    • RSC Advances, Vol. 9, Issue 49
    • DOI: 10.1039/c9ra05427h

    Reversible H-T′ phase transition in monolayer molybdenum disulfide via electron beam assisted solid state lithiation/delithiation
    journal, January 2020

    • Ji, Xujing; Wu, Chunyang; Deng, Jingfei
    • Applied Physics Letters, Vol. 116, Issue 3
    • DOI: 10.1063/1.5125312

    Superconductivity in the metastable 1 T ′ and 1 T ′ ″ phases of Mo S 2 crystals
    journal, November 2018

    Rhenium-Doped and Stabilized MoS 2 Atomic Layers with Basal-Plane Catalytic Activity
    journal, October 2018

    • Yang, Shi-Ze; Gong, Yongji; Manchanda, Priyanka
    • Advanced Materials, Vol. 30, Issue 51
    • DOI: 10.1002/adma.201803477

    Large thermoelectric power factor of high-mobility transition-metal dichalcogenides with 1 T ″ phase
    journal, February 2020

    Unraveling the Role of Lithium in Enhancing the Hydrogen Evolution Activity of MoS2: Intercalation versus Adsorption
    journal, June 2019

    Effect of Structural Phases on Mechanical Properties of Molybdenum Disulfide
    journal, March 2020

    Interface confined hydrogen evolution reaction in zero valent metal nanoparticles-intercalated molybdenum disulfide
    journal, February 2017

    • Chen, Zhongxin; Leng, Kai; Zhao, Xiaoxu
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms14548

    2DMatPedia, an open computational database of two-dimensional materials from top-down and bottom-up approaches
    journal, June 2019

    Stable and scalable 1T MoS2 with low temperature-coefficient of resistance
    journal, August 2018

    Pyrene Coating Transition Metal Disulfides as Protection from Photooxidation and Environmental Aging
    journal, February 2020

    • Canton-Vitoria, Ruben; Sayed-Ahmad-Baraza, Yuman; Humbert, Bernard
    • Nanomaterials, Vol. 10, Issue 2
    • DOI: 10.3390/nano10020363
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