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Instruments / Technical Area	Publication Details	Published
B22-Multimode InfraRed imaging And Microspectroscopy I11-High Resolution Powder Diffraction	Trace benzene capture by decoration of structural defects in metal–organic framework materials Yu Han , Wenyuan Huang , Meng He , Bing An , Yinlin Chen , Xue Han , Lan An , Meredydd Kippax-Jones , Jiangnan Li , Yuhang Yang , Mark D. Frogley , Cheng Li , Danielle Crawshaw , Pascal Manuel , Svemir Rudic , Yongqiang Chen , Ian Silverwood , Luke L. Daemen , Anibal J. Ramirez-Cuesta , Sarah J. Day , Stephen P. Thompson , Ben F. Spencer , Marek Nikiel , Daniel Lee , Martin Schroeder , Sihai Yang Nature Materials 23, 1531 - 1538 DOI: 10.1038/s41563-024-02029-1 Diamond Proposal Number(s): [37155, 36474] Open Access Show Abstract ▼ Abstract: Capture of trace benzene is an important and challenging task. Metal–organic framework materials are promising sorbents for a variety of gases, but their limited capacity towards benzene at low concentration remains unresolved. Here we report the adsorption of trace benzene by decorating a structural defect in MIL-125-defect with single-atom metal centres to afford MIL-125-X (X = Mn, Fe, Co, Ni, Cu, Zn; MIL-125, Ti8O8(OH)4(BDC)6 where H2BDC is 1,4-benzenedicarboxylic acid). At 298 K, MIL-125-Zn exhibits a benzene uptake of 7.63 mmol g−1 at 1.2 mbar and 5.33 mmol g−1 at 0.12 mbar, and breakthrough experiments confirm the removal of trace benzene (from 5 to <0.5 ppm) from air (up to 111,000 min g−1 of metal–organic framework), even after exposure to moisture. The binding of benzene to the defect and open Zn(II) sites at low pressure has been visualized by diffraction, scattering and spectroscopy. This work highlights the importance of fine-tuning pore chemistry for designing adsorbents for the removal of air pollutants.	Nov 2024
B18-Core EXAFS I11-High Resolution Powder Diffraction	Efficient electrochemical reduction of nitrate to ammonia over metal-organic framework single-atom catalysts Lutong Shan , Yujie Ma , Shaojun Xu , Meng Zhou , Meng He , Alena M. Sheveleva , Rongsheng Cai , Daniel Lee , Yongqiang Chen , Boya Tang , Bing Han , Yinlin Chen , Lan An , Tianze Zhou , Martin Wilding , Alexander S. Eggeman , Floriana Tuna , Eric J. L. Mcinnes , Sarah J. Day , Stephen P. Thompson , Sarah J. Haigh , Xinchen Kang , Buxing Han , Martin Schroeder , Sihai Yang Communications Materials 5 DOI: 10.1038/s43246-024-00535-y Diamond Proposal Number(s): [33115, 31729] Open Access Show Abstract ▼ Abstract: The design and preparation of efficient catalysts for ammonia production under mild conditions is a desirable but highly challenging target. Here, we report a series of single-atom catalysts [M-SACs, M = Mn(II), Fe(III), Co(II), Ni(II), Cu(II), Zn(II), Mo(II)] derived from UiO-66 containing structural defects and their application to electrochemical reduction of nitrate (NO3-) to ammonia (NH3). Cu-SAC and Fe-SAC exhibit remarkable yield rates for NH3 production of 30.0 and 29.0 mg h−1 cm−2, respectively, with a high Faradaic efficiency (FENH3) of over 96% at −1.0 V versus the reversible hydrogen electrode. Importantly, their catalytic performance can be retained in various simulated wastewaters. Complementary experiments confirmed the nature of single-atom sites within these catalysts and the binding domains of NO3- in UiO-66-Cu. In situ spectroscopic techniques, coupled with density functional theory calculations confirm the strong binding of NO3- and the formation of reaction intermediates, thus facilitating the catalytic conversion to NH3.	Jun 2024
I19-Small Molecule Single Crystal Diffraction	Direct observation of enhanced iodine binding within a series of functionalized metal-organic frameworks with exceptional irradiation stability Jiangnan Li , Xinran Zhang , Mengtian Fan , Yinlin Chen , Yujie Ma , Gemma Smith , Inigo Vitórica-Yrezábal , Daniel Lee , Shaojun Xu , Martin Schroeder , Sihai Yang Journal Of The American Chemical Society DOI: 10.1021/jacs.4c02405 Diamond Proposal Number(s): [34413] Open Access Show Abstract ▼ Abstract: Optimization of active sites and stability under irradiation are important targets for sorbent materials that might be used for iodine (I2) storage. Herein, we report the direct observation of I2 binding in a series of Cu(II)-based isostructural metal–organic frameworks, MFM-170, MFM-172, MFM-174, NJU-Bai20, and NJU-Bai21, incorporating various functional groups (–H, −CH3, – NH2, –C≡C–, and −CONH–, respectively). MFM-170 shows a reversible uptake of 3.37 g g–1 and a high packing density of 4.41 g cm–3 for physiosorbed I2. The incorporation of −NH2 and –C≡C– moieties in MFM-174 and NJU-Bai20, respectively, enhances the binding of I2, affording uptakes of up to 3.91 g g–1. In addition, an exceptional I2 packing density of 4.83 g cm–3 is achieved in MFM-174, comparable to that of solid iodine (4.93 g cm–3). In situ crystallographic studies show the formation of a range of supramolecular and chemical interactions [I···N, I···H2N] and [I···C≡C, I–C═C–I] between −NH2, –C≡C– sites, respectively, and adsorbed I2 molecules. These observations have been confirmed via a combination of solid-state nuclear magnetic resonance, X-ray photoelectron, and Raman spectroscopies. Importantly, γ-irradiation confirmed the ultraresistance of MFM-170, MFM-174, and NJU-Bai20 suggesting their potential as efficient sorbents for cleanup of radioactive waste.	May 2024
