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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]
  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 Lab. (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. https://doi.org/10.1038/ncomms11857.
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
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.
@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 = {2016},
month = {6}
}

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