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Title: Crystallinity Dependence of Ruthenium Nanocatalyst toward Hydrogen Evolution Reaction

Abstract

The development of highly active and durable inexpensive electrocatalysts for hydrogen evolution reaction (HER) is still a formidable challenge. Herein, an ordered hexagonal-closed-packed (hcp)-Ru nanocrystal coated with a thin layer of N-doped carbon (hcp-Ru@NC) was fabricated through the thermal annealing of polydopamine (PDA)-coated Ru nanoparticle (RuNP@PDA). As an alternative to Pt/C catalyst, the hcp-Ru@NC nanocatalyst exhibited the small overpotential of 27.5 mV at a current density of 10 mA cm –2, as well as long-term stability for HER in acid media. Interestingly, the HER performance of hcp-Ru is highly dependent on its crystallinity. The calculation from density functional theory (DFT) revealed that the difference in HER activity over various exposed surface causes the crystallinity-dependent property of hcp-Ru. The results of this study provided clues to guide the design of Ru-based inexpensive HER electrocatalyst.

Authors:
 [1];  [2]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1];  [1]; ORCiD logo [3];  [2]; ORCiD logo [2]
  1. Changzhou Univ., Changzhou, Jiangsu (China). School of Petrochemical Engineering, Jiangsu Key Lab. of Advanced Materials and Technology
  2. Georgia Inst. of Technology, Atlanta, GA (United States). School of Materials Science and Engineering
  3. Nanjing Univ. of Information & Technology, Nanjing, Jiangsu (China). School of Environmental Science and Engineering
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of California, Oakland, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1543701
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 8; Journal Issue: 7; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; chemistry; Ruthenium nanocatalyst; crystallinity-dependence; hydrogen evolution reaction; N-doped graphene; electrocatalyst

Citation Formats

Li, Yutong, Zhang, Lei A., Qin, Yong, Chu, Fuqiang, Kong, Yong, Tao, Yongxin, Li, Yongxin, Bu, Yunfei, Ding, Dong, and Liu, Meilin. Crystallinity Dependence of Ruthenium Nanocatalyst toward Hydrogen Evolution Reaction. United States: N. p., 2018. Web. doi:10.1021/acscatal.8b01609.
Li, Yutong, Zhang, Lei A., Qin, Yong, Chu, Fuqiang, Kong, Yong, Tao, Yongxin, Li, Yongxin, Bu, Yunfei, Ding, Dong, & Liu, Meilin. Crystallinity Dependence of Ruthenium Nanocatalyst toward Hydrogen Evolution Reaction. United States. doi:10.1021/acscatal.8b01609.
Li, Yutong, Zhang, Lei A., Qin, Yong, Chu, Fuqiang, Kong, Yong, Tao, Yongxin, Li, Yongxin, Bu, Yunfei, Ding, Dong, and Liu, Meilin. Tue . "Crystallinity Dependence of Ruthenium Nanocatalyst toward Hydrogen Evolution Reaction". United States. doi:10.1021/acscatal.8b01609. https://www.osti.gov/servlets/purl/1543701.
@article{osti_1543701,
title = {Crystallinity Dependence of Ruthenium Nanocatalyst toward Hydrogen Evolution Reaction},
author = {Li, Yutong and Zhang, Lei A. and Qin, Yong and Chu, Fuqiang and Kong, Yong and Tao, Yongxin and Li, Yongxin and Bu, Yunfei and Ding, Dong and Liu, Meilin},
abstractNote = {The development of highly active and durable inexpensive electrocatalysts for hydrogen evolution reaction (HER) is still a formidable challenge. Herein, an ordered hexagonal-closed-packed (hcp)-Ru nanocrystal coated with a thin layer of N-doped carbon (hcp-Ru@NC) was fabricated through the thermal annealing of polydopamine (PDA)-coated Ru nanoparticle (RuNP@PDA). As an alternative to Pt/C catalyst, the hcp-Ru@NC nanocatalyst exhibited the small overpotential of 27.5 mV at a current density of 10 mA cm–2, as well as long-term stability for HER in acid media. Interestingly, the HER performance of hcp-Ru is highly dependent on its crystallinity. The calculation from density functional theory (DFT) revealed that the difference in HER activity over various exposed surface causes the crystallinity-dependent property of hcp-Ru. The results of this study provided clues to guide the design of Ru-based inexpensive HER electrocatalyst.},
doi = {10.1021/acscatal.8b01609},
journal = {ACS Catalysis},
number = 7,
volume = 8,
place = {United States},
year = {2018},
month = {5}
}

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Cited by: 22 works
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Figures / Tables:

Scheme 1 Scheme 1: Illustration of the fabricating process of hcp-Ru@NC on NG.

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Works referencing / citing this record:

Controllable fabrication of uniform ruthenium phosphide nanocrystals for the hydrogen evolution reaction
journal, January 2019

  • Li, Yutong; Chu, Fuqiang; Bu, Yunfei
  • Chemical Communications, Vol. 55, Issue 54
  • DOI: 10.1039/c9cc03668g

    Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.