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Title: Efficient hydrogen evolution in transition metal dichalcogenides via a simple one-step hydrazine reaction

Abstract

In this study, hydrogen evolution reaction is catalyzed efficiently with precious metals, such as platinum; however, transition metal dichalcogenides have recently emerged as a promising class of materials for electrocatalysis, but these materials still have low activity and durability when compared with precious metals. Here we report a simple one-step scalable approach, where MoOx/MoS2 core-shell nanowires and molybdenum disulfide sheets are exposed to dilute aqueous hydrazine at room temperature, which results in marked improvement in electrocatalytic performance. The nanowires exhibit ~100 mV improvement in over potential following exposure to dilute hydrazine, while also showing a 10-fold increase in current density and a significant change in Tafel slope. In situ electrical, gate-dependent measurements and spectroscopic investigations reveal that hydrazine acts as an electron dopant in molybdenum disulfide, increasing its conductivity, while also reducing the MoOx core in the core-shell nanowires, which leads to improved electrocatalytic performance.

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [3];  [2];  [3];  [5];  [6];  [5];  [7];  [3];  [2];  [3];  [2]
+ Show Author Affiliations
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Louisville, Louisville, KY (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. Univ. of Louisville, Louisville, KY (United States)
  4. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Rutgers Univ., Piscataway, NJ (United States)
  5. Rice Univ., Houston, TX (United States)
  6. Pittsburg State Univ., Pittsburg, KS (United States)
  7. Rutgers Univ., Piscataway, NJ (United States)
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1341863
Report Number(s):
LA-UR-16-23488
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; energy sciences; inorganic and physical chemistry; material science; electrocatalysis; nanowires; reaction mechanisms

Citation Formats

Cummins, Dustin R., Martinez, Ulises, Sherehiy, Andriy, Kappera, Rajesh, Martinez-Garcia, Alejandro, Schulze, Roland K., Jasinski, Jacek, Zhang, Jing, Gupta, Ram K., Lou, Jun, Chhowalla, Manish, Sumanasekera, Gamini, Mohite, Aditya D., Sunkara, Mahendra K., and Gupta, Gautam. Efficient hydrogen evolution in transition metal dichalcogenides via a simple one-step hydrazine reaction. United States: N. p., 2016. Web. doi:10.1038/ncomms11857.
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Cummins, Dustin R., Martinez, Ulises, Sherehiy, Andriy, Kappera, Rajesh, Martinez-Garcia, Alejandro, Schulze, Roland K., Jasinski, Jacek, Zhang, Jing, Gupta, Ram K., Lou, Jun, Chhowalla, Manish, Sumanasekera, Gamini, Mohite, Aditya D., Sunkara, Mahendra K., & Gupta, Gautam. Efficient hydrogen evolution in transition metal dichalcogenides via a simple one-step hydrazine reaction. United States. https://doi.org/10.1038/ncomms11857
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Cummins, Dustin R., Martinez, Ulises, Sherehiy, Andriy, Kappera, Rajesh, Martinez-Garcia, Alejandro, Schulze, Roland K., Jasinski, Jacek, Zhang, Jing, Gupta, Ram K., Lou, Jun, Chhowalla, Manish, Sumanasekera, Gamini, Mohite, Aditya D., Sunkara, Mahendra K., and Gupta, Gautam. Fri . "Efficient hydrogen evolution in transition metal dichalcogenides via a simple one-step hydrazine reaction". United States. https://doi.org/10.1038/ncomms11857. https://www.osti.gov/servlets/purl/1341863.
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@article{osti_1341863,
title = {Efficient hydrogen evolution in transition metal dichalcogenides via a simple one-step hydrazine reaction},
author = {Cummins, Dustin R. and Martinez, Ulises and Sherehiy, Andriy and Kappera, Rajesh and Martinez-Garcia, Alejandro and Schulze, Roland K. and Jasinski, Jacek and Zhang, Jing and Gupta, Ram K. and Lou, Jun and Chhowalla, Manish and Sumanasekera, Gamini and Mohite, Aditya D. and Sunkara, Mahendra K. and Gupta, Gautam},
abstractNote = {In this study, hydrogen evolution reaction is catalyzed efficiently with precious metals, such as platinum; however, transition metal dichalcogenides have recently emerged as a promising class of materials for electrocatalysis, but these materials still have low activity and durability when compared with precious metals. Here we report a simple one-step scalable approach, where MoOx/MoS2 core-shell nanowires and molybdenum disulfide sheets are exposed to dilute aqueous hydrazine at room temperature, which results in marked improvement in electrocatalytic performance. The nanowires exhibit ~100 mV improvement in over potential following exposure to dilute hydrazine, while also showing a 10-fold increase in current density and a significant change in Tafel slope. In situ electrical, gate-dependent measurements and spectroscopic investigations reveal that hydrazine acts as an electron dopant in molybdenum disulfide, increasing its conductivity, while also reducing the MoOx core in the core-shell nanowires, which leads to improved electrocatalytic performance.},
doi = {10.1038/ncomms11857},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {Fri Jun 10 00:00:00 EDT 2016},
month = {Fri Jun 10 00:00:00 EDT 2016}
}
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https://doi.org/10.1038/ncomms11857
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Phase-engineered low-resistance contacts for ultrathin MoS2 transistors
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Large-area ultrathin films of reduced graphene oxide as a transparent and flexible electronic material
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Electrochemical tuning of vertically aligned MoS2 nanofilms and its application in improving hydrogen evolution reaction
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The dissociation energy of the N-N bond in hydrazine
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PbSe Nanocrystal Solids for n- and p-Channel Thin Film Field-Effect Transistors
journal, October 2005

