Surface-functionalized three-dimensional MXene supports to boost the hydrogen evolution activity of Pt catalysts in alkaline media

Haeji Hong; Ho Young Kim; Won Il Cho; Ho Chang Song; Hyung Chul Ham; Kyunghee Chae; Filipe Marques Mota; Jin Young Kim; Dong Ha Kim

doi:10.1039/d2ta08852e

Surface-functionalized three-dimensional MXene supports to boost the hydrogen evolution activity of Pt catalysts in alkaline media

Haeji Hong, Ho Young Kim, Won Il Cho, Ho Chang Song, Hyung Chul Ham, Kyunghee Chae, Filipe Marques Mota, Jin Young Kim, Dong Ha Kim

Department of Chemistry & Nanoscience

Research output: Contribution to journal › Article › peer-review

13 Scopus citations

Abstract

Alkaline water electrolysis is the most promising technology for green-hydrogen production, which is considered a cornerstone of carbon-neutral energy society. In the development of functional catalysts able to overcome the sluggish kinetics of the alkaline hydrogen evolution reaction (HER), MXenes emerge as attractive support candidates with distinctive hydrophilicity, high conductivity, and high (electro)chemical stability. Herein, we assess the promise of three-dimensionally interconnected Ti₃C₂T_x MXenes with distinct surface terminations (-O, -OH, and -F) as efficient support materials for Pt-loaded alkaline HER catalysts. In particular, our OH-functionalized Pt/Ti₃C₂(OH)_x shows the highest HER activity (30 mV dec⁻¹), unlocking a competitive performance against the Pt/C reference (61 mV dec⁻¹) and benchmark literature reports. The outstanding performance is ascribed to the cooperative effects of the extended MXene surface area and established interactions between Pt and Ti(OH)_x surface centers. In parallel, the oxophilic nature of Ti₃C₂(OH)_x facilitates Pt dispersion, presumably playing a key role in the extended catalytic stability here reported. The superior activity is further substantiated by density functional theory calculations, with the modeled Pt/Ti₃C₂(OH)₂ unveiling a significantly higher onset potential and the weakest hydrogen binding energy over supported Pt nanoparticles (−2.51 eV) against both -O (−2.72 eV) and -F (−3.15 eV) functionalized counterparts.

Original language	English
Pages (from-to)	5328-5336
Number of pages	9
Journal	Journal of Materials Chemistry A
Volume	11
Issue number	10
DOIs	https://doi.org/10.1039/d2ta08852e
State	Published - 17 Feb 2023

Bibliographical note

Funding Information:
The work was supported by the National Research Foundation (NRF) of Korea Grant funded by the Korean Government (2020R 1A 2C 3003958), by the Basic Science Research Program (Priority Research Institute) through the NRF funded by the Ministry of Education (2021R1A6A1A10039823), and by the Korea Basic Science Institute (National Research Facilities and Equipment Center) grant funded by the Ministry of Education (2020R1A6C101B194). F. M. M. acknowledges the support by the Brain Pool Program through the NRF funded by the Ministry of Science and ICT (2017H1D3A1A02054206). The work was also supported by the KIST Institutional Program (2E31871) and by the program of Future Hydrogen Original Technology Development (NRF-2021M3I3A1082879) through the NRF funded by the Korea government (Ministry of Science and ICT). This work was also financially supported by the NRF grant funded by the Korea government (MSIT) (NRF-2020R1A2C1099711). This work was supported by the Korea Institute Energy Technology Evaluation and Planning (KETEP) grant funded by the Korea government (MOTIE) (no. 20213030030260).

Publisher Copyright:
© 2023 The Royal Society of Chemistry

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@article{87f7cb098b434ee7ae46b4bc6c77daf0,

title = "Surface-functionalized three-dimensional MXene supports to boost the hydrogen evolution activity of Pt catalysts in alkaline media",

abstract = "Alkaline water electrolysis is the most promising technology for green-hydrogen production, which is considered a cornerstone of carbon-neutral energy society. In the development of functional catalysts able to overcome the sluggish kinetics of the alkaline hydrogen evolution reaction (HER), MXenes emerge as attractive support candidates with distinctive hydrophilicity, high conductivity, and high (electro)chemical stability. Herein, we assess the promise of three-dimensionally interconnected Ti3C2Tx MXenes with distinct surface terminations (-O, -OH, and -F) as efficient support materials for Pt-loaded alkaline HER catalysts. In particular, our OH-functionalized Pt/Ti3C2(OH)x shows the highest HER activity (30 mV dec−1), unlocking a competitive performance against the Pt/C reference (61 mV dec−1) and benchmark literature reports. The outstanding performance is ascribed to the cooperative effects of the extended MXene surface area and established interactions between Pt and Ti(OH)x surface centers. In parallel, the oxophilic nature of Ti3C2(OH)x facilitates Pt dispersion, presumably playing a key role in the extended catalytic stability here reported. The superior activity is further substantiated by density functional theory calculations, with the modeled Pt/Ti3C2(OH)2 unveiling a significantly higher onset potential and the weakest hydrogen binding energy over supported Pt nanoparticles (−2.51 eV) against both -O (−2.72 eV) and -F (−3.15 eV) functionalized counterparts.",

author = "Haeji Hong and Kim, {Ho Young} and Cho, {Won Il} and Song, {Ho Chang} and Ham, {Hyung Chul} and Kyunghee Chae and {Marques Mota}, Filipe and Kim, {Jin Young} and Kim, {Dong Ha}",

