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Han, Xue; Lu, Wanpeng; Chen, Yinlin; da Silva, Ivan; Li, Jiangnan; Lin, Longfei; Li, Weiyao; Sheveleva, Alena M; Godfrey, Harry G. W; Lu, Zhenzhong; Tuna, Floriana; McInnes, Eric J. L; Cheng, Yongqiang; Daemen, Luke L; M, Laura J. M; Teat, Simon J; Frogley, Mark D; Rudić, Svemir; Manuel, Pascal; Ramirez-Cuesta, Anibal J; Yang, Sihai; Schröder, Martin
Journal of the American Chemical Society, 03/2021, Letnik: 143, Številka: 8Journal Article
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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JCR | SNIP | JCR | SNIP | JCR | SNIP | JCR | SNIP |
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