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Instruments / Technical Area	Publication Details	Published
B22-Multimode InfraRed imaging And Microspectroscopy I11-High Resolution Powder Diffraction	Structural and dynamic analysis of adsorption of sulphur dioxide in a series of Zr‐based metal‐organic frameworks Jiangnan Li , Gemma L. Smith , Yinlin Chen , Yujie Ma , Meredydd Kippax-Jones , Mengtian Fan , Wanpeng Lu , Mark D. Frogley , Gianfelice Cinque , Sarah Day , Stephen P. Thompson , Yongqiang Cheng , Luke L. Daemen , Anibal J. Ramirez-Cuetos , Martin Schroeder , Sihai Yang Angewandte Chemie International Edition DOI: 10.1002/anie.202207259 Diamond Proposal Number(s): [28497, 29649] Open Access Show Abstract ▼ Abstract: We report reversible high capacity adsorption of SO2 in robust Zr-based metal-organic frameworks (MOFs). Zr-bptc (H4bptc = biphenyl-3,3’,5,5’-tetracarboxylic acid) shows a high SO2 uptake of 6.2 mmol g-1 at 0.1 bar and 298 K, reflecting excellent capture capability and removal of SO2 at low concentration (2500 ppm). Dynamic breakthrough experiments confirm that the introduction of amine, atomically-dispersed Cu(II) or heteroatomic sulphur sites into the pores enhance the capture of SO2 at low concentrations. The captured SO2 can be converted quantitatively to a pharmaceutical intermediate, aryl N-aminosulfonamide, thus converting waste to chemical values. In situ X-ray diffraction, infrared micro-spectroscopic and inelastic neutron scattering enable the visualisation of the binding domains of adsorbed SO2 molecules and host-guest binding dynamics in these materials at the atomic level. The refinement of pore environment plays a critical role in designing efficient sorbent materials.	Jun 2022
B18-Core EXAFS B22-Multimode InfraRed imaging And Microspectroscopy	Direct observation of ammonia storage in UIO-66 incorporating Cu(II) binding sites Yujie Ma , Wanpeng Lu , Xue Han , Yinlin Chen , Ivan Da Silva , Daniel Lee , Alena M. Sheveleva , Zi Wang , Jiangnan Li , Weiyao Li , Mengtian Fan , Shaojun Xu , Floriana Tuna , Eric J. L. Mcinnes , Yongqiang Cheng , Svemir Rudic , Pascal Manuel , Mark D. Frogley , Anibal J. Ramirez-Cuesta , Martin Schroeder , Sihai Yang Journal Of The American Chemical Society DOI: 10.1021/jacs.2c00952 Diamond Proposal Number(s): [19850] Open Access Show Abstract ▼ Abstract: The presence of active sites in metal–organic framework (MOF) materials can control and affect their performance significantly in adsorption and catalysis. However, revealing the interactions between the substrate and active sites in MOFs at atomic precision remains a challenging task. Here, we report the direct observation of binding of NH3 in a series of UiO-66 materials containing atomically dispersed defects and open Cu(I) and Cu(II) sites. While all MOFs in this series exhibit similar surface areas (1111–1135 m2 g–1), decoration of the −OH site in UiO-66-defect with Cu(II) results in a 43% enhancement of the isothermal uptake of NH3 at 273 K and 1.0 bar from 11.8 in UiO-66-defect to 16.9 mmol g–1 in UiO-66-CuII. A 100% enhancement of dynamic adsorption of NH3 at a concentration level of 630 ppm from 2.07 mmol g–1 in UiO-66-defect to 4.15 mmol g–1 in UiO-66-CuII at 298 K is observed. In situ neutron powder diffraction, inelastic neutron scattering, and electron paramagnetic resonance, solid-state nuclear magnetic resonance, and infrared spectroscopies, coupled with modeling reveal that the enhanced NH3 uptake in UiO-66-CuII originates from a {Cu(II)···NH3} interaction, with a reversible change in geometry at Cu(II) from near-linear to trigonal coordination. This work represents the first example of structural elucidation of NH3 binding in MOFs containing open metal sites and will inform the design of new efficient MOF sorbents by targeted control of active sites for NH3 capture and storage.	May 2022
B22-Multimode InfraRed imaging And Microspectroscopy	High capacity ammonia adsorption in a robust metal-organic framework mediated by reversible host-guest interactions Lixia Guo , Xue Han , Yujie Ma , Jiangnan Li , Wanpeng Lu , Weiyao Li , Daniel Lee , Ivan Da Silva , Yongqiang Cheng , Svemir Rudic , Pascal Manuel , Mark D. Frogley , Anibal Javier Ramirez-Cuesta , Martin Schroeder , Sihai Yang Chemical Communications DOI: 10.1039/D2CC01197B Diamond Proposal Number(s): [30398] Open Access Show Abstract ▼ Abstract: To understand the exceptional adsorption of ammonia (NH3) in MFM-300(Sc) (19.5 mmol g−1 at 273 K and 1 bar without hysteresis), we report a systematic investigation of the mechanism of adsorption by a combination of in situ neutron powder diffraction, inelastic neutron scattering, synchrotron infrared microspectroscopy, and solid-state 45Sc NMR spectroscopy. These complementary techniques reveal the formation of reversible host-guest supramolecular interactions, which explains directly the observed excellent reversibility of this material over 90 adsorption-desorption cycles.	Apr 2022
B22-Multimode InfraRed imaging And Microspectroscopy	A {Ni12}-wheel-based metal-organic framework for coordinative binding of sulphur dioxide and nitrogen dioxide Sihai Yang , Zongsu Han , Jiangnan Li , Wanpeng Lu , Kunyun Wang , Yinlin Chen , Xiaoping Zhang , Longfei Lin , Xue Han , Simon Teat , Mark Frogley , Wei Shi , Peng Cheng Angewandte Chemie International Edition DOI: 10.1002/anie.202115585 Diamond Proposal Number(s): [23782] Show Abstract ▼ Abstract: Air pollutions by SO2 and NO2 have caused significant risks on the environment and human health. Understanding the mechanism of active sites within capture materials is of fundamental importance to the development of new clean-up technologies. Here we report the crystallographic observation of reversible coordinative binding of SO2 and NO2 on open Ni(II) sites in a metal-organic framework (NKU-100) incorporating an unprecedented {Ni 12 }-wheel, which exhibits six open Ni(II) sites on desolvation. Immobilised gas molecules are further stabilised by cooperative host-guest interactions comprised of hydrogen bonds, π ··· π interactions and dipole interactions. At 298 K and 1.0 bar, NKU-100 shows adsorption uptakes of 6.21 and 5.80 mmol g -1 for SO2 and NO2 , respectively. Dynamic breakthrough experiments have confirmed the selective retention of SO2 and NO2 at low concentrations under dry conditions. This work will inspire the future design of efficient sorbents for the capture of SO2 and NO2 .	Nov 2021
B22-Multimode InfraRed imaging And Microspectroscopy	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 Mcpherson , Simon J. Teat , Mark D. Frogley , Svemir Rudic , Pascal Manuel , Anibal J. Ramirez-Cuesta , Sihai Yang , Martin Schroeder Journal Of The American Chemical Society DOI: 10.1021/jacs.0c11930 Diamond Proposal Number(s): [23782] Show Abstract ▼ 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.	Feb 2021

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