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

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

doi:10.1039/C9TA07123G

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

Journal Article · Mon Aug 19 00:00:00 EDT 2019 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/C9TA07123G· OSTI ID:1574914

^[1];

^[2]; Wang, Yunting ^[3]; Pan, Zhenhua ^[2]; Shen, Xin ^[2]; Yanagi, Rito ^[2]; Hutchings, Gregory S. ^[4];

^[5]; Zheng, Shili ^[6]; Zhang, Yi ^[6];

^[4];

^[2]

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)
Yale Univ., New Haven, CT (United States). Dept. of Chemical and Environmental Engineering; Yale Univ., West Haven, CT (United States). Energy Sciences Inst.
China Univ. of Mining and Technology, Beijing (China). School of Chemical and Environmental Engineering
Yale Univ., New Haven, CT (United States). Dept. of Chemical and Environmental Engineering
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials
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

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.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1574914

Report Number(s):: BNL-212338-2019-JAAM; JMCAET; TRN: US2001295

Journal Information:: Journal of Materials Chemistry. A, Vol. 7, Issue 36; ISSN 2050-7488

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 8 works

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