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113 items found (0 items not approved), displaying 1 to 10.[First/Prev] 1, 2, 3, 4, 5, 6, 7, 8 [Next/Last]

Instruments / Technical Area	Publication Details	Published
B22-Multimode InfraRed imaging And Microspectroscopy I11-High Resolution Powder Diffraction	Highly reversible and selective capture of trace SO2 in a scalable aluminum-based metal-organic framework Shan Dai , Longzhang Dong , Yinlin Chen , Jiangnan Li , Justyna Rogacka , Yuhang Yang , Zi Wang , Benjamin J. Moore , Daniel Lee , Yongqiang Cheng , Svemir Rudic , Bogdan Kuchta , Mark D. Frogley , Lucy Saunders , Martin Schroeder , Sihai Yang Journal Of The American Chemical Society 13 DOI: 10.1021/jacs.6c01974 Diamond Proposal Number(s): [39702, 41731] Show Abstract ▼ Abstract: The desulfurization of flue gas requires sorbents capable of selective and reversible SO2 capture. However, top-performing materials operate through either strong binding sites or the use of narrow pores, leading to difficulties in desorption and materials regeneration. Here, we report the efficient capture of trace SO2 using a robust and scalable aluminum-based metal–organic framework, MIL-120, which shows an exceptional SO2 uptake of 2.1 mmol g–1 at 2500 ppm and 298 K, coupled with optimal heats of adsorption (19–42 kJ mol–1) and fully reversible desorption at room temperature. Direct visualization of adsorbed SO2 molecules reveals host–guest and guest–guest interactions, collectively affording an SO2 packing density of 1.92 g cm–3, formally surpassing that of solid SO2 (1.62 g cm–3). Breakthrough experiments demonstrate that MIL-120 exhibits remarkable trace SO2 capture in the presence of dry or wet NO2 (another corrosive gas present in flue gas) with a record dynamic selectivity of 124, confirming the potential for MIL-120 to separate SO2/NO2 mixtures. This work sets a new benchmark for sorbent materials for reversible trace SO2 capture and separation.	Apr 2026
I11-High Resolution Powder Diffraction	A robust metal-organic framework with ‘molecular gates’ for efficient separation of ethane from ethylene Shao‐min Wang , Liping Zhang , Yitao Li , Ziluo Fang , Xue Han , Stephen P. Thompson , Qing‐yuan Yang , Sihai Yang Angewandte Chemie International Edition DOI: 10.1002/anie.6088623 Diamond Proposal Number(s): [42583] Open Access Show Abstract ▼ Abstract: Ethane-selective sorbents can enable single-step purification of ethylene but remain elusive to date. We report a Zn-based metal-organic framework (ZAI-3N) decorated with amino-based ‘molecular gates’ that exhibit highly selective adsorption of C2H6 over C2H4. Upon activation, ZAI-3N (zinc-adenine-3-aminoisonicotinic acid) features contractions of both Zn─N bonds and pores (from 2.009 to 1.914 Å and from 4.88 × 3.40 to 3.47 × 2.75 Å2, respectively). At 313 K and 1 bar, ZAI-3N exhibits an exceptional ratio of 10.6 for C2H6/C2H4 uptakes and a benchmark selectivity of 11.7, outperforming state-of-the-art porous solids. Synchrotron X-ray powder diffraction and modelling reveal that the methyl group in C2H6 can trigger amino rotation and facilitate gate opening, while π-electrons of C2H4 hinder such a process with a notably increased barrier (～5 and 11 kJ mol−1, respectively). Dynamic breakthrough experiments confirm the efficient separation of C2H6/C2H4 (v/v = 5/5 and 1/9), affording C2H4 with a high purity of 99.4% in single step with excellent recyclability and an C2H4 productivity of 10.3 mL g−1. This work demonstrates the judicious choice of ‘molecular gate’ as a promising protocol for challenging industrial gas separations.	Apr 2026
B18-Core EXAFS I11-High Resolution Powder Diffraction	Light-induced binding and reduction of CO2 over transient open Ce(III) sites in a metal-organic framework Shan Dai , Xiangdi Zeng , Benjamin J. Moore , Yuxiang Zhu , Yuhang Yang , Zi Wang , Luyan Li , Te Wang , Ivan Da Silva , Luke Keenan , Floriana Tuna , Daniel Lee , Sarah Day , Lucy Saunders , Martin Schroeder , Sihai Yang Journal Of The American Chemical Society DOI: 10.1021/jacs.5c20721 Show Abstract ▼ Abstract: Metal–organic framework (MOF) materials share some common features with metalloenzymes including site-isolated metal centers that template dynamic substrate activation within a functionalized cavity or pocket. We report the light-induced reversible binding of CO2 in a cerium-based MOF, Ce-UiO-66-NH2, incorporating an amino functionalized linker, which enables photoreduction of CO2 to CO in H2O without using sacrificial agents. A production rate for CO of 126 μmol·g–1·h–1 with 100% selectivity is observed, outperforming its non-amine analogue (Ce-UiO-66) and benchmark catalysts reported to date. In situ infrared, X-ray absorption, electron paramagnetic resonance and transient absorption spectroscopy reveal that photoexcitation induces a ligand-to-metal charge transfer to generate transient open Ce(III) sites that bind CO2 in a μ-(η1-O)(η1-C) binding mode. This binding is reversible and activates CO2 for subsequent photoreduction to CO. This work will promote the design of photocatalysts capable of synthesizing fuels from CO2.	Mar 2026
