High Ammonia Adsorption in MFM-300 Materials: Dynamics and Charge Transfer in Host-Guest Binding

Xue Han; Wanpeng Lu; Yinlin Chen; Ivan Da Silva; Jiangnan Li; Longfei Lin; Weiyao Li; Alena M. Sheveleva; Harry G.W. Godfrey; Zhenzhong Lu; Floriana Tuna; Eric J.L. McInnes; Yongqiang Cheng; Luke L. Daemen; Laura J.Mc Cormick Mcpherson; Simon J. Teat; Mark D. Frogley; Svemir Rudić; Pascal Manuel; Anibal J. Ramirez-Cuesta; Sihai Yang; Martin Schröder

doi:10.1021/jacs.0c11930

High Ammonia Adsorption in MFM-300 Materials: Dynamics and Charge Transfer in Host-Guest Binding

Xue Han, Wanpeng Lu, Yinlin Chen, Ivan Da Silva, Jiangnan Li, Longfei Lin, Weiyao Li, Alena M. Sheveleva, Harry G.W. Godfrey, Zhenzhong Lu, Floriana Tuna, Eric J.L. McInnes, Yongqiang Cheng, Luke L. Daemen, Laura J.Mc Cormick Mcpherson, Simon J. Teat, Mark D. Frogley, Svemir Rudić, Pascal Manuel, Anibal J. Ramirez-CuestaSihai Yang, Martin Schröder

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

87 Scopus citations

Abstract

Ammonia (NH3) is a promising energy resource owing to its high hydrogen density. However, its widespread application is restricted by the lack of efficient and corrosion-resistant storage materials. Here, we report high NH3 adsorption in a series of robust metal-organic framework (MOF) materials, MFM-300(M) (M = Fe, V, Cr, In). MFM-300(M) (M = Fe, VIII, Cr) show fully reversible capacity for >20 cycles, reaching capacities of 16.1, 15.6, and 14.0 mmol g-1, respectively, at 273 K and 1 bar. Under the same conditions, MFM-300(VIV) exhibits the highest uptake among this series of MOFs of 17.3 mmol g-1. In situ neutron powder diffraction, single-crystal X-ray diffraction, and electron paramagnetic resonance spectroscopy confirm that the redox-active V center enables host-guest charge transfer, with VIV being reduced to VIII and NH3 being oxidized to hydrazine (N2H4). A combination of in situ inelastic neutron scattering and DFT modeling has revealed the binding dynamics of adsorbed NH3 within these MOFs to afford a comprehensive insight into the application of MOF materials to the adsorption and conversion of NH3.

Original language	English
Pages (from-to)	3153-3161
Number of pages	9
Journal	Journal of the American Chemical Society
Volume	143
Issue number	8
DOIs	https://doi.org/10.1021/jacs.0c11930
State	Published - Mar 3 2021

Funding

We thank EPSRC (EP/I011870), the Royal Society, and University of Manchester. This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement no. 742401, NANOCHEM). We are grateful to Diamond Light Source and STFC/ISIS Facility for access to Beamlines B22 (SM23782) and TOSCA/WISH, respectively, and to Oak Ridge National Laboratory for access to the VISION spectrometer at the Spallation Neutron Source, a DOE Office of Science User Facility under Contract No. DE-AC0500OR22725 with UT Battelle, LLC. This research used resources of Beamlines 11.3.1 and 12.2.1 at the Advanced Light Source, which is a U.S. DOE Office of Science User Facility under contract no. DE-AC02-05CH11231. The computing resources were made available through the VirtuES and the ICE-MAN projects, funded by Laboratory Directed Research and Development program and Compute and Data Environment for Science (CADES) at ORNL. J.L. thanks China Scholarship Council (CSC) for funding. A.M.S. is supported by a Royal Society Newton Fellowship. We thank the EPSRC National EPR Facility at the University of Manchester for support with the EPR measurements.

Funders	Funder number
Compute and Data Environment for Science
Office of Science	DE-AC0500OR22725, DE-AC02-05CH11231
Laboratory Directed Research and Development
Horizon 2020 Framework Programme	SM23782, 742401
Royal Society
European Research Council
China Scholarship Council

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Han, X., Lu, W., Chen, Y., Da Silva, I., Li, J., Lin, L., Li, W., Sheveleva, A. M., Godfrey, H. G. W., Lu, Z., Tuna, F., McInnes, E. J. L., Cheng, Y., Daemen, L. L., Mcpherson, L. J. M. C., Teat, S. J., Frogley, M. D., Rudić, S., Manuel, P., ... Schröder, M. (2021). High Ammonia Adsorption in MFM-300 Materials: Dynamics and Charge Transfer in Host-Guest Binding. Journal of the American Chemical Society, 143(8), 3153-3161. https://doi.org/10.1021/jacs.0c11930

