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High ammonia adsorption in MFM-300 materials: Dynamics and charge transfer in host–guest binding
Authors:
Xue
Han
(University of Manchester)
,
Wanpeng
Lu
(University of Manchester)
,
Yinlin
Chen
(University of Manchester)
,
Ivan
Da Silva
(ISIS Facility)
,
Jiangnan
Li
(University of Manchester)
,
Longfei
Lin
(University of Manchester)
,
Weiyao
Li
(University of Manchester)
,
Alena M.
Sheveleva
(University of Manchester)
,
Harry G. W.
Godfrey
(University of Manchester)
,
Zhenzhong
Lu
(University of Manchester)
,
Floriana
Tuna
(University of Manchester)
,
Eric J. L.
Mcinnes
(University of Manchester)
,
Yongqiang
Cheng
(Oak Ridge National Laboratory)
,
Luke L.
Daemen
(Oak Ridge National Laboratory)
,
Laura J.
Mccormick Mcpherson
(Advanced Light Source)
,
Simon J.
Teat
(Advanced Light Source)
,
Mark D.
Frogley
(Diamond Light Source)
,
Svemir
Rudic
(ISIS Facility)
,
Pascal
Manuel
(ISIS Facility)
,
Anibal J.
Ramirez-Cuesta
(Oak Ridge National Laboratory)
,
Sihai
Yang
(University of Manchester)
,
Martin
Schroeder
(University of Manchester)
Co-authored by industrial partner:
No
Type:
Journal Paper
Journal:
Journal Of The American Chemical Society
State:
Published (Approved)
Published:
February 2021
Diamond Proposal Number(s):
23782
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.
Journal Keywords: Adsorption; Molecules; Metal organic frameworks; Physical and chemical processes; Materials
Diamond Keywords: Hydrogen Storage
Subject Areas:
Materials,
Chemistry
Instruments:
B22-Multimode InfraRed imaging And Microspectroscopy
Other Facilities: TOSCA/WISH at ISIS
Added On:
22/02/2021 08:39
Discipline Tags:
Chemistry
Materials Science
Metal-Organic Frameworks
Metallurgy
Organometallic Chemistry
Technical Tags:
Spectroscopy
Infrared Spectroscopy
Synchtron-based Fourier Transform Infrared Spectroscopy (SR-FTIR)