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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
I10-Beamline for Advanced Dichroism - scattering	Magnetic and EPR spectroscopic studies of heterometallic rings featuring {Cr6} chains and rare-earth metal centres Yuan Huang , Grigore A. Timco , George F. S. Whitehead , Selena J. Lockyer , Niklas Geue , Zhibo Qi , Adam Brookfield , Peter Bencok , Perdita E. Barran , Nicholas F. Chilton , Michael L. Baker , Eric J. L. Mcinnes , Richard E. P. Winpenny Inorganica Chimica Acta 31 DOI: 10.1016/j.ica.2025.123037 Diamond Proposal Number(s): [34857, 35250] Show Abstract ▼ Abstract: A rare example of a seven-membered heterometallic ring [CrIII6CeIIIF7(O2CtBu)14(THF)2] (MeCN)2 (1) and five eight-membered heterometallic rings, [nPr2NH2][CrIII6LnIII2F8(O2CtBu)17Lx] (2, Ln = Ce, L = HO2CtBu, x = 2, 3, Ln = Y, L = H2O, x = 1, 4, Ln = Gd, L = HO2CtBu, x = 1; 5, Ln = Tb, L = HO2CtBu, x = 1; 6, Ln = Yb, no L) have been synthesized and structurally characterized through X-ray diffraction. The structures consist of eight metals in an octagon, with Cr…Cr and Cr…Ln edges bridged by a fluoride and two carboxylates, while the Ln…Ln edges are bridged by a fluoride and three carboxylates. The magnetisation and susceptibility of these compounds were measured using SQUID magnetometry and electron paramagnetic resonance (EPR) spectroscopy. The magnetic data were fitted with antiferromagnetic exchange interactions between chromium(III) ions, which can be fitted in the {Cr6Y2} complex 3 and these parameters were then used to fit the magnetic properties of the {Cr6Gd2} complex 4 adding in exchange interactions between the CrIII and GdIII The magnetisation and susceptibility below 80 K of 1 and 2 were fitted on the basis of CASSCF-SO calculations at the CeIII site, and showed a weak ferromagnetic interaction between CrIII and CeIII. For 5 and 6 the magnetisation data was fitted by subtracting the data for 3 and treating the residual data as a {Tb2} and {Yb2} dimer respectively. The EPR spectra are rich, and for 3 can be modelled as due to S = 1 and S = 2 states of the {Cr6} chain. The spectra of 1 and 2 are similar, consistent with very weak interactions between the CeIII and the {Cr6} chain, while the spectra of 5 and 6 are different to that of 3, suggesting that the low temperature spectroscopy is due to a spin system in which the LnIII ions interact with the {Cr6} chain.	Dec 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
B18-Core EXAFS B22-Multimode InfraRed imaging And Microspectroscopy I11-High Resolution Powder Diffraction	Selective production of olefins from methanol over a heteroatomic SAPO-34 zeolite Zhaodong Zhu , Mengtian Fan , Meng He , Bing An , Yinlin Chen , Shaojun Xu , Tianze Zhou , Alena M. Sheveleva , Meredydd Kippax-Jones , Lutong Shan , Yongqiang Chen , Hamish Cavaye , Jeff Armstrong , Svemir Rudic , Stewart F. Parker , William Thornley , Evan Tillotson , Matthew Lindley , Shenglong Tian , Daniel Lee , Shiyu Fu , Mark D. Frogley , Floriana Tuna , Eric J. L. Mcinnes , Sarah J. Haigh , Sihai Yang Science Bulletin 149 DOI: 10.1016/j.scib.2024.12.050 Show Abstract ▼ Abstract: The methanol-to-olefins (MTO) process has the potential to bridge future gaps in the supply of sustainable lower olefins. Promoting the selectivity of propylene and ethylene and revealing the catalytic role of active sites are challenging goals in MTO reactions. Here, we report a novel heteroatomic silicoaluminophosphate (SAPO) zeolite, SAPO-34-Ta, which incorporates active tantalum(V) sites within the framework to afford an optimal distribution of acidity. SAPO-34-Ta exhibits a remarkable total selectivity of 85.8% for propylene and ethylene with a high selectivity of 54.9% for propylene on full conversion of methanol at 400 oC. In situ and operando synchrotron powder X-ray diffraction, diffuse reflectance infrared Fourier transform spectroscopy and inelastic neutron scattering, coupled with theoretical calculations, reveal trimethyloxonium as the key reaction intermediate, promoting the formation of first carbon-carbon bonds in olefins. The tacit cooperation between tantalum(V) and Brønsted acid sites within SAPO-34 provides an efficient platform for selective production of lower olefins from methanol.	Jan 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
