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Instruments / Technical Area	Publication Details	Published
B22-Multimode InfraRed imaging And Microspectroscopy	Efficient capture and storage of ammonia in robust aluminium-based metal-organic frameworks Lixia Guo , Joseph Hurd , Meng He , Wanpeng Lu , Jiangnan Li , Danielle Crawshaw , Mengtian Fan , Sergey A. Sapchenko , Yinlin Chen , Xiangdi Zeng , Meredydd Kippax-Jones , Wenyuan Huang , Zhaodong Zhu , Pascal Manuel , Mark D. Frogley , Daniel Lee , Martin Schroeder , Sihai Yang Communications Chemistry 6 DOI: 10.1038/s42004-023-00850-4 Diamond Proposal Number(s): [30398] Open Access Show Abstract ▼ Abstract: The development of stable sorbent materials to deliver reversible adsorption of ammonia (NH3) is a challenging task. Here, we report the efficient capture and storage of NH3 in a series of robust microporous aluminium-based metal-organic framework materials, namely MIL-160, CAU-10-H, Al-fum, and MIL-53(Al). In particular, MIL-160 shows high uptakes of NH3 of 4.8 and 12.8 mmol g−1 at both low and high pressure (0.001 and 1.0 bar, respectively) at 298 K. The combination of in situ neutron powder diffraction, synchrotron infrared micro-spectroscopy and solid-state nuclear magnetic resonance spectroscopy reveals the preferred adsorption domains of NH3 molecules in MIL-160, with H/D site-exchange between the host and guest and an unusual distortion of the local structure of [AlO6] moieties being observed. Dynamic breakthrough experiments confirm the excellent ability of MIL-160 to capture of NH3 with a dynamic uptake of 4.2 mmol g−1 at 1000 ppm. The combination of high porosity, pore aperture size and multiple binding sites promotes the significant binding affinity and capacity for NH3, which makes it a promising candidate for practical applications.	Mar 2023
I20-EDE-Energy Dispersive EXAFS (EDE)	Bimetallic aluminum- and niobium-doped MCM-41 for efficient conversion of biomass-derived 2-methyltetrahydrofuran to pentadienes Mengtian Fan , Shaojun Xu , Bing An , Alena M. Sheveleva , Alexander Betts , Joseph Hurd , Zhaodong Zhu , Meng He , Dinu Iuga , Longfei Lin , Xinchen Kang , Christopher M. A. Parlett , Floriana Tuna , Eric J. L. Mcinnes , Luke L. Keenan , Daniel Lee , Martin P. Attfield , Sihai Yang Angewandte Chemie International Edition DOI: 10.1002/anie.202212164 Diamond Proposal Number(s): [28575] Show Abstract ▼ Abstract: The production of conjugated C4-C5 dienes from biomass can enable the sustainable synthesis of many important polymers and liquid fuels. Here, we report the first example of bimetallic (Nb, Al)-atomically doped mesoporous silica, denoted as AlNb-MCM-41, which affords quantitative conversion of 2-methyltetrahydrofuran (2-MTHF) to pentadienes with a high selectivity of 91%. The incorporation of Al(III) and Nb(V) sites into the framework of AlNb-MCM-41 has effectively tuned the nature and distribution of Lewis and Brønsted acid sites within the structure. Operando X-ray absorption, diffuse reflectance infrared and solid-state NMR spectroscopy collectively reveal the molecular mechanism of the conversion of adsorbed 2-MTHF over AlNb-MCM-41. Specifically, the atomically-dispersed Nb(V) sites play an important role in binding 2-MTHF to drive the conversion. Overall, this study highlights the potential of hetero-atomic mesoporous solids for the manufacture of renewable materials.	Oct 2022
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
I11-High Resolution Powder Diffraction I20-EDE-Energy Dispersive EXAFS (EDE)	Control of zeolite microenvironment for propene synthesis from methanol Longfei Lin , Mengtian Fan , Alena M. Sheveleva , Xue Han , Zhimou Tang , Joseph H. Carter , Ivan Da Silva , Christopher Parlett , Floriana Tuna , Eric J. L. Mcinnes , German Sastre , Svemir Rudic , Hamish Cavaye , Stewart F. Parker , Yongqiang Cheng , Luke L. Daemen , Anibal J. Ramirez-Cuesta , Martin P. Attfield , Yueming Liu , Chiu C. Tang , Buxing Han , Sihai Yang Nature Communications 12 DOI: 10.1038/s41467-021-21062-1 Diamond Proposal Number(s): [2359] Open Access Show Abstract ▼ Abstract: Optimising the balance between propene selectivity, propene/ethene ratio and catalytic stability and unravelling the explicit mechanism on formation of the first carbon–carbon bond are challenging goals of great importance in state-of-the-art methanol-to-olefin (MTO) research. We report a strategy to finely control the nature of active sites within the pores of commercial MFI-zeolites by incorporating tantalum(V) and aluminium(III) centres into the framework. The resultant TaAlS-1 zeolite exhibits simultaneously remarkable propene selectivity (51%), propene/ethene ratio (8.3) and catalytic stability (>50 h) at full methanol conversion. In situ synchrotron X-ray powder diffraction, X-ray absorption spectroscopy and inelastic neutron scattering coupled with DFT calculations reveal that the first carbon–carbon bond is formed between an activated methanol molecule and a trimethyloxonium intermediate. The unprecedented cooperativity between tantalum(V) and Brønsted acid sites creates an optimal microenvironment for efficient conversion of methanol and thus greatly promotes the application of zeolites in the sustainable manufacturing of light olefins.	Feb 2021
B18-Core EXAFS I11-High Resolution Powder Diffraction	Quantitative production of butenes from biomass-derived γ-valerolactone catalysed by hetero-atomic MFI zeolite Longfei Lin , Alena M. Sheveleva , Ivan Da Silva , Christopher M. A. Parlett , Zhimou Tang , Yueming Liu , Mengtian Fan , Xue Han , Joseph H. Carter , Floriana Tuna , Eric J. L. Mcinnes , Yongqiang Cheng , Luke L. Daemen , Svemir Rudic , Anibal J. Ramirez-Cuesta , Chiu C. Tang , Sihai Yang Nature Materials 19, 86 - 93 DOI: 10.1038/s41563-019-0562-6 Diamond Proposal Number(s): [15151, 24726] Show Abstract ▼ Abstract: The efficient production of light olefins from renewable biomass is a vital and challenging target to achieve future sustainable chemical processes. Here we report a hetero-atomic MFI-type zeolite (NbAlS-1), over which aqueous solutions of γ-valerolactone (GVL), obtained from biomass-derived carbohydrates, can be quantitatively converted into butenes with a yield of >99% at ambient pressure under continuous flow conditions. NbAlS-1 incorporates simultaneously niobium(v) and aluminium(iii) centres into the framework and thus has a desirable distribution of Lewis and Brønsted acid sites with optimal strength. Synchrotron X-ray diffraction and absorption spectroscopy show that there is cooperativity between Nb(v) and the Brønsted acid sites on the confined adsorption of GVL, whereas the catalytic mechanism for the conversion of the confined GVL into butenes is revealed by in situ inelastic neutron scattering, coupled with modelling. This study offers a prospect for the sustainable production of butene as a platform chemical for the manufacture of renewable materials.	Dec 2019

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