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Title: 3D Printed Nickel–Molybdenum-Based Electrocatalysts for Hydrogen Evolution at Low Overpotentials in a Flow-Through Configuration

Abstract

Three-dimensional (3D) printed, hierarchically porous nickel molybdenum (NiMo) electrocatalysts were synthesized and evaluated in a flow-through configuration for the hydrogen evolution reaction (HER) in 1.0 M KOH(aq) in a simple electrochemical H-cell. 3D NiMo electrodes possess hierarchically porous structures because of the resol-based aerogel precursor, which generates superporous carbon aerogel as a catalyst support. Relative to a traditional planar electrode configuration, the flow-through configuration allowed efficient removal of the hydrogen bubbles from the catalyst surface, especially at high operating current densities, and significantly decreased the overpotentials required for HER. An analytical model that accounted for the electrokinetics of HER as well as the mass transport with or without the flow-through configuration was developed to quantitatively evaluate voltage losses associated with kinetic overpotentials and ohmic resistance due to bubble formation in the porous electrodes. Furthermore, the chemical composition, electrochemical surface area (ECSA), and roughness factor (RF) were also systematically studied to assess the electrocatalytic performance of the 3D printed, hierarchically porous NiMo electrodes. An ECSA of 25163 cm2 was obtained with the highly porous structures, and an average overpotential of 45 mV at 10 mA cm–2 was achieved over 24 h by using the flow-through configuration. The flow-through configuration evaluated inmore » the simple H-cell achieved high electrochemical accessible surface areas for electrochemical reactions and provided useful information for adaption of the porous electrodes in flow cells.« less

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3];  [3];  [3];  [3];  [3];  [3]; ORCiD logo [2];  [3];  [3]; ORCiD logo [1]
+ Show Author Affiliations
  1. California Institute of Technology (CalTech), Pasadena, CA (United States). Liquid Sunlight Alliance (LiSA)
  2. Southern Univ. of Science and Technology, Shenzhen (China)
  3. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1810667
Report Number(s):
LLNL-JRNL-816169
Journal ID: ISSN 1944-8244; 1025498
Grant/Contract Number:  
AC52-07NA27344; SC0021266
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 13; Journal Issue: 17; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; hydrogen evolution reaction; electrocatalysis; 3D printing; alkaline electrolysis; NiMo; flow-through; electrochemistry; solar fuel

Citation Formats

Sullivan, Ian, Zhang, Huanlei, Zhu, Cheng, Wood, Marissa, Nelson, Art J., Baker, Sarah E., Spadaccini, Christopher M., Van Buuren, Tony, Lin, Meng, Duoss, Eric B., Liang, Siwei, and Xiang, Chengxiang. 3D Printed Nickel–Molybdenum-Based Electrocatalysts for Hydrogen Evolution at Low Overpotentials in a Flow-Through Configuration. United States: N. p., 2021. Web. doi:10.1021/acsami.1c05648.
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Sullivan, Ian, Zhang, Huanlei, Zhu, Cheng, Wood, Marissa, Nelson, Art J., Baker, Sarah E., Spadaccini, Christopher M., Van Buuren, Tony, Lin, Meng, Duoss, Eric B., Liang, Siwei, & Xiang, Chengxiang. 3D Printed Nickel–Molybdenum-Based Electrocatalysts for Hydrogen Evolution at Low Overpotentials in a Flow-Through Configuration. United States. https://doi.org/10.1021/acsami.1c05648
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Sullivan, Ian, Zhang, Huanlei, Zhu, Cheng, Wood, Marissa, Nelson, Art J., Baker, Sarah E., Spadaccini, Christopher M., Van Buuren, Tony, Lin, Meng, Duoss, Eric B., Liang, Siwei, and Xiang, Chengxiang. Thu . "3D Printed Nickel–Molybdenum-Based Electrocatalysts for Hydrogen Evolution at Low Overpotentials in a Flow-Through Configuration". United States. https://doi.org/10.1021/acsami.1c05648. https://www.osti.gov/servlets/purl/1810667.
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@article{osti_1810667,
title = {3D Printed Nickel–Molybdenum-Based Electrocatalysts for Hydrogen Evolution at Low Overpotentials in a Flow-Through Configuration},
author = {Sullivan, Ian and Zhang, Huanlei and Zhu, Cheng and Wood, Marissa and Nelson, Art J. and Baker, Sarah E. and Spadaccini, Christopher M. and Van Buuren, Tony and Lin, Meng and Duoss, Eric B. and Liang, Siwei and Xiang, Chengxiang},
abstractNote = {Three-dimensional (3D) printed, hierarchically porous nickel molybdenum (NiMo) electrocatalysts were synthesized and evaluated in a flow-through configuration for the hydrogen evolution reaction (HER) in 1.0 M KOH(aq) in a simple electrochemical H-cell. 3D NiMo electrodes possess hierarchically porous structures because of the resol-based aerogel precursor, which generates superporous carbon aerogel as a catalyst support. Relative to a traditional planar electrode configuration, the flow-through configuration allowed efficient removal of the hydrogen bubbles from the catalyst surface, especially at high operating current densities, and significantly decreased the overpotentials required for HER. An analytical model that accounted for the electrokinetics of HER as well as the mass transport with or without the flow-through configuration was developed to quantitatively evaluate voltage losses associated with kinetic overpotentials and ohmic resistance due to bubble formation in the porous electrodes. Furthermore, the chemical composition, electrochemical surface area (ECSA), and roughness factor (RF) were also systematically studied to assess the electrocatalytic performance of the 3D printed, hierarchically porous NiMo electrodes. An ECSA of 25163 cm2 was obtained with the highly porous structures, and an average overpotential of 45 mV at 10 mA cm–2 was achieved over 24 h by using the flow-through configuration. The flow-through configuration evaluated in the simple H-cell achieved high electrochemical accessible surface areas for electrochemical reactions and provided useful information for adaption of the porous electrodes in flow cells.},
doi = {10.1021/acsami.1c05648},
journal = {ACS Applied Materials and Interfaces},
number = 17,
volume = 13,
place = {United States},
year = {Thu Apr 22 00:00:00 EDT 2021},
month = {Thu Apr 22 00:00:00 EDT 2021}
}
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