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42 items found (0 items not approved), displaying 1 to 10.[First/Prev] 1, 2, 3, 4, 5 [Next/Last]

Instruments / Technical Area	Publication Details	Published
B18-Core EXAFS I11-High Resolution Powder Diffraction	Ruthenium-loaded heteroatomic zeolite for selective hydrodeoxygenation reaction in aqueous medium Zhaodong Zhu , Xin Lian , Xue Han , Zi Wang , Siyu Zhou , Meng He , Tianze Zhou , Yuting Chen , Mengtian Fan , Wenyuan Huang , Yuhang Yang , Shaojun Xu , Yongqiang Cheng , Luke L. Daemen , Jeff Armstrong , Svemir Rudic , William Thornley , Evan Tillotson , Daniel Lee , Sarah Haigh , Shiyu Fu , Floriana Tuna , Eric J. L. Mcinnes , Sihai Yang Journal Of The American Chemical Society DOI: 10.1021/jacs.5c19607 Diamond Proposal Number(s): [37887, 31729, 36450] Show Abstract ▼ Abstract: Catalytic hydrodeoxygenation (HDO) is critical for bio-oil upgrading, yet the selective cleavage of stable C(sp2)–OH bonds in lignin-derived substrates under aqueous conditions remains a challenge. Here, we report a heteroatomic zeolite catalyst, RuFA/SAPO-34-Nb, featuring few-atom Ru clusters on a Nb(V)-modified SAPO-34 framework, which achieves highly efficient HDO of lignin-derived creosol (2-methoxy-4-methylphenol) in water. Under mild conditions (250 °C, 7 bar H2, 24 h), this catalyst delivers quantitative conversion of creosol to toluene (99.2% conversion, 99.6% selectivity), fully preserving the aromaticity of lignin-derived feedstocks─a key requirement for sustainable production of chemicals. Synchrotron X-ray diffraction, X-ray absorption spectroscopy, and inelastic neutron scattering, combined with theoretical modeling, elucidate the cooperative mechanism: the Nb(V) sites selectively cleave the strong C–O bonds, while the few-atom Ru cluster generates hydrogen species with an exceptionally low rotational barrier of 65 cm–1. This synergistic interaction enables the direct and selective HDO of C(sp2)–O bonds without saturation of the aromatic ring. This work establishes a promissing strategy for aqueous-phase HDO catalysis and provides a general approach for designing bimetallic zeolite catalysts to convert lignin-derived compounds to value-added aromatic chemicals, advancing sustainable biorefinery processes.	Jan 2026
I04-Macromolecular Crystallography	Ribonuclease toxin RelE1 inhibits growth of Mycobacterium tuberculosis through specific cleavage of the ribosomal anti-Shine-Dalgarno region Xue Han , Izaak N. Beck , Moise Mansour , Tom J. Arrowsmith , Roland Barriot , Paul Chansigaud , Carine Pagès , Hussein Hamze , Hatice Akarsu , Laurent Falquet , Peter Redder , Xibing Xu , Tim R. Blower , Pierre Genevaux Nucleic Acids Research 53 DOI: 10.1093/nar/gkaf1070 Diamond Proposal Number(s): [24948] Open Access Show Abstract ▼ Abstract: Toxin–antitoxin (TA) systems are central to bacterial immunity, genome maintenance, and pathogenicity. Toxins of TA systems use diverse strategies to control bacterial growth and represent attractive therapeutic targets to fight pathogens. In this work, we have investigated the toxic mechanism of the three RelE toxins of Mycobacterium tuberculosis, the bacterium responsible for tuberculosis in humans. Structural studies showed that RelBE1, RelBE2, and RelBE3 TA complexes share conserved structural motifs distinct from the RelBE complex of Escherichia coli. Although RelE homologs have previously been reported to perform ribosome-dependent messenger RNA (mRNA) cleavage, detection of cleavage products by nEMOTE demonstrated that only RelE3 targets mRNA. In contrast, in vitro and in vivo analyses using Mycobacterium smegmatis and M. tuberculosis revealed that RelE1 is a site-specific RNase, able to cleave 16S rRNA from free 30S and formed 70S ribosomes, to release the anti-Shine–Dalgarno region and prevent translation. This stunning mode of action, which is likely shared with RelE2, demonstrates that there is broader diversity for toxic mechanisms within the widespread RelE family.	Nov 2025
