Effects of Catalyst Phase on the Hydrogen Evolution Reaction of Water Splitting: Preparation of Phase-Pure Films of FeP, Fe2P, and Fe3 P and Their Relative Catalytic Activities
Abstract
The comparative catalytic activities of iron phosphides, FexP (x = 1–3), have been established with phase-pure material grown by chemical vapor deposition (CVD) from single-source organometallic precursors. This is the first report of the preparation of phase-pure thin films of FeP and Fe2P, and their identity was established with scanning-electron microscopy, X-ray photoelectron spectroscopy, and powder X-ray diffraction. All materials were deposited on fluorine-doped tin oxide (FTO) for evaluation of their activities toward the hydrogen evolution reaction (HER) of water splitting in 0.5 M H2SO4. HER activity follows the trend Fe3P > Fe2P > FeP, with Fe3P having the lowest overpotential of 49 mV at a current density of 10 mA cm–2. Density functional theory (DFT) calculations are congruent with the observed activity trend with hydrogen binding favoring the iron-rich terminating surfaces of Fe3P and Fe2P over the iron-poor terminating surfaces of FeP. The results present a clear trend of activity with iron-rich phosphide phases outperforming phosphorus rich phases for hydrogen evolution. The films of Fe2P were grown using Fe(CO)4PH3 (1), while the films of FeP were prepared using either Fe(CO)4PtBuH2 (2) or the new molecule {Fe(CO)4P(H)tBu}2 (3) on quartz and FTO. Compound 3 was prepared from the reaction ofmore »
- Authors:
-
- Rice Univ., Houston, TX (United States)
- Univ. of Houston, TX (United States); Univ. of Electronic Science and Technology of China, Chengdu (China)
- Univ. of Houston, TX (United States)
- Univ. of Electronic Science and Technology of China, Chengdu (China)
- 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 Office of Science (SC)
- OSTI Identifier:
- 1543610
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Volume: 30; Journal Issue: 10; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry; Materials Science
Citation Formats
Schipper, Desmond E., Zhao, Zhenhuan, Thirumalai, Hari, Leitner, Andrew P., Donaldson, Samantha L., Kumar, Arvind, Qin, Fan, Wang, Zhiming, Grabow, Lars C., Bao, Jiming, and Whitmire, Kenton H. Effects of Catalyst Phase on the Hydrogen Evolution Reaction of Water Splitting: Preparation of Phase-Pure Films of FeP, Fe2P, and Fe3 P and Their Relative Catalytic Activities. United States: N. p., 2018.
Web. doi:10.1021/acs.chemmater.8b01624.
Schipper, Desmond E., Zhao, Zhenhuan, Thirumalai, Hari, Leitner, Andrew P., Donaldson, Samantha L., Kumar, Arvind, Qin, Fan, Wang, Zhiming, Grabow, Lars C., Bao, Jiming, & Whitmire, Kenton H. Effects of Catalyst Phase on the Hydrogen Evolution Reaction of Water Splitting: Preparation of Phase-Pure Films of FeP, Fe2P, and Fe3 P and Their Relative Catalytic Activities. United States. https://doi.org/10.1021/acs.chemmater.8b01624
Schipper, Desmond E., Zhao, Zhenhuan, Thirumalai, Hari, Leitner, Andrew P., Donaldson, Samantha L., Kumar, Arvind, Qin, Fan, Wang, Zhiming, Grabow, Lars C., Bao, Jiming, and Whitmire, Kenton H. Thu .
"Effects of Catalyst Phase on the Hydrogen Evolution Reaction of Water Splitting: Preparation of Phase-Pure Films of FeP, Fe2P, and Fe3 P and Their Relative Catalytic Activities". United States. https://doi.org/10.1021/acs.chemmater.8b01624. https://www.osti.gov/servlets/purl/1543610.
@article{osti_1543610,
title = {Effects of Catalyst Phase on the Hydrogen Evolution Reaction of Water Splitting: Preparation of Phase-Pure Films of FeP, Fe2P, and Fe3 P and Their Relative Catalytic Activities},
author = {Schipper, Desmond E. and Zhao, Zhenhuan and Thirumalai, Hari and Leitner, Andrew P. and Donaldson, Samantha L. and Kumar, Arvind and Qin, Fan and Wang, Zhiming and Grabow, Lars C. and Bao, Jiming and Whitmire, Kenton H.},
abstractNote = {The comparative catalytic activities of iron phosphides, FexP (x = 1–3), have been established with phase-pure material grown by chemical vapor deposition (CVD) from single-source organometallic precursors. This is the first report of the preparation of phase-pure thin films of FeP and Fe2P, and their identity was established with scanning-electron microscopy, X-ray photoelectron spectroscopy, and powder X-ray diffraction. All materials were deposited on fluorine-doped tin oxide (FTO) for evaluation of their activities toward the hydrogen evolution reaction (HER) of water splitting in 0.5 M H2SO4. HER activity follows the trend Fe3P > Fe2P > FeP, with Fe3P having the lowest overpotential of 49 mV at a current density of 10 mA cm–2. Density functional theory (DFT) calculations are congruent with the observed activity trend with hydrogen binding favoring the iron-rich terminating surfaces of Fe3P and Fe2P over the iron-poor terminating surfaces of FeP. The results present a clear trend of activity with iron-rich phosphide phases outperforming phosphorus rich phases for hydrogen evolution. The films of Fe2P were grown using Fe(CO)4PH3 (1), while the films of FeP were prepared using either Fe(CO)4PtBuH2 (2) or the new molecule {Fe(CO)4P(H)tBu}2 (3) on quartz and FTO. Compound 3 was prepared from the reaction of PCl2tBu with a mixture of Na[HFe(CO)4] and Na2[Fe(CO)4] and characterized by single-crystal X-ray diffraction, ESI-MS, elemental analysis, and 31P/1H NMR spectroscopies. Films of Fe3P were prepared as previously described from H2Fe3(CO)9PtBu (4).},
doi = {10.1021/acs.chemmater.8b01624},
journal = {Chemistry of Materials},
number = 10,
volume = 30,
place = {United States},
year = {Thu Apr 26 00:00:00 EDT 2018},
month = {Thu Apr 26 00:00:00 EDT 2018}
}
Web of Science
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