Hydrogen Spillover and Storage on Graphene with Single-Site Ti Catalysts

Jhih Wei Chen; Shang Hsien Hsieh; Sheng Shong Wong; Ya Chi Chiu; Hung Wei Shiu; Chia Hsin Wang; Yaw Wen Yang; Yao Jane Hsu; Domenica Convertino; Camilla Coletti; Stefan Heun; Chia Hao Chen; Chung Lin Wu

doi:10.1021/acsenergylett.2c00941

Hydrogen Spillover and Storage on Graphene with Single-Site Ti Catalysts

Jhih Wei Chen, Shang Hsien Hsieh, Sheng Shong Wong, Ya Chi Chiu, Hung Wei Shiu, Chia Hsin Wang, Yaw Wen Yang, Yao Jane Hsu, Domenica Convertino, Camilla Coletti, Stefan Heun, Chia Hao Chen, Chung Lin Wu

Department of Physics

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

20 Citations (Scopus)

Abstract

Hydrogen spillover and storage for single-site metal catalysts, including single-atom catalysts (SACs) and single nanocluster catalysts, have been elucidated for various supports but remain poorly understood for inert carbon supports. Here, we use synchrotron-radiation-based methods to investigate the role of single-site Ti catalysts on graphene for hydrogen spillover and storage. Our in situ angle-resolved photoemission spectra results demonstrate a band gap opening, and X-ray absorption spectra reveal the formation of C-H bonds, both indicating partial graphene hydrogenation. With increasing Ti deposition and H2 exposure, the Ti atoms tend to aggregate to form nanocluster catalysts and yield 13.5% sp3-hybridized carbon atoms corresponding to a hydrogen-storage capacity of 1.11 wt % (excluding the weight of the Ti nanoclusters [Bhowmick, R. et al. J. Am. Chem. Soc. 2011, 133 (14), 5580]). Our results demonstrate how a simple spillover process at Ti SACs can lead to covalent hydrogen bonding on graphene, thereby providing a strategy for the rational design of carbon-supported single-site catalysts.

Original language	English
Pages (from-to)	2297-2303
Number of pages	7
Journal	ACS Energy Letters
Volume	7
Issue number	7
DOIs	https://doi.org/10.1021/acsenergylett.2c00941
Publication status	Published - 2022 Jul 8

All Science Journal Classification (ASJC) codes

Chemistry (miscellaneous)
Renewable Energy, Sustainability and the Environment
Fuel Technology
Energy Engineering and Power Technology
Materials Chemistry

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1021/acsenergylett.2c00941

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title = "Hydrogen Spillover and Storage on Graphene with Single-Site Ti Catalysts",

abstract = "Hydrogen spillover and storage for single-site metal catalysts, including single-atom catalysts (SACs) and single nanocluster catalysts, have been elucidated for various supports but remain poorly understood for inert carbon supports. Here, we use synchrotron-radiation-based methods to investigate the role of single-site Ti catalysts on graphene for hydrogen spillover and storage. Our in situ angle-resolved photoemission spectra results demonstrate a band gap opening, and X-ray absorption spectra reveal the formation of C-H bonds, both indicating partial graphene hydrogenation. With increasing Ti deposition and H2 exposure, the Ti atoms tend to aggregate to form nanocluster catalysts and yield 13.5% sp3-hybridized carbon atoms corresponding to a hydrogen-storage capacity of 1.11 wt % (excluding the weight of the Ti nanoclusters [Bhowmick, R. et al. J. Am. Chem. Soc. 2011, 133 (14), 5580]). Our results demonstrate how a simple spillover process at Ti SACs can lead to covalent hydrogen bonding on graphene, thereby providing a strategy for the rational design of carbon-supported single-site catalysts.",

author = "Chen, {Jhih Wei} and Hsieh, {Shang Hsien} and Wong, {Sheng Shong} and Chiu, {Ya Chi} and Shiu, {Hung Wei} and Wang, {Chia Hsin} and Yang, {Yaw Wen} and Hsu, {Yao Jane} and Domenica Convertino and Camilla Coletti and Stefan Heun and Chen, {Chia Hao} and Wu, {Chung Lin}",

note = "Funding Information: We thank Dr. Yeu-Kuang Hwu of Academia Sinica for providing a mu-metal chamber for the ARPES measurements and NSRRC beamline staff for skillful assistance during SR experiments. This work was funded by the Taiwan Ministry of Science and Technology. Publisher Copyright: {\textcopyright} 2022 American Chemical Society.",

year = "2022",

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doi = "10.1021/acsenergylett.2c00941",

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AU - Chen, Jhih Wei

AU - Hsieh, Shang Hsien

AU - Wong, Sheng Shong

AU - Chiu, Ya Chi

AU - Shiu, Hung Wei

AU - Wang, Chia Hsin

AU - Yang, Yaw Wen

AU - Hsu, Yao Jane

AU - Convertino, Domenica

AU - Coletti, Camilla

AU - Heun, Stefan

AU - Chen, Chia Hao

AU - Wu, Chung Lin

N1 - Funding Information: We thank Dr. Yeu-Kuang Hwu of Academia Sinica for providing a mu-metal chamber for the ARPES measurements and NSRRC beamline staff for skillful assistance during SR experiments. This work was funded by the Taiwan Ministry of Science and Technology. Publisher Copyright: © 2022 American Chemical Society.

PY - 2022/7/8

Y1 - 2022/7/8

N2 - Hydrogen spillover and storage for single-site metal catalysts, including single-atom catalysts (SACs) and single nanocluster catalysts, have been elucidated for various supports but remain poorly understood for inert carbon supports. Here, we use synchrotron-radiation-based methods to investigate the role of single-site Ti catalysts on graphene for hydrogen spillover and storage. Our in situ angle-resolved photoemission spectra results demonstrate a band gap opening, and X-ray absorption spectra reveal the formation of C-H bonds, both indicating partial graphene hydrogenation. With increasing Ti deposition and H2 exposure, the Ti atoms tend to aggregate to form nanocluster catalysts and yield 13.5% sp3-hybridized carbon atoms corresponding to a hydrogen-storage capacity of 1.11 wt % (excluding the weight of the Ti nanoclusters [Bhowmick, R. et al. J. Am. Chem. Soc. 2011, 133 (14), 5580]). Our results demonstrate how a simple spillover process at Ti SACs can lead to covalent hydrogen bonding on graphene, thereby providing a strategy for the rational design of carbon-supported single-site catalysts.

AB - Hydrogen spillover and storage for single-site metal catalysts, including single-atom catalysts (SACs) and single nanocluster catalysts, have been elucidated for various supports but remain poorly understood for inert carbon supports. Here, we use synchrotron-radiation-based methods to investigate the role of single-site Ti catalysts on graphene for hydrogen spillover and storage. Our in situ angle-resolved photoemission spectra results demonstrate a band gap opening, and X-ray absorption spectra reveal the formation of C-H bonds, both indicating partial graphene hydrogenation. With increasing Ti deposition and H2 exposure, the Ti atoms tend to aggregate to form nanocluster catalysts and yield 13.5% sp3-hybridized carbon atoms corresponding to a hydrogen-storage capacity of 1.11 wt % (excluding the weight of the Ti nanoclusters [Bhowmick, R. et al. J. Am. Chem. Soc. 2011, 133 (14), 5580]). Our results demonstrate how a simple spillover process at Ti SACs can lead to covalent hydrogen bonding on graphene, thereby providing a strategy for the rational design of carbon-supported single-site catalysts.

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Hydrogen Spillover and Storage on Graphene with Single-Site Ti Catalysts

Abstract

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