B18-Core EXAFS	Selective reductive amination of carbonyls to primary amines under ambient conditions over Rh/MFM-300(Cr) Qingqing Mei , Wenyuan Huang , Longfei Lin , Xue Han , Shaojun Xu , Bing An , Svemir Rudic , Rongsheng Cai , Sarah J. Haigh , Buxing Han , Martin Schroeder , Sihai Yang Angewandte Chemie International Edition DOI: 10.1002/anie.202519641 Diamond Proposal Number(s): [36450] Open Access Show Abstract ▼ Abstract: The synthesis of organic amines via reductive amination of biomass-derived carbonyl compounds is an important target for sustainable chemical industries. The control of selectivity for the formation of primary amines versus secondary amines is challenging, and high temperature and pressures using H2 are required to generate the desired selectivity. Herein, we report the highly selective reductive amination of a broad range of aldehydes and ketones by NH3 and H2 over Rh/MFM-300(Cr) to form primary amines with a selectivity of up to 99% under ambient conditions. Inelastic neutron scattering reveals that the Rh species not only promote the hydrogenation process, but also catalyzes the ammonolysis of the Schiff base intermediate, facilitating the selective synthesis of primary amines. This protocol achieves selective reductive amination at 25 °C and 1 atm, providing an energy-efficient route to a broad spectrum of amines.	Nov 2025
B18-Core EXAFS I20-EDE-Energy Dispersive EXAFS (EDE)	Synthesis of primary amines via reductive amination of aldehydes and ketones over a Ni-Doped MFM-300(Cr) catalyst Wenyuan Huang , Bing An , Zeyu Chen , Yu Han , Yinlin Chen , Jiangnan Li , Xue Han , Shaojun Xu , Danielle Crawshaw , Evan Tillotson , Sarah J. Haigh , Bing Han , Christopher M. A. Parlett , Luke Keenan , Svemir Rudic , Yongqiang Cheng , Ben F. Spencer , Martin Schroeder , Sihai Yang Advanced Science DOI: 10.1002/advs.202508892 Diamond Proposal Number(s): [28575, 31729] Open Access Show Abstract ▼ Abstract: The development of earth-abundant metal-based catalysts is an important goal for the synthesis of fine chemicals. Here, an active nickel catalyst supported on a robust metal–organic framework, MFM-300(Cr), is reported which shows an exceptional performance for reductive amination, a reaction that has long been dominated by noble metals. Ni/MFM-300(Cr) promotes the synthesis of 38 primary amines via reductive amination of their parent carbonyl compounds, including biomass-derived aldehydes and ketones, using NH3 in the presence of H2 operating under relatively mild conditions (5 bar and 160 °C). X-ray absorption spectroscopy confirms the formation of mixtures of metallic Ni0 and Nin+ active sites, while in situ inelastic neutron scattering, coupled with modeling, reveals details of the mechanism of catalysis involving the formation of N-benzyl-1-phenylmethanediamine (BPDI) as an intermediate species in the generation of benzylamine. Cooperativity between Ni sites and MFM-300(Cr) creates an optimal microenvironment for the efficient activation of carbonyl compounds and the selective production of primary amines using a non-precious metal-based catalyst.	Oct 2025
B18-Core EXAFS B22-Multimode InfraRed imaging And Microspectroscopy I11-High Resolution Powder Diffraction	Photocatalytic synthesis of hydrogen peroxide by rhenium modified metal-organic frameworks incorporating bianthracene ligands Boya Tang , David Brooks , Meng He , Yinlin Chen , Zhaozhao Hu , Xue Han , Jiangnan Li , Siyu Zhao , Jiarui Fan , Yukun Ye , Ivan Da Silva , Cheng Li , Zi Wang , Lutong Shan , Bing Han , Weiyao Li , Daniil Polyukhov , Bing An , Catherine Dejoie , Martin Wilding , Shaojun Xu , Meredydd Kippax-Jones , Zhaodong Zhu , Yujie Ma , Floriana Tuna , Eric J. L. Mcinnes , Sarah J. Day , Stephen P. Thompson , Mark D. Frogley , Louise S. Natrajan , Martin Schroeder , Sihai Yang Journal Of The American Chemical Society DOI: 10.1021/jacs.5c00603 Diamond Proposal Number(s): [37900, 37887, 36450] Show Abstract ▼ Abstract: Photocatalytic synthesis of hydrogen peroxide (H2O2) from oxygen (O2) is a challenging process. Metal–organic framework (MOF) materials are emerging photocatalysts with potential tunable light absorption properties. Herein, we report a rhenium (Re) modified Zr-based MOF, Re10-MFM-67, in which active Re sites are incorporated into MFM-67 by partial replacement of 9,9′-bianthracene-10,10′-dicarboxylic acid (H2L1) with a [(H2L2)ReI(CO)3Cl] (H2L2 = 2,2′-bipyridine-5,5′-dicarboxylic acid) moiety. Re10-MFM-67 (10 refers to the molar percentage content of Re complex within the material) exhibits broadband light absorption with an exceptional rate of formation of H2O2 from O2 of 8.50 mmol gcat–1 h–1 and a record turnover frequency (TOF) of 28.7 h–1 under visible light irradiation (λ > 400 nm). Synchrotron powder X-ray diffraction (SPXRD) and neutron powder diffraction (NPD) confirm the structure of Re10-MFM-67, and together with extended X-ray absorption fine structure (EXAFS) analysis establish the coordination environment and binding of the [ReI(CO)3Cl] moiety within the framework structure. In situ electron paramagnetic resonance (EPR) spectroscopy suggests that photocatalytic H2O2 generation on Re10-MFM-67 occurs via a two-step oxygen reduction reaction (ORR) pathway with the superoxide anion formed as an intermediate. This study promotes the design of MOF-based photocatalysts with conjugated ligands for efficient photosynthesis.	Jul 2025
I11-High Resolution Powder Diffraction	Hierarchical porous metal-organic polyhedra for efficient oxidative cleavage of β-O-4 bonds in lignin model compound Xinchen Kang , Lili Li , Hengan Wang , Tian Luo , Shaojun Xu , Yinlin Chen , Joseph H. Carter , Zi Wang , Alena M. Sheveleva , Kai Lyu , Xue Han , Floriana Tuna , Eric J. L. Mcinnes , Chiu C. Tang , Lifei Liu , Buxing Han , Emma K. Gibson , C. Richard A. Catlow , Sihai Yang , Martin Schroeder Ccs Chemistry DOI: 10.31635/ccschem.024.202404991 Diamond Proposal Number(s): [33115] Open Access Show Abstract ▼ Abstract: Catalytic cleavage of β-O-4 linkages is an essential but challenging step in the depolymerisation of lignin. Here, we report the templated electrosynthesis of a hydrophobic metal-organic polyhedral catalyst (Cu-MOP-e), which exhibits excellent hydrothermal stability and exceptional activity for this reaction. The oxidative cleavage of 2-phenoxyacetophenone, 1, a lignin model compound, over Cu-MOP-e at 90 oC for 1 h affords full conversion with yields of the monomer products phenol and benzoic acid of 99%. The reusability of Cu-MOP-e has been confirmed by carrying out ten cycles of reaction. The mechanism of catalyst-substrate binding has been investigated by high resolution synchrotron X-ray powder diffraction, in situ X-ray absorption spectroscopy, electron paramagnetic resonance spectroscopy and density functional theory calculations. The combination of optimal porosity and active Cu(II) sites provides confined binding of 2-phenoxyacetophenone, thus promoting the cleavage of β-O-4 linkage under relatively mild conditions.	Dec 2024
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
B22-Multimode InfraRed imaging And Microspectroscopy I11-High Resolution Powder Diffraction	Enhanced benzene adsorption in chloro-functionalized metal-organic frameworks Yu Han , David Brooks , Meng He , Yinlin Chen , Wenyuan Huang , Boya Tang , Bing An , Xue Han , Meredydd Kippax-Jones , Mark D. Frogley , Sarah J. Day , Stephen P. Thompson , Svemir Rudic , Yongqiang Chen , Luke L. Daemen , Anibal J. Ramirez-Cuesta , Catherine Dejoie , Martin Schroeder , Sihai Yang Journal Of The American Chemical Society DOI: 10.1021/jacs.4c07207 Diamond Proposal Number(s): [33115, 30398] Open Access Show Abstract ▼ Abstract: The functionalization of metal–organic frameworks (MOFs) to enhance the adsorption of benzene at trace levels remains a significant challenge. Here, we report the exceptional adsorption of trace benzene in a series of zirconium-based MOFs functionalized with chloro groups. Notably, MFM-68-Cl2, constructed from an