note = "Funding Information: The work was supported by the National Research Foundation (NRF) of Korea Grant funded by the Korean Government (2020R 1A 2C 3003958), by the Basic Science Research Program (Priority Research Institute) through the NRF funded by the Ministry of Education (2021R1A6A1A10039823), and by the Korea Basic Science Institute (National Research Facilities and Equipment Center) grant funded by the Ministry of Education (2020R1A6C101B194). F. M. M. acknowledges the support by the Brain Pool Program through the NRF funded by the Ministry of Science and ICT (2017H1D3A1A02054206). The work was also supported by the KIST Institutional Program (2E31871) and by the program of Future Hydrogen Original Technology Development (NRF-2021M3I3A1082879) through the NRF funded by the Korea government (Ministry of Science and ICT). This work was also financially supported by the NRF grant funded by the Korea government (MSIT) (NRF-2020R1A2C1099711). This work was supported by the Korea Institute Energy Technology Evaluation and Planning (KETEP) grant funded by the Korea government (MOTIE) (no. 20213030030260). Publisher Copyright: {\textcopyright} 2023 The Royal Society of Chemistry",

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doi = "10.1039/d2ta08852e",

language = "English",

volume = "11",

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T1 - Surface-functionalized three-dimensional MXene supports to boost the hydrogen evolution activity of Pt catalysts in alkaline media

AU - Hong, Haeji

AU - Kim, Ho Young

AU - Cho, Won Il

AU - Song, Ho Chang

AU - Ham, Hyung Chul

AU - Chae, Kyunghee

AU - Marques Mota, Filipe

AU - Kim, Jin Young

AU - Kim, Dong Ha

N1 - Funding Information: The work was supported by the National Research Foundation (NRF) of Korea Grant funded by the Korean Government (2020R 1A 2C 3003958), by the Basic Science Research Program (Priority Research Institute) through the NRF funded by the Ministry of Education (2021R1A6A1A10039823), and by the Korea Basic Science Institute (National Research Facilities and Equipment Center) grant funded by the Ministry of Education (2020R1A6C101B194). F. M. M. acknowledges the support by the Brain Pool Program through the NRF funded by the Ministry of Science and ICT (2017H1D3A1A02054206). The work was also supported by the KIST Institutional Program (2E31871) and by the program of Future Hydrogen Original Technology Development (NRF-2021M3I3A1082879) through the NRF funded by the Korea government (Ministry of Science and ICT). This work was also financially supported by the NRF grant funded by the Korea government (MSIT) (NRF-2020R1A2C1099711). This work was supported by the Korea Institute Energy Technology Evaluation and Planning (KETEP) grant funded by the Korea government (MOTIE) (no. 20213030030260). Publisher Copyright: © 2023 The Royal Society of Chemistry

PY - 2023/2/17

Y1 - 2023/2/17

N2 - Alkaline water electrolysis is the most promising technology for green-hydrogen production, which is considered a cornerstone of carbon-neutral energy society. In the development of functional catalysts able to overcome the sluggish kinetics of the alkaline hydrogen evolution reaction (HER), MXenes emerge as attractive support candidates with distinctive hydrophilicity, high conductivity, and high (electro)chemical stability. Herein, we assess the promise of three-dimensionally interconnected Ti3C2Tx MXenes with distinct surface terminations (-O, -OH, and -F) as efficient support materials for Pt-loaded alkaline HER catalysts. In particular, our OH-functionalized Pt/Ti3C2(OH)x shows the highest HER activity (30 mV dec−1), unlocking a competitive performance against the Pt/C reference (61 mV dec−1) and benchmark literature reports. The outstanding performance is ascribed to the cooperative effects of the extended MXene surface area and established interactions between Pt and Ti(OH)x surface centers. In parallel, the oxophilic nature of Ti3C2(OH)x facilitates Pt dispersion, presumably playing a key role in the extended catalytic stability here reported. The superior activity is further substantiated by density functional theory calculations, with the modeled Pt/Ti3C2(OH)2 unveiling a significantly higher onset potential and the weakest hydrogen binding energy over supported Pt nanoparticles (−2.51 eV) against both -O (−2.72 eV) and -F (−3.15 eV) functionalized counterparts.

AB - Alkaline water electrolysis is the most promising technology for green-hydrogen production, which is considered a cornerstone of carbon-neutral energy society. In the development of functional catalysts able to overcome the sluggish kinetics of the alkaline hydrogen evolution reaction (HER), MXenes emerge as attractive support candidates with distinctive hydrophilicity, high conductivity, and high (electro)chemical stability. Herein, we assess the promise of three-dimensionally interconnected Ti3C2Tx MXenes with distinct surface terminations (-O, -OH, and -F) as efficient support materials for Pt-loaded alkaline HER catalysts. In particular, our OH-functionalized Pt/Ti3C2(OH)x shows the highest HER activity (30 mV dec−1), unlocking a competitive performance against the Pt/C reference (61 mV dec−1) and benchmark literature reports. The outstanding performance is ascribed to the cooperative effects of the extended MXene surface area and established interactions between Pt and Ti(OH)x surface centers. In parallel, the oxophilic nature of Ti3C2(OH)x facilitates Pt dispersion, presumably playing a key role in the extended catalytic stability here reported. The superior activity is further substantiated by density functional theory calculations, with the modeled Pt/Ti3C2(OH)2 unveiling a significantly higher onset potential and the weakest hydrogen binding energy over supported Pt nanoparticles (−2.51 eV) against both -O (−2.72 eV) and -F (−3.15 eV) functionalized counterparts.

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DO - 10.1039/d2ta08852e

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VL - 11

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JO - Journal of Materials Chemistry A

JF - Journal of Materials Chemistry A

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ER -

Surface-functionalized three-dimensional MXene supports to boost the hydrogen evolution activity of Pt catalysts in alkaline media

Abstract

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