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Title: Hydrogen evolution activity tuning via two-dimensional electron accumulation at buried interfaces

Abstract

Developing efficient earth-abundant transition metal-based electrocatalysts for the hydrogen evolution reaction (HER) is crucial for hydrogen production at scale. This paper reports that the buried electrocatalytic interfaces between Ni–Fe sulfide (NiFeS) nanosheets and TiO 2 conformal coatings (about 5 nm) achieved remarkable HER activity improvement, lowering the HER overpotential from –170 mV to –107 mV at –50 mA cm –2 in a base. Non-HER active, permeable TiO 2 coatings grown by atomic layer deposition (ALD) achieved continuous fine-tuning of the electronic properties at the buried TiO 2/NiFeS interfaces, as a novel strategy and the main factor for electron accumulation at the interface. Core-level and valence band X-ray photoelectron spectroscopy (XPS) was used to investigate the TiO 2 electronic-structure tuning effect on the charge-transfer energetics during the HER. Their alkaline HER mechanism was elucidated by supplementing characterizations of membrane permeation, Tafel slope, and synchrotron X-ray absorption spectroscopy, which verified that the buried TiO 2/NiFeS interfaces are electrocatalytically active. Here, this study offers a general strategy for improving the charge-transfer kinetics of an electrocatalytic system by confining catalysis at a permeable solid–solid interface. The broad applicability of permeable and tunable coatings potentially accelerates the optimization of earth-abundant catalysts to achieve high performancemore » under operationally relevant conditions.« less

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [2];  [2];  [2];  [4]; ORCiD logo [5];  [6];  [6]; ORCiD logo [4]; ORCiD logo [2]
  1. Yale Univ., New Haven, CT (United States). Dept. of Chemical and Environmental Engineering; Chinese Academy of Sciences (CAS), Beijing (China). National Engineering Lab. for Hydrometallurgical Cleaner Production Technology, CAS Key Laboratory of Green Process and Engineering, Inst. of Process Engineering; Yale Univ., West Haven, CT (United States). Energy Sciences Inst.; Univ. of Chinese Academy of Sciences, Beijing (China)
  2. Yale Univ., New Haven, CT (United States). Dept. of Chemical and Environmental Engineering; Yale Univ., West Haven, CT (United States). Energy Sciences Inst.
  3. China Univ. of Mining and Technology, Beijing (China). School of Chemical and Environmental Engineering
  4. Yale Univ., New Haven, CT (United States). Dept. of Chemical and Environmental Engineering
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
  6. Chinese Academy of Sciences (CAS), Beijing (China). National Engineering Lab. for Hydrometallurgical Cleaner Production Technology, CAS Key Laboratory of Green Process and Engineering, Inst. of Process Engineering
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1574914
Report Number(s):
BNL-212338-2019-JAAM
Journal ID: ISSN 2050-7488; JMCAET
Grant/Contract Number:  
SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 7; Journal Issue: 36; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY

Citation Formats

Xue, Yudong, Fishman, Zachary S., Wang, Yunting, Pan, Zhenhua, Shen, Xin, Yanagi, Rito, Hutchings, Gregory S., Liu, Mingzhao, Zheng, Shili, Zhang, Yi, Altman, Eric I., and Hu, Shu. Hydrogen evolution activity tuning via two-dimensional electron accumulation at buried interfaces. United States: N. p., 2019. Web. doi:10.1039/C9TA07123G.
Xue, Yudong, Fishman, Zachary S., Wang, Yunting, Pan, Zhenhua, Shen, Xin, Yanagi, Rito, Hutchings, Gregory S., Liu, Mingzhao, Zheng, Shili, Zhang, Yi, Altman, Eric I., & Hu, Shu. Hydrogen evolution activity tuning via two-dimensional electron accumulation at buried interfaces. United States. doi:10.1039/C9TA07123G.
Xue, Yudong, Fishman, Zachary S., Wang, Yunting, Pan, Zhenhua, Shen, Xin, Yanagi, Rito, Hutchings, Gregory S., Liu, Mingzhao, Zheng, Shili, Zhang, Yi, Altman, Eric I., and Hu, Shu. Mon . "Hydrogen evolution activity tuning via two-dimensional electron accumulation at buried interfaces". United States. doi:10.1039/C9TA07123G.
@article{osti_1574914,
title = {Hydrogen evolution activity tuning via two-dimensional electron accumulation at buried interfaces},
author = {Xue, Yudong and Fishman, Zachary S. and Wang, Yunting and Pan, Zhenhua and Shen, Xin and Yanagi, Rito and Hutchings, Gregory S. and Liu, Mingzhao and Zheng, Shili and Zhang, Yi and Altman, Eric I. and Hu, Shu},
abstractNote = {Developing efficient earth-abundant transition metal-based electrocatalysts for the hydrogen evolution reaction (HER) is crucial for hydrogen production at scale. This paper reports that the buried electrocatalytic interfaces between Ni–Fe sulfide (NiFeS) nanosheets and TiO2 conformal coatings (about 5 nm) achieved remarkable HER activity improvement, lowering the HER overpotential from –170 mV to –107 mV at –50 mA cm–2 in a base. Non-HER active, permeable TiO2 coatings grown by atomic layer deposition (ALD) achieved continuous fine-tuning of the electronic properties at the buried TiO2/NiFeS interfaces, as a novel strategy and the main factor for electron accumulation at the interface. Core-level and valence band X-ray photoelectron spectroscopy (XPS) was used to investigate the TiO2 electronic-structure tuning effect on the charge-transfer energetics during the HER. Their alkaline HER mechanism was elucidated by supplementing characterizations of membrane permeation, Tafel slope, and synchrotron X-ray absorption spectroscopy, which verified that the buried TiO2/NiFeS interfaces are electrocatalytically active. Here, this study offers a general strategy for improving the charge-transfer kinetics of an electrocatalytic system by confining catalysis at a permeable solid–solid interface. The broad applicability of permeable and tunable coatings potentially accelerates the optimization of earth-abundant catalysts to achieve high performance under operationally relevant conditions.},
doi = {10.1039/C9TA07123G},
journal = {Journal of Materials Chemistry. A},
number = 36,
volume = 7,
place = {United States},
year = {2019},
month = {8}
}

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