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title = "High Ammonia Adsorption in MFM-300 Materials: Dynamics and Charge Transfer in Host-Guest Binding",

abstract = "Ammonia (NH3) is a promising energy resource owing to its high hydrogen density. However, its widespread application is restricted by the lack of efficient and corrosion-resistant storage materials. Here, we report high NH3 adsorption in a series of robust metal-organic framework (MOF) materials, MFM-300(M) (M = Fe, V, Cr, In). MFM-300(M) (M = Fe, VIII, Cr) show fully reversible capacity for >20 cycles, reaching capacities of 16.1, 15.6, and 14.0 mmol g-1, respectively, at 273 K and 1 bar. Under the same conditions, MFM-300(VIV) exhibits the highest uptake among this series of MOFs of 17.3 mmol g-1. In situ neutron powder diffraction, single-crystal X-ray diffraction, and electron paramagnetic resonance spectroscopy confirm that the redox-active V center enables host-guest charge transfer, with VIV being reduced to VIII and NH3 being oxidized to hydrazine (N2H4). A combination of in situ inelastic neutron scattering and DFT modeling has revealed the binding dynamics of adsorbed NH3 within these MOFs to afford a comprehensive insight into the application of MOF materials to the adsorption and conversion of NH3.",

author = "Xue Han and Wanpeng Lu and Yinlin Chen and {Da Silva}, Ivan and Jiangnan Li and Longfei Lin and Weiyao Li and Sheveleva, {Alena M.} and Godfrey, {Harry G.W.} and Zhenzhong Lu and Floriana Tuna and McInnes, {Eric J.L.} and Yongqiang Cheng and Daemen, {Luke L.} and Mcpherson, {Laura J.Mc Cormick} and Teat, {Simon J.} and Frogley, {Mark D.} and Svemir Rudi{\'c} and Pascal Manuel and Ramirez-Cuesta, {Anibal J.} and Sihai Yang and Martin Schr{\"o}der",

note = "Publisher Copyright: {\textcopyright} 2021 American Chemical Society.",

year = "2021",

month = mar,

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doi = "10.1021/jacs.0c11930",

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Han, X, Lu, W, Chen, Y, Da Silva, I, Li, J, Lin, L, Li, W, Sheveleva, AM, Godfrey, HGW, Lu, Z, Tuna, F, McInnes, EJL, Cheng, Y, Daemen, LL, Mcpherson, LJMC, Teat, SJ, Frogley, MD, Rudić, S, Manuel, P, Ramirez-Cuesta, AJ, Yang, S & Schröder, M 2021, 'High Ammonia Adsorption in MFM-300 Materials: Dynamics and Charge Transfer in Host-Guest Binding', Journal of the American Chemical Society, vol. 143, no. 8, pp. 3153-3161. https://doi.org/10.1021/jacs.0c11930

TY - JOUR

T1 - High Ammonia Adsorption in MFM-300 Materials

T2 - Dynamics and Charge Transfer in Host-Guest Binding

AU - Han, Xue

AU - Lu, Wanpeng

AU - Chen, Yinlin

AU - Da Silva, Ivan

AU - Li, Jiangnan

AU - Lin, Longfei

AU - Li, Weiyao

AU - Sheveleva, Alena M.

AU - Godfrey, Harry G.W.

AU - Lu, Zhenzhong

AU - Tuna, Floriana

AU - McInnes, Eric J.L.

AU - Cheng, Yongqiang

AU - Daemen, Luke L.

AU - Mcpherson, Laura J.Mc Cormick

AU - Teat, Simon J.

AU - Frogley, Mark D.

AU - Rudić, Svemir

AU - Manuel, Pascal

AU - Ramirez-Cuesta, Anibal J.

AU - Yang, Sihai

AU - Schröder, Martin

PY - 2021/3/3

Y1 - 2021/3/3

N2 - Ammonia (NH3) is a promising energy resource owing to its high hydrogen density. However, its widespread application is restricted by the lack of efficient and corrosion-resistant storage materials. Here, we report high NH3 adsorption in a series of robust metal-organic framework (MOF) materials, MFM-300(M) (M = Fe, V, Cr, In). MFM-300(M) (M = Fe, VIII, Cr) show fully reversible capacity for >20 cycles, reaching capacities of 16.1, 15.6, and 14.0 mmol g-1, respectively, at 273 K and 1 bar. Under the same conditions, MFM-300(VIV) exhibits the highest uptake among this series of MOFs of 17.3 mmol g-1. In situ neutron powder diffraction, single-crystal X-ray diffraction, and electron paramagnetic resonance spectroscopy confirm that the redox-active V center enables host-guest charge transfer, with VIV being reduced to VIII and NH3 being oxidized to hydrazine (N2H4). A combination of in situ inelastic neutron scattering and DFT modeling has revealed the binding dynamics of adsorbed NH3 within these MOFs to afford a comprehensive insight into the application of MOF materials to the adsorption and conversion of NH3.

AB - Ammonia (NH3) is a promising energy resource owing to its high hydrogen density. However, its widespread application is restricted by the lack of efficient and corrosion-resistant storage materials. Here, we report high NH3 adsorption in a series of robust metal-organic framework (MOF) materials, MFM-300(M) (M = Fe, V, Cr, In). MFM-300(M) (M = Fe, VIII, Cr) show fully reversible capacity for >20 cycles, reaching capacities of 16.1, 15.6, and 14.0 mmol g-1, respectively, at 273 K and 1 bar. Under the same conditions, MFM-300(VIV) exhibits the highest uptake among this series of MOFs of 17.3 mmol g-1. In situ neutron powder diffraction, single-crystal X-ray diffraction, and electron paramagnetic resonance spectroscopy confirm that the redox-active V center enables host-guest charge transfer, with VIV being reduced to VIII and NH3 being oxidized to hydrazine (N2H4). A combination of in situ inelastic neutron scattering and DFT modeling has revealed the binding dynamics of adsorbed NH3 within these MOFs to afford a comprehensive insight into the application of MOF materials to the adsorption and conversion of NH3.

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U2 - 10.1021/jacs.0c11930

DO - 10.1021/jacs.0c11930

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AN - SCOPUS:85101881133

SN - 0002-7863

VL - 143

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EP - 3161

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 8

ER -

High Ammonia Adsorption in MFM-300 Materials: Dynamics and Charge Transfer in Host-Guest Binding

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