anthracene linker incorporating chloro groups, exhibits a remarkable benzene uptake of 4.62 mmol g–1 at 298 K and 0.12 mbar, superior to benchmark materials. In situ synchrotron X-ray diffraction, Fourier transform infrared microspectroscopy, and inelastic neutron scattering, coupled with density functional theory modeling, reveal the mechanism of binding of benzene in these materials. Overall, the excellent adsorption performance is promoted by an unprecedented cooperation between chloro-groups, the optimized pore size, aromatic functionality, and the flexibility of the linkers in response to benzene uptake in MFM-68-Cl2. This study represents the first example of enhanced adsorption of trace benzene promoted by −CH···Cl and Cl···π interactions in porous materials.	Oct 2024
I19-Small Molecule Single Crystal Diffraction	Rapid extraction of trace benzene by a crown-ether-based metal-organic framework Zhonghang Chen , Peiyu Fang , Jiangnan Li , Xue Han , Wenhao Huang , Wenyue Cui , Zhiwei Liu , Mark R. Warren , David Allan , Peng Cheng , Sihai Yang , Wei Shi National Science Review DOI: 10.1093/nsr/nwae342 Diamond Proposal Number(s): [36394] Open Access Show Abstract ▼ Abstract: Due to almost identical boiling points of benzene and cyclohexane, the extraction of trace benzene from cyclohexane is currently performed via the energy-intensive extractive distillation method. Their adsorptive separation by porous materials is hampered by their similar dimensions. Metal-organic frameworks (MOFs) with versatile pore environments are capable of molecular discrimination, but the separation of trace substrates in liquid-phase remains extremely challenging. Herein, we report a robust MOF (NKU-300) with triangular channels decorated with crown ether that can discriminate trace benzene from cyclohexane, exhibiting an unprecedented selectivity of 8615(10) for the mixture of benzene/cyclohexane (v/v = 1/1000). Remarkably, NKU-300 demonstrates exceptional selectivities for the extraction of benzene from cyclohexane over a wide range of concentrations of 0.1%–50% with ultrafast sorption kinetics and excellent stability. Single-crystal X-ray diffraction and computational modelling reveal that multiple supramolecular interactions cooperatively immobilise benzene molecules in the triangular channel, enabling the superior separation performance. This study will promote the application of advanced sorbents with tailored binding sites for challenging industrial separations.	Oct 2024
I11-High Resolution Powder Diffraction	Binding of carbon dioxide and acetylene to free carboxylic-acid sites in a metal-organic framework Martin Schroeder , Christopher Marsh , Xue Han , Zhenzhong Lu , Ivan Da Silva , Yongqiang Chen , Luke L. Daemen , Sarah J. Day , Stephen P. Thompson , Anibal Javier Ramirez-Cuesta , Sihai Yang Chemical Science DOI: 10.1039/D4SC00101J Open Access Show Abstract ▼ Abstract: The functionalisation of organic linkers in metal-organic frameworks (MOFs) to improve gas uptake is well-documented. Although the positive role of free carboxylic acid sites in MOFs for binding gas molecules has been proposed in computational studies, relatively little experimental evidence has been reported in support of this. Primarily this is because of the inherent synthetic difficulty to prepare MOF materials bearing free, accessible –COOH moieties which would normally bind to metal ions within the framework structure. Here, we describe the direct binding of CO2 and C2H2 molecules to the free -COOH sites within the pores of MFM-303(Al). MFM-303(Al) exhibits highly selective adsorption of CO2 and C2H2 with a high selectivity for C2H2 over C2H4. In situ synchrotron X-ray diffraction and inelastic neutron scattering, coupled with modelling, highlight the cooperative interactions of adsorbed CO2 and C2H2 molecules with free -COOH and -OH sites within MFM-303(Al), thus rationalising the observed high selectivity for gas separation.	Apr 2024

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