Two-Dimensional Nanosheets Produced by Liquid Exfoliation of Layered Materials
journal, February 2011

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    • DOI: 10.1039/c8ta06029k

    Energy-Saving Electrolytic Hydrogen Generation: Ni 2 P Nanoarray as a High-Performance Non-Noble-Metal Electrocatalyst
    journal, December 2016

    A bimetallic oxide Fe 1.89 Mo 4.11 O 7 electrocatalyst with highly efficient hydrogen evolution reaction activity in alkaline and acidic media
    journal, January 2018

    • Hao, Zhaomin; Yang, Shishuai; Niu, Jingyang
    • Chemical Science, Vol. 9, Issue 25
    • DOI: 10.1039/c8sc01710g

    Ni–Mo–O nanorod-derived composite catalysts for efficient alkaline water-to-hydrogen conversion via urea electrolysis
    journal, January 2018

    • Yu, Zi-You; Lang, Chao-Chao; Gao, Min-Rui
    • Energy & Environmental Science, Vol. 11, Issue 7
    • DOI: 10.1039/c8ee00521d

    Unveiling the Interfacial Effects for Enhanced Hydrogen Evolution Reaction on MoS 2 /WTe 2 Hybrid Structures
    journal, April 2019

    Modulating the Volmer Step by MOF Derivatives Assembled with Heterogeneous Ni 2 P-CoP Nanocrystals in Alkaline Hydrogen Evolution Reaction
    journal, January 2018

    • Liang, Da; Jiang, Hao; Xu, Qiucheng
    • Journal of The Electrochemical Society, Vol. 165, Issue 16
    • DOI: 10.1149/2.0131816jes

    Large-area MoS 2 -MoO x heterojunction thin-film photodetectors with wide spectral range and enhanced photoresponse
    journal, June 2019

    • Im, Healin; Liu, Na; Bala, Arindam
    • APL Materials, Vol. 7, Issue 6
    • DOI: 10.1063/1.5094586

    Efficient Hydrogen Production on a 3D Flexible Heterojunction Material
    journal, April 2018

    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

    Activating the MoS 2 Basal Plane by Controllable Fabrication of Pores for an Enhanced Hydrogen Evolution Reaction
    journal, November 2018

    • Geng, Shuo; Liu, Hu; Yang, Weiwei
    • Chemistry - A European Journal, Vol. 24, Issue 71
    • DOI: 10.1002/chem.201804658

    Boron‐Induced Electronic‐Structure Reformation of CoP Nanoparticles Drives Enhanced pH‐Universal Hydrogen Evolution
    journal, January 2020

    Oxygen Doping to Optimize Atomic Hydrogen Binding Energy on NiCoP for Highly Efficient Hydrogen Evolution
    journal, April 2018

    The development of 2D materials for electrochemical energy applications: A mechanistic approach
    journal, March 2019

    • Hynek, David J.; Pondick, Joshua V.; Cha, Judy J.
    • APL Materials, Vol. 7, Issue 3
    • DOI: 10.1063/1.5085187

    Hydrogen adsorption engineering by intramolecular proton transfer on 2D nanosheets
    journal, May 2018

    An overview on Pd-based electrocatalysts for the hydrogen evolution reaction
    journal, January 2018

    • Sarkar, Shreya; Peter, Sebastian C.
    • Inorganic Chemistry Frontiers, Vol. 5, Issue 9
    • DOI: 10.1039/c8qi00042e

    Kinetic‐Oriented Construction of MoS 2 Synergistic Interface to Boost pH‐Universal Hydrogen Evolution
    journal, December 2019

    • Hu, Jue; Zhang, Chengxu; Yang, Peng
    • Advanced Functional Materials, Vol. 30, Issue 6
    • DOI: 10.1002/adfm.201908520

    Tungsten-inert gas welding electrodes as low-cost, green and pH-universal electrocatalysts for the hydrogen evolution reaction
    journal, January 2019

    • Hashemniaye-Torshizi, Reihaneh; Ashraf, Narges; Arbab-Zavar, Mohammad Hossein
    • New Journal of Chemistry, Vol. 43, Issue 29
    • DOI: 10.1039/c9nj02298h

    Controlled Growth of MoS 2 Nanosheets on 2D N‐Doped Graphdiyne Nanolayers for Highly Associated Effects on Water Reduction
    journal, March 2018

    • Yu, Huidi; Xue, Yurui; Hui, Lan
    • Advanced Functional Materials, Vol. 28, Issue 19
    • DOI: 10.1002/adfm.201707564

    Electron density modulation of NiCo2S4 nanowires by nitrogen incorporation for highly efficient hydrogen evolution catalysis
    journal, April 2018

    Surface states in bulk single crystal of topological semimetal Co 3 Sn 2 S 2 toward water oxidation
    journal, August 2019

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