I11-High Resolution Powder Diffraction	A novel cerium-based metal-organic framework supported Pd catalyst for semi-hydrogenation of phenylacetylene Xiangdi Zeng , Zi Wang , Meng He , Wanpeng Lu , Wenyuan Huang , Bing An , Jiangnan Li , Mufan Li , Ben F. Spencer , Sarah J. Day , Floriana Tuna , Eric J. L. Mcinnes , Martin Schroeder , Sihai Yang Inorganic Chemistry Frontiers DOI: 10.1039/D4QI02225D Diamond Proposal Number(s): [37155] Open Access Show Abstract ▼ Abstract: Phenylacetylene is a detrimental impurity in the polymerisation of styrene, capable of poisoning catalysts even at ppm levels and significantly degrading the quality of polystyrene. The semi-hydrogenation of phenylacetylene to styrene instead of ethylbenzene is, therefore, an important industrial process. We report a novel cerium(IV)-based metal-organic framework (denoted as Ce-bptc), which is comprised of {Ce6} clusters bridged by biphenyl-3,3’,5,5’-tetracarboxylate linkers. Ce-bptc serves as an ideal support for palladium nanoparticles and the Pd@Ce-bptc catalyst demonstrates an excellent catalytic performance for semi-hydrogenation of phenylacetylene, achieving a selectivity of 93% to styrene on full conversion under ambient conditions with excellent reusability. In situ synchrotron X-ray powder diffraction and electron paramagnetic resonance spectroscopy revealed the binding domain of phenylacetylene within Ce-bptc and details of the reaction mechanism.	Oct 2024
B22-Multimode InfraRed imaging And Microspectroscopy I15-1-X-ray Pair Distribution Function (XPDF)	High ammonia adsorption in copper-carboxylate materials: host-guest interactions and crystalline-amorphous-crystalline phase transitions Wanpeng Lu , Yinlin Chen , Zi Wang , Jin Chen , Yujie Ma , Weiyao Li , Jiangnan Li , Meng He , Mengtian Fan , Alena M. Sheveleva , Floriana Tuna , Eric J. L. Mcinnes , Mark D. Frogley , Philip A. Chater , Catherine Dejoie , Martin Schroder , Sihai Yang , Lixia Guo Chemical Communications DOI: 10.1039/D4CC02604G Open Access Show Abstract ▼ Abstract: The development of materials for ammonia (NH3) storage is an important and challenging task. Here, we report the high NH3 uptake in a series of copper-carboxylate materials, namely MFM-100, MFM-101, MFM-102, MFM-126, MFM-127, MFM-190(F), MFM-170, and Cu-MOP-1a. At 273 K and 1 bar, MFM-101 shows an exceptional uptake of 21.9 mmol g−1. X-ray pair distribution function analysis reveals an unusual crystalline-amorphous-crystalline phase transition for the isoreticular MFM-100, MFM-101 and MFM-102 upon adsorption and desorption of NH3 followed by regeneration in water. In situ X-ray diffraction, synchrotron infrared micro-spectroscopy, and electron paramagnetic resonance spectroscopy are employed to elucidate the presence of strong Cu(II)⋯NH3 interactions and changes in coordination at the [Cu2(O2CR)4] (R = di-, tri-, and tetra-phenyl ligands) paddlewheel.	Sep 2024
I19-Small Molecule Single Crystal Diffraction	One-, two- and three-dimensional interlocked polymers based on hybrid inorganic-organic rotaxanes Selena Lockyer , George F. S. Whitehead , Grigore A. Timco , Eric J. L. Mcinnes , Richard E. P. Winpenny Chemical Communications DOI: 10.1039/D4CC03566F Diamond Proposal Number(s): [31541] Open Access Show Abstract ▼ Abstract: We report three new polymers, based on mechanically interlocked inorganic-organic rotaxanes. They are made in very mild conditions and involve pyrimidine head groups binding to copper(II) linking units. A two-dimensional 6,3 net and a three-dimensional 10,3b net are found depending on the solvent used in the reaction.	Aug 2024
I19-Small Molecule Single Crystal Diffraction	Two- and three-spin hybrid inorganic-organic [2]rotaxanes containing metallated salen groups Richard Winpenny , Tom Bennett , Selena J. Lockyer , Deepak Asthana , George F. S. Whitehead , Iñigo J. Vitorica-Yrezabal , Grigore A. Timco , Eric J. L. Mcinnes Chemistry – An Asian Journal DOI: 10.1002/asia.202400641 Diamond Proposal Number(s): [31541] Show Abstract ▼ Abstract: Mono- and bis-salen functionalised [2]rotaxanes have been synthesised from the esterification of [2]rotaxanes containing phenol-terminated threads (salen = N,N′-bis(salicylidene)ethylenediamine). The [2]rotaxanes have general formula [RH][Cr7NiF8(O2CtBu)16], where [RH]+ is a thread with a central secondary ammonium site that templates a [Cr7NiF8(O2CtBu)16]− ring. The threads are terminated at one or both ends by carboxylic acid functionalised salen groups. The {M(salen)} groups can be free-base [M = (H+)2] or metallated [M = Cu2+, Ni2+, (VO)2+]. The [2]rotaxanes have been characterised by single crystal XRD and solid- and solution-state EPR spectroscopy. Where two paramagnetic M ions are involved [M = Cu2+ and/or (VO)2+] the [2]rotaxanes contain three electron spin S = ½ centres, since the {Cr7Ni} ring has an S = ½ ground state which is well isolated at low temperatures. These three-spin [2]rotaxanes have been characterised in solution by pulsed dipolar EPR spectroscopies (DEER, also known as PELDOR, and RIDME). The M···M and M···{Cr7Ni} interactions measured are consistent with dipolar interactions and also with the distances from single crystal XRD.	Jun 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

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