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Title: Integrating Rh Species with NiFe-Layered Double Hydroxide for Overall Water Splitting

Abstract

NiFe-layered double hydroxide (LDH) is thought of as a promising bifunctional water-splitting catalyst, owing to its excellent performances for alkaline oxygen evolution reactions (OERs). However, it shows extremely poor activity toward hydrogen evolution reactions (HERs) due to the weak hydrogen adsorption. We demonstrated that the integration of Rh species and NiFe-LDH can dramatically improve its HER kinetics without sacrificing the OER performance. The Rh species were initially integrated into NiFe-LDH as oxidized dopants and metallic clusters (< 1 nm). In 1 M KOH electrolyte, an overpotential of 58 mV is needed to catalyze 10 mA cm–2 HER current density. Furthermore, this catalyst only requires 1.46 V to drive an electrolyzer at 10 mA cm–2. A strong interaction between metallic Rh clusters and NiFe hydroxide during the HER process is revealed. The theoretical calculation shows the Rh ions replace Fe ions as the major active sites that are responsible for OERs.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3];  [4];  [5];  [5];  [3];  [3];  [6];  [5]; ORCiD logo [7]; ORCiD logo [6]; ORCiD logo [6]; ORCiD logo [3]; ORCiD logo [2]
  1. Yale Univ., New Haven, CT (United States); Iowa State Univ., Ames, IA (United States)
  2. Univ. of Pennsylvania, Philadelphia, PA (United States)
  3. Yale Univ., New Haven, CT (United States)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  5. Ames Lab., Ames, IA (United States)
  6. Iowa State Univ., Ames, IA (United States)
  7. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1603279
Report Number(s):
BNL-213650-2020-JAAM
Journal ID: ISSN 1530-6984
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 20; Journal Issue: 1; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Transition metal hydroxides; electrolysis; metallic clusters; interaction; nanostructures

Citation Formats

Zhang, Bowei, Zhu, Chongqin, Wu, Zishan, Stavitski, Eli, Lui, Yu Hui, Kim, Tae-Hoon, Liu, Huan, Huang, Ling, Luan, Xuechen, Zhou, Lin, Jiang, Kun, Huang, Wenyu, Hu, Shan, Wang, Hailiang, and Francisco, Joseph S. Integrating Rh Species with NiFe-Layered Double Hydroxide for Overall Water Splitting. United States: N. p., 2019. Web. https://doi.org/10.1021/acs.nanolett.9b03460.
Zhang, Bowei, Zhu, Chongqin, Wu, Zishan, Stavitski, Eli, Lui, Yu Hui, Kim, Tae-Hoon, Liu, Huan, Huang, Ling, Luan, Xuechen, Zhou, Lin, Jiang, Kun, Huang, Wenyu, Hu, Shan, Wang, Hailiang, & Francisco, Joseph S. Integrating Rh Species with NiFe-Layered Double Hydroxide for Overall Water Splitting. United States. https://doi.org/10.1021/acs.nanolett.9b03460
Zhang, Bowei, Zhu, Chongqin, Wu, Zishan, Stavitski, Eli, Lui, Yu Hui, Kim, Tae-Hoon, Liu, Huan, Huang, Ling, Luan, Xuechen, Zhou, Lin, Jiang, Kun, Huang, Wenyu, Hu, Shan, Wang, Hailiang, and Francisco, Joseph S. Wed . "Integrating Rh Species with NiFe-Layered Double Hydroxide for Overall Water Splitting". United States. https://doi.org/10.1021/acs.nanolett.9b03460. https://www.osti.gov/servlets/purl/1603279.
@article{osti_1603279,
title = {Integrating Rh Species with NiFe-Layered Double Hydroxide for Overall Water Splitting},
author = {Zhang, Bowei and Zhu, Chongqin and Wu, Zishan and Stavitski, Eli and Lui, Yu Hui and Kim, Tae-Hoon and Liu, Huan and Huang, Ling and Luan, Xuechen and Zhou, Lin and Jiang, Kun and Huang, Wenyu and Hu, Shan and Wang, Hailiang and Francisco, Joseph S.},
abstractNote = {NiFe-layered double hydroxide (LDH) is thought of as a promising bifunctional water-splitting catalyst, owing to its excellent performances for alkaline oxygen evolution reactions (OERs). However, it shows extremely poor activity toward hydrogen evolution reactions (HERs) due to the weak hydrogen adsorption. We demonstrated that the integration of Rh species and NiFe-LDH can dramatically improve its HER kinetics without sacrificing the OER performance. The Rh species were initially integrated into NiFe-LDH as oxidized dopants and metallic clusters (< 1 nm). In 1 M KOH electrolyte, an overpotential of 58 mV is needed to catalyze 10 mA cm–2 HER current density. Furthermore, this catalyst only requires 1.46 V to drive an electrolyzer at 10 mA cm–2. A strong interaction between metallic Rh clusters and NiFe hydroxide during the HER process is revealed. The theoretical calculation shows the Rh ions replace Fe ions as the major active sites that are responsible for OERs.},
doi = {10.1021/acs.nanolett.9b03460},
journal = {Nano Letters},
number = 1,
volume = 20,
place = {United States},
year = {2019},
month = {11}
}

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