B18-Core EXAFS I11-High Resolution Powder Diffraction	Direct synthesis of N‐formamides by integrating reductive amination of ketones and aldehydes with CO2 fixation in a metal‐organic framework Wenyaun Huang , Qingqing Mei , Shaojun Xu , Bing An , Meng He , Jiangnan Li , Yinlin Chen , Xue Han , Tian Luo , Lixia Guo , Joseph Hurd , Daniel Lee , Evan Tillotson , Sarah Haigh , Alex Walton , Sarah Day , Louise S. Natrjan , Martin Schroeder , Sihai Yang Chemistry – A European Journal DOI: 10.1002/chem.202303289 Open Access Show Abstract ▼ Abstract: Formamides are important feedstocks for the manufacture of many fine chemicals. State-of-the-art synthesis of formamides relies on the use of an excess amount of reagents, giving copious waste and thus poor atom-economy. Here, we report the first example of direct synthesis of N-formamides by coupling two challenging reactions, namely reductive amination of carbonyl compounds, particularly biomass-derived aldehydes and ketones, and fixation of CO2 in the presence of H2 over a metal-organic framework supported ruthenium catalyst, Ru/MFM-300(Cr). Highly selective production of N-formamides has been observed for a wide range of carbonyl compounds. Synchrotron X-ray powder diffraction reveals the presence of strong host-guest binding interactions via hydrogen bonding and parallel-displaced π···π interactions between the catalyst and adsorbed substrates facilitating the activation of substrates and promoting selectivity to formamides. The use of multifunctional porous catalysts to integrate CO2 utilisation in the synthesis of formamide products will have a significant impact in the sustainable synthesis of feedstock chemicals.	Oct 2023
B18-Core EXAFS	Direct conversion of methane to ethylene and acetylene over an iron-based metal–organic framework Yujie Ma , Xue Han , Shaojun Xu , Zhe Li , Wanpeng Lu , Bing An , Daniel Lee , Sarayute Chansai , Alena M. Sheveleva , Zi Wang , Yinlin Chen , Jiangnan Li , Weiyao Li , Rongsheng Cai , Ivan Da Silva , Yongqiang Cheng , Luke L. Daemen , Floriana Tuna , Eric J. L. Mcinnes , Lewis Hughes , Pascal Manuel , Anibal J. Ramirez-Cuesta , Sarah J. Haigh , Christopher Hardacre , Martin Schroeder , Sihai Yang Journal Of The American Chemical Society DOI: 10.1021/jacs.3c03935 Diamond Proposal Number(s): [19850] Open Access Show Abstract ▼ Abstract: Conversion of methane (CH4) to ethylene (C2H4) and/or acetylene (C2H2) enables routes to a wide range of products directly from natural gas. However, high reaction temperatures and pressures are often required to activate and convert CH4 controllably, and separating C2+ products from unreacted CH4 can be challenging. Here, we report the direct conversion of CH4 to C2H4 and C2H2 driven by non-thermal plasma under ambient (25 °C and 1 atm) and flow conditions over a metal–organic framework material, MFM-300(Fe). The selectivity for the formation of C2H4 and C2H2 reaches 96% with a high time yield of 334 μmol gcat–1 h–1. At a conversion of 10%, the selectivity to C2+ hydrocarbons and time yield exceed 98% and 2056 μmol gcat–1 h–1, respectively, representing a new benchmark for conversion of CH4. In situ neutron powder diffraction, inelastic neutron scattering and solid-state nuclear magnetic resonance, electron paramagnetic resonance (EPR), and diffuse reflectance infrared Fourier transform spectroscopies, coupled with modeling studies, reveal the crucial role of Fe–O(H)–Fe sites in activating CH4 and stabilizing reaction intermediates via the formation of an Fe–O(CH3)–Fe adduct. In addition, a cascade fixed-bed system has been developed to achieve online separation of C2H4 and C2H2 from unreacted CH4 for direct use. Integrating the processes of CH4 activation, conversion, and product separation within one system opens a new avenue for natural gas utility, bridging the gap between fundamental studies and practical applications in this area.	Sep 2023
