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. Mccormick Mpherson, Simon J. Teat, Mark D. Frogley, Svemir Rudić, Pascal Manuel, Anibal J. Ramirez-cuestaSihai Yang, Martin Schroder

Research output: Contribution to journalArticlepeer-review

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 languageEnglish
JournalJournal of the American Chemical Society
Early online date19 Feb 2021
DOIs
Publication statusPublished - 19 Feb 2021

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