Search Results

You searched for all publications:

with publication states 'Published (Approved)'

Search Again...

These results only include publications that have been reviewed and processed by Diamond Light Source. To also view papers that have not yet been processed click here.

You can use the folder icon under Actions to collate papers as required. You can then click on View Folder in the left-hand navigation to review and/or download your folder.

Exact matches
Related results

9 items found (0 items not approved), displaying all items.1

Instruments / Technical Area	Publication Details	Published
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
B22-Multimode InfraRed imaging And Microspectroscopy	A flexible phosphonate metal-organic framework for enhanced cooperative ammonia capture Dukula De Alwis Jayasinghe , Yinlin Chen , Jiangnan Li , Justyna M. Rogacka , Meredydd Kippax-Jones , Wanpeng Lu , Sergey Sapchenko , Jinyue Yang , Sarayute Chansai , Tianze Zhou , Lixia Guo , Yujie Ma , Longzhang Dong , Daniil Polyukhov , Lutong Shan , Yu Han , Danielle Crawshaw , Xiangdi Zeng , Zhaodong Zhu , Lewis Hughes , Mark D. Frogley , Pascal Manuel , Svemir Rudic , Yongqiang Chen , Christopher Hardacre , Martin Schroeder , Sihai Yang Journal Of The American Chemical Society DOI: 10.1021/jacs.4c12430 Open Access Show Abstract ▼ Abstract: Ammonia (NH3) production in 2023 reached 150 million tons and is associated with potential concomitant production of up to 500 million tons of CO2 each year. Efforts to produce green NH3 are compromised since it is difficult to separate using conventional condensation chillers, but in situ separation with minimal cooling is challenging. While metal–organic framework materials offer some potential, they are often unstable and decompose in the presence of caustic and corrosive NH3. Here, we address these challenges by developing a pore-expansion strategy utilizing the flexible phosphonate framework, STA-12(Ni), which shows exceptional stability and capture of NH3 at ppm levels at elevated temperatures (100–220 °C) even under humid conditions. A remarkable NH3 uptake of 4.76 mmol g–1 at 100 μbar (equivalent to 100 ppm) is observed, and in situ neutron powder diffraction, inelastic neutron scattering, and infrared microspectroscopy, coupled with modeling, reveal a pore expansion from triclinic to a rhombohedral structure on cooperative binding of NH3 to unsaturated Ni(II) sites and phosphonate groups. STA-12(Ni) can be readily engineered into pellets or monoliths without losing adsorption capacity, underscoring its practical potential.	Nov 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
B22-Multimode InfraRed imaging And Microspectroscopy	High adsorption of ammonia in a titanium–based metal-organic framework Xiangbing Zeng , Jiangnan Li , Meng He , Wanpeng Lu , Danielle Crawshaw , Lixia Guo , Yujie Ma , Meredydd Kippax-Jones , Yongqiang Cheng , Pascal Manuel , Svemir Rudic , Mark D. Frogley , Martin Schroeder , Sihai Yang Chemical Communications DOI: 10.1039/D4CC01449A Diamond Proposal Number(s): [30398] Open Access Show Abstract ▼ Abstract: We report the high adsorption of NH3 in the titanium-based metal-organic framework, MFM-300(Ti), comprising extended [TiO6]∞ chains linked by biphenyl-3,3’,5,5’-tetracarboxylate ligands. At 273 K and 1 bar, MFM-300(Ti) shows an exceptional NH3 uptake of 23.4 mmol g–1 with a record-high packing density of 0.84 g cm–3. Dynamic breakthrough experiments confirm the excellent uptake and separation of NH3 at low concentration (1000 ppm). The combination of in situ neutron powder diffraction and spectroscopic studies reveal strong, yet reversible binding interactions of NH3 to the framework oxygen sites.	Apr 2024
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	Highly efficient proton conduction in the metal–organic framework material MFM-300(Cr)·SO4(H3O)2 Jin Chen , Qingqing Mei , Yinlin Chen , Christopher Marsh , Bing An , Xue Han , Ian P. Silverwood , Ming Li , Yongqiang Cheng , Meng He , Xi Chen , Weiyao Li , Meredydd Kippax-Jones , Danielle Crawshaw , Mark D. Frogley , Sarah J. Day , Victoria García-Sakai , Pascal Manuel , Anibal J. Ramirez-Cuesta , Sihai Yang , Martin Schroeder Journal Of The American Chemical Society DOI: 10.1021/jacs.2c04900 Diamond Proposal Number(s): [29649] Open Access Show Abstract ▼ Abstract: The development of materials showing rapid proton conduction with a low activation energy and stable performance over a wide temperature range is an important and challenging line of research. Here, we report confinement of sulfuric acid within porous MFM-300(Cr) to give MFM-300(Cr)·SO4(H3O)2, which exhibits a record-low activation energy of 0.04 eV, resulting in stable proton conductivity between 25 and 80 °C of >10–2 S cm–1. In situ synchrotron X-ray powder diffraction (SXPD), neutron powder diffraction (NPD), quasielastic neutron scattering (QENS), and molecular dynamics (MD) simulation reveal the pathways of proton transport and the molecular mechanism of proton diffusion within the pores. Confined sulfuric acid species together with adsorbed water molecules play a critical role in promoting the proton transfer through this robust network to afford a material in which proton conductivity is almost temperature-independent.	Jul 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

Publications Database

Search Results

You searched for all publications:

Search Again...

Subject Areas (check all that apply) select all

Instruments used to collect data (check all that apply) select all

Collaborations involved (check all that apply) select all

Diamond Offline Facilities used

Relevant Technical Areas (check all that apply) select all

Menu for Anonymous User