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Instruments / Technical Area	Publication Details	Published	Actions
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

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