Enhanced Hydrogen-Storage Capacity and Structural Stability of an Organic Clathrate Structure with Fullerene (C60) Guests and Lithium Doping

Yesol Woo; Byeong Soo Kim; Jong Won Lee; Jeasung Park; Minjun Cha; Satoshi Takeya; Junhyuck Im; Yongjae Lee; Tae In Jeon; Hyeonhu Bae; Hoonkyung Lee; Sang Soo Han; Byung Chul Yeo; Dongseon Kim; Ji Ho Yoon

doi:10.1021/acs.chemmater.8b00749

Enhanced Hydrogen-Storage Capacity and Structural Stability of an Organic Clathrate Structure with Fullerene (C₆₀) Guests and Lithium Doping

Yesol Woo, Byeong Soo Kim, Jong Won Lee, Jeasung Park, Minjun Cha, Satoshi Takeya, Junhyuck Im, Yongjae Lee, Tae In Jeon, Hyeonhu Bae, Hoonkyung Lee, Sang Soo Han, Byung Chul Yeo, Dongseon Kim, Ji Ho Yoon

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

25 Citations (Scopus)

Abstract

An effective combination of host and guest molecules in a framework type of architecture can enhance the structural stability and physical properties of clathrate compounds. We report here that an organic clathrate compound consisting of a fullerene (C₆₀) guest and a hydroquinone (HQ) host framework shows enhanced hydrogen-storage capacity and good structural stability under pressures and temperatures up to 10 GPa and 438 K, respectively. This combined structure is formed in the extended β-type HQ clathrate and admits 16 hydrogen molecules per cage, leading to a volumetric hydrogen uptake of 49.5 g L^-1 at 77 K and 8 MPa, a value enhanced by 130% compared to that associated with the β-type HQ clathrate. A close examination according to density functional theory calculations and grand canonical Monte Carlo simulations confirms the synergistic combination effect of the guest-host molecules tailored for enhanced hydrogen storage. Moreover, the model simulations demonstrate that the lithium-doped HQ clathrates with C₆₀ guests reveal exceptionally high hydrogen-storage capacities. These results provide a new playground for additional fundamental studies of the structure-property relationships and migration characteristics of small molecules in nanostructured materials.

Original language	English
Pages (from-to)	3028-3039
Number of pages	12
Journal	Chemistry of Materials
Volume	30
Issue number	9
DOIs	https://doi.org/10.1021/acs.chemmater.8b00749
Publication status	Published - 2018 May 8

Bibliographical note

Publisher Copyright:
© 2018 American Chemical Society.

All Science Journal Classification (ASJC) codes

General Chemistry
General Chemical Engineering
Materials Chemistry

Access to Document

10.1021/acs.chemmater.8b00749

Cite this

Woo, Y., Kim, B. S., Lee, J. W., Park, J., Cha, M., Takeya, S., Im, J., Lee, Y., Jeon, T. I., Bae, H., Lee, H., Han, S. S., Yeo, B. C., Kim, D., & Yoon, J. H. (2018). Enhanced Hydrogen-Storage Capacity and Structural Stability of an Organic Clathrate Structure with Fullerene (C₆₀) Guests and Lithium Doping. Chemistry of Materials, 30(9), 3028-3039. https://doi.org/10.1021/acs.chemmater.8b00749

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title = "Enhanced Hydrogen-Storage Capacity and Structural Stability of an Organic Clathrate Structure with Fullerene (C60) Guests and Lithium Doping",

abstract = "An effective combination of host and guest molecules in a framework type of architecture can enhance the structural stability and physical properties of clathrate compounds. We report here that an organic clathrate compound consisting of a fullerene (C60) guest and a hydroquinone (HQ) host framework shows enhanced hydrogen-storage capacity and good structural stability under pressures and temperatures up to 10 GPa and 438 K, respectively. This combined structure is formed in the extended β-type HQ clathrate and admits 16 hydrogen molecules per cage, leading to a volumetric hydrogen uptake of 49.5 g L-1 at 77 K and 8 MPa, a value enhanced by 130% compared to that associated with the β-type HQ clathrate. A close examination according to density functional theory calculations and grand canonical Monte Carlo simulations confirms the synergistic combination effect of the guest-host molecules tailored for enhanced hydrogen storage. Moreover, the model simulations demonstrate that the lithium-doped HQ clathrates with C60 guests reveal exceptionally high hydrogen-storage capacities. These results provide a new playground for additional fundamental studies of the structure-property relationships and migration characteristics of small molecules in nanostructured materials.",