	Humin formation on SBA-15-pr-SO3H catalysts during the alcoholysis of furfuryl alcohol to ethyl levulinate: effect of pore size on catalyst stability, transport, and adsorption Graziano Di Carmine , Costanza Leonardi , Luke Forster , Min Hu , Daniel Lee , Christopher M. A. Parlett , Olga Bortolini , Mark Isaacs , Alessandro Massi , Carmine D’agostino Acs Applied Materials & Interfaces DOI: 10.1021/acsami.3c04613 Open Access Show Abstract ▼ Abstract: Herein, the alcoholysis of furfuryl alcohol in a series of SBA-15-pr-SO3H catalysts with different pore sizes is reported. Elemental analysis and NMR relaxation/diffusion methods show that changes in pore size have a significant effect on catalyst activity and durability. In particular, the decrease in catalyst activity after catalyst reuse is mainly due to carbonaceous deposition, whereas leaching of sulfonic acid groups is not significant. This effect is more pronounced in the largest-pore-size catalyst C3, which rapidly deactivates after one reaction cycle, whereas catalysts with a relatively medium and small average pore size (named, respectively, C2 and C1) deactivate after two reaction cycles and to a lesser extent. CHNS elemental analysis showed that C1 and C3 experience a similar amount of carbonaceous deposition, suggesting that the increased reusability of the small-pore-size catalyst can be attributed to the presence of SO3H groups mostly present on the external surface, as corroborated by results on pore clogging obtained by NMR relaxation measurements. The increased reusability of the C2 catalyst is attributed to a lower amount of humin being formed and, at the same time, reduced pore clogging, which helps to maintain accessible the internal pore space.	May 2023
I11-High Resolution Powder Diffraction	Modulation of uptake and reactivity of nitrogen dioxide in metal-organic framework materials Zi Wang , Alena M. Sheveleva , Daniel Lee , Yinlin Chen , Dinu Iuga , W. Trent Franks , Yujie Ma , Jiangnan Li , Lei Li , Yongqiang Cheng , Luke L. Daemen , Sarah J. Day , Anibal J. Ramirez-Cuesta , Bing Han , Alexander S. Eggeman , Eric J. L. Mcinnes , Floriana Tuna , Sihai Yang , Martin Schroeder Angewandte Chemie International Edition DOI: 10.1002/anie.202302602 Open Access Show Abstract ▼ Abstract: We report the modulation of reactivity of nitrogen dioxide (NO2) in a charged metal-organic framework (MOF) material, MFM-305-CH3 in which unbound N-centres are methylated and the cationic charge counter-balanced by Cl− ions in the pores. Uptake of NO2 into MFM-305-CH3 leads to reaction between NO2 and Cl– to give nitrosyl chloride (NOCl) and NO3− anions. A high dynamic uptake of 6.58 mmol g−1 at 298 K is observed for MFM-305-CH3 as measured using a flow of 500 ppm NO2 in He. In contrast, the analogous neutral material, MFM-305, shows a much lower uptake of 2.38 mmol g−1. The binding domains and reactivity of adsorbed NO2 molecules within MFM-305-CH3 and MFM-305 have been probed using in situ synchrotron X-ray diffraction, inelastic neutron scattering and by electron paramagnetic resonance, high-field solid-state nuclear magnetic resonance and UV-vis spectroscopies. The design of charged porous sorbents provides a new platform to control the reactivity of corrosive air pollutants.	Apr 2023
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
B22-Multimode InfraRed imaging And Microspectroscopy I11-High Resolution Powder Diffraction	Control of the pore chemistry in metal-organic frameworks for efficient adsorption of benzene and separation of benzene/cyclohexane Yu Han , Yinlin Chen , Yujie Ma , Jamie Bailey , Zi Wang , Daniel Lee , Alena M. Sheveleva , Floriana Tuna , Eric J. L. Mcinnes , Mark D. Frogley , Sarah J. Day , Stephen P. Thompson , Ben F. Spencer , Marek Nikiel , Pascal Manuel , Danielle Crawshaw , Martin Schroeder , Sihai Yang Chem 359 DOI: 10.1016/j.chempr.2023.02.002 Diamond Proposal Number(s): [30398] Open Access Show Abstract ▼ Abstract: Benzene is an important air pollutant and a key chemical feedstock for the synthesis of cyclohexane. Because of the small difference of 0.6°C in their boiling points, the separation of benzene and cyclohexane is extremely challenging. Here, we report the high adsorption of benzene at low pressure and efficient separation of benzene/cyclohexane, achieved by the control of pore chemistry of two families of robust metal-organic frameworks, UiO-66 and MFM-300. At 298 K, UiO-66-CuII shows an exceptional adsorption of benzene of 3.92 mmol g−1 at 1.2 mbar and MFM-300(Sc) exhibits a high selectivity of 166 for the separation of benzene/cyclohexane (v/v = 1/1) mixture. In situ synchrotron X-ray diffraction and neutron powder diffraction, and multiple spectroscopic techniques reveal the binding mechanisms of benzene and cyclohexane in these materials. We also report the first example of direct visualization of reversible binding of benzene at an open Cu(II) site within metal-organic frameworks.	Feb 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] Open Access 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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