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
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
I19-Small Molecule Single Crystal Diffraction	Efficient capture and separation of xenon/krypton from off-gas by a radiation-resistant metal-organic framework Thien D. Duong , Jiangnan Li , Ruohan Li , Xin Lian , Yinlin Chen , Jiarui Fan , Joseph Hurd , Lixia Guo , Daniel Lee , Mark Warren , Sihai Yang Small 2013 DOI: 10.1002/smll.202508918 Diamond Proposal Number(s): [41123] Show Abstract ▼ Abstract: The capture of xenon (Xe) and krypton (Kr) from the off-gas of used nuclear fuel is of great importance to the treatment of radioactive wastes and production of high purity Xe. Solid sorbents, in particular metal–organic frameworks (MOFs), show promise in gas capture. However, the unknown radiation resistance of MOFs has limited their development. Herein, the efficient capture and separation of Xe/Kr by MFM-520, which strikes a remarkable stability toward 1750 kilogray (kGy) γ-irradiation, is reported. Under ambient conditions, dynamic breakthrough experiments confirm the efficient separation performance, yielding a Xe capacity of 66 and 0.2 mg g−1 from a by-product of air separation (Xe/Kr: 20/80; v/v) and off-gas (Xe/Kr: 400/40 ppm balance in air), respectively. In situ synchrotron X-ray single crystal diffraction and solid-state nuclear magnetic resonance (ssNMR) studies reveal that the optimal micropore of MFM-520 underpins specific host-guest interactions to Xe, resulting in selective Xe capture.	Oct 2025
I11-High Resolution Powder Diffraction	Exceptional electroreduction of nitrate to ammonia promoted by concerted electron-proton transfer in Cu-decorated MFI zeolites Lutong Shan , Tianxiang Chen , Shiyun Li , Boya Tang , Yuhang Yang , Peng Rao , Jiangnan Li , Ching Kit Tommy Wun , Daniel Lee , Mufan Li , Tsz Woon Benedict Lo , Sihai Yang Acs Applied Materials & Interfaces DOI: 10.1021/acsami.5c12561 Diamond Proposal Number(s): [37887] Show Abstract ▼ Abstract: The concerted electron–proton transfer (CEPT) can substantially enhance the microkinetics of electrocatalysis by circumventing the formation of high-energy intermediates. Herein, we report the decoration of the MFI zeolite matrix with isolated Cu(II) sites in the proximity of intrinsic Brønsted acid sites (BASs), promoting the CEPT synergy in electrocatalysis. By modulating the spatial arrangement of “Cu-BAS” pairs in Cu-Z(23) zeolite, we show a Faradaic efficiency of 98% for electroreduction of nitrate to ammonia, achieving an exceptional yield of 103.1 mg h–1 cm–2 at a current density of 1.3 A cm–2. Cu-Z(23) also exhibits an excellent activity at low concentrations of nitrate (e.g., 50 ppm) and a high catalytic stability of 50 h. Synchrotron X-ray powder diffraction, solid-state nuclear magnetic resonance spectroscopy, and modeling studies reveal the critical role of the proximate “Cu-BAS” pairs in facilitating the CEPT process. This approach uncovers the overlooked capability of “electrical insulating” zeolites as effective electrocatalysts to drive future sustainable chemical synthesis.	Sep 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
B22-Multimode InfraRed imaging And Microspectroscopy	Enhancing CO2 photoreduction efficiency through improved interaction enabled by a decorated covalent-organic framework Wenling Zhao , Jiangnan Li , Ke Li , Jiapeng Jiao , Shiqiang Liu , Jiahao Yang , Mark D. Frogley , Yaguang Peng , Yiyong Wang , Hengan Wang , Shipeng Zhang , Lihong Jing , Chengcheng Liu , Sihai Yang , Xinchen Kang , Buxing Han Angewandte Chemie International Edition 15 DOI: 10.1002/anie.202510550 Show Abstract ▼ Abstract: Photoreduction of CO2 is often hindered by the sluggish kinetics for its activation. Refinement of host–guest interactions is an effective strategy to overcome this barrier. Here, we report the immobilization of active Co(II) sites within a covalent-organic framework (COF) with a one-dimensional (1D) chain structure, Co-PyPDA-COF, which demonstrates a remarkable CO generation rate of 30.5 mmol g−1 h−1 and a high CO selectivity of 95.8% in 2 h for CO2 photoreduction at room temperature. The pore size of Co-PyPDA-COF is comparable to the diameter of CO2, which allows simultaneous interaction of a single CO2 molecule with the two Co(II) sites. The enhanced interaction result in increased local CO2 pressure, limited CO2 diffusion after adsorption, shortened distance for photoelectron transfer, and reduced energy barrier for the rate-determining step in CO2 reduction, promoting CO2 activation and conversion. This work opens a new way to design efficient catalysts by optimizing the pore size of the host.	Jul 2025

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