author = "Yesol Woo and Kim, {Byeong Soo} and Lee, {Jong Won} and Jeasung Park and Minjun Cha and Satoshi Takeya and Junhyuck Im and Yongjae Lee and Jeon, {Tae In} and Hyeonhu Bae and Hoonkyung Lee and Han, {Sang Soo} and Yeo, {Byung Chul} and Dongseon Kim and Yoon, {Ji Ho}",

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Woo, Y, Kim, BS, Lee, JW, Park, J, Cha, M, Takeya, S, Im, J, Lee, Y, Jeon, TI, Bae, H, Lee, H, Han, SS, Yeo, BC, Kim, D & Yoon, JH 2018, 'Enhanced Hydrogen-Storage Capacity and Structural Stability of an Organic Clathrate Structure with Fullerene (C₆₀) Guests and Lithium Doping', Chemistry of Materials, vol. 30, no. 9, pp. 3028-3039. https://doi.org/10.1021/acs.chemmater.8b00749

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AU - Woo, Yesol

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AU - Park, Jeasung

AU - Cha, Minjun

AU - Takeya, Satoshi

AU - Im, Junhyuck

AU - Lee, Yongjae

AU - Jeon, Tae In

AU - Bae, Hyeonhu

AU - Lee, Hoonkyung

AU - Han, Sang Soo

AU - Yeo, Byung Chul

AU - Kim, Dongseon

AU - Yoon, Ji Ho

PY - 2018/5/8

Y1 - 2018/5/8

N2 - An effective combination of host and guest molecules in a framework type of architecture can enhance the structural stability and physical properties of clathrate compounds. We report here that an organic clathrate compound consisting of a fullerene (C60) guest and a hydroquinone (HQ) host framework shows enhanced hydrogen-storage capacity and good structural stability under pressures and temperatures up to 10 GPa and 438 K, respectively. This combined structure is formed in the extended β-type HQ clathrate and admits 16 hydrogen molecules per cage, leading to a volumetric hydrogen uptake of 49.5 g L-1 at 77 K and 8 MPa, a value enhanced by 130% compared to that associated with the β-type HQ clathrate. A close examination according to density functional theory calculations and grand canonical Monte Carlo simulations confirms the synergistic combination effect of the guest-host molecules tailored for enhanced hydrogen storage. Moreover, the model simulations demonstrate that the lithium-doped HQ clathrates with C60 guests reveal exceptionally high hydrogen-storage capacities. These results provide a new playground for additional fundamental studies of the structure-property relationships and migration characteristics of small molecules in nanostructured materials.

AB - An effective combination of host and guest molecules in a framework type of architecture can enhance the structural stability and physical properties of clathrate compounds. We report here that an organic clathrate compound consisting of a fullerene (C60) guest and a hydroquinone (HQ) host framework shows enhanced hydrogen-storage capacity and good structural stability under pressures and temperatures up to 10 GPa and 438 K, respectively. This combined structure is formed in the extended β-type HQ clathrate and admits 16 hydrogen molecules per cage, leading to a volumetric hydrogen uptake of 49.5 g L-1 at 77 K and 8 MPa, a value enhanced by 130% compared to that associated with the β-type HQ clathrate. A close examination according to density functional theory calculations and grand canonical Monte Carlo simulations confirms the synergistic combination effect of the guest-host molecules tailored for enhanced hydrogen storage. Moreover, the model simulations demonstrate that the lithium-doped HQ clathrates with C60 guests reveal exceptionally high hydrogen-storage capacities. These results provide a new playground for additional fundamental studies of the structure-property relationships and migration characteristics of small molecules in nanostructured materials.

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