B21-High Throughput SAXS
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Diamond Proposal Number(s):
[21035, 29470]
Open Access
Abstract: Advanced cell therapies require robust matrices for enhanced efficacy and delivery, but fabricating cell-specific hydrogels with strong tissue adhesiveness remains challenging. Cell membrane engineering offers a non-genetic strategy to modify cell surfaces and improve therapeutic properties. This study reports an artificial membrane-binding protein (AMBP), [cat.mTG(S)], that drives in situ formation of proteinaceous hydrogels on the plasma membrane of human dermal fibroblasts (HDFs). The AMBP is created by chemically supercharging (cationizing) microbial transglutaminase (mTG) and then electrostatically complexing it with an anionic polymer-surfactant (S). Biophysical studies confirm that this polymer surfactant complexation stabilizes the enzyme's structure and partially restores its activity lost during cationization. [cat.mTG(S)] effectively labels HDF plasma membranes with low cytotoxicity, unlike unmodified mTG (no binding) or cationized mTG (internalized). Live-cell confocal microscopy demonstrates that [cat.mTG(S)] on HDFs successfully cross-links external proteins into robust hydrogels extending beyond the cell surface and bridging cells, maintaining high cell viability. This AMBP provides a novel, non-genetic approach for localized, cell-surface engineering, enabling direct creation of protective and interactive hydrogel microenvironments for advanced cell-based therapies.
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Nov 2025
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I06-Nanoscience (XPEEM)
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Lingzhi
Wen
,
Cong
Li
,
Guanshihan
Du
,
Sijie
Wu
,
Jianbing
Zhang
,
Xiaoyin
Pan
,
Clodomiro
Cafolla
,
Lizhe
Hu
,
Yongjun
Wu
,
Zijian
Hong
,
Qing
He
,
Pu
Yu
Diamond Proposal Number(s):
[42042, 36503, 34602, 26142, 22361, 38419]
Abstract: Topological polar textures have garnered significant attention for next-generation electronic devices due to associated emergent functionalities (e.g., chirality, enhanced conductivity, and negative capacitance). Most studies stabilize topological textures using depolarization field in ferroelectric- dielectric superlattices or heterostructures; however, the lack of direct electrical contacts dramatically hinders the corresponding field-driven control and applications. Here, the formation of electric-field-switchable Néel-type polar skyrmions at room temperature is demonstrated in Ba0.8Sr0.2TiO3 (BSTO) thin films directly grown on metallic SrRuO3 electrodes. In this study, strategic Sr substitution is employed to engineer the Landau energy landscape of ferroelectric material BaTiO3, which eventually facilitates the coexistence of multiple polarization states without sacrificing room-temperature ferroelectricity. Piezoelectric force microscopy (PFM) uncovers a critical BSTO thickness to host the phenomena: conventional ferroelectric domains dominate 60-nm thick BSTO, whereas high-density topological polar textures emerge in 10-nm thick BSTO. Specifically, vector-PFM analysis identifies two stable skyrmion states in 10-nm BSTO with convergent- and divergent- in-plane polarization components. Importantly, an electric-field-driven interconversion between these topological states is demonstrated by reconfiguring the free-energy landscape, which is also supported by the phase-field simulations. This work provides a direct pathway of using metallic electrodes for the dynamic control of topological ferroelectrics in functional devices.
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Nov 2025
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I09-Surface and Interface Structural Analysis
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Diamond Proposal Number(s):
[29113]
Open Access
Abstract: LiNi0.5Mn1.5O4 (LNMO) cathodes offer a cobalt-free, high-voltage alternative to current state-of-the-art Li-ion battery cathodes, and are particularly well-suited for high-power applications due to their 3D lithium-ion pathways and structural stability. However, degradation of commercial electrolytes at high voltages exacerbates capacity decay, as instability at the cathode surface causes active material loss, surface reconstructions, thickening surface layers, and increases in internal cell resistance. Cationic substitution has been proposed to enhance surface stability, thus limiting capacity decay. Here, we demonstrate the stabilizing effect of Mg on the LNMO cathode surface, which is most evident during the early stages of cycling. This study indicates that improved O 2p-TM 3d hybridization in Mg-substituted LNMO, facilitated by Li-site defects, leads to the formation of a stable surface layer that is corrosion-resistant at high voltage. Examination of Fe-substituted and unsubstituted LNMO further confirms that the surface stability is uniquely enabled by Mg substitution. This work offers valuable insights into surface design for reducing degradation in high-voltage spinel cathodes.
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Nov 2025
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B07-B1-Versatile Soft X-ray beamline: High Throughput ES1
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Diamond Proposal Number(s):
[35956]
Abstract: Electrocatalytic water splitting is a sustainable route to high-purity hydrogen, yet its efficiency is hindered by the sluggish kinetics of the oxygen evolution reaction (OER). Replacing OER with the thermodynamically favorable ammonia oxidation reaction (AOR) significantly reduces the energy input required for hydrogen production while simultaneously addressing ammonia utilization. However, progress is limited by the need for expensive noble metal catalysts like PtIr/C and the poor performance of non-noble alternatives. Herein, a series of perovskite oxide catalysts is reported with tunable B-site configurational entropy. Among them, the high-entropy La0.7Sr0.3(Ni0.2Cu0.2Co0.2Mn0.2Fe0.2)O3-δ (LS5B) catalyst demonstrates exceptional activity and stability for the ammonia-water co-oxidation reaction (AWOR), outperforming lower-entropy analogs. The enhanced performance is attributed to its entropy-stabilized structure, which generates abundant surface oxygen vacancies and suppresses atomic diffusion, increasing both active site density and structural durability. Density functional theory (DFT) calculations reveal that the high-entropy configuration lowers the energy barrier for ammonia adsorption and facilitates intermediate formation. In a practical ammonia-water co-electrolyzer, LS5B delivers a current density of 2.6 A·cm−2 at 2.0 V, surpassing PtIr/C and representing the best performance to date. A stable operation over 90 h at ampere-level current demonstrates LS5B's potential for scalable, efficient green hydrogen production via ammonia-water co-electrolysis.
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Nov 2025
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I15-1-X-ray Pair Distribution Function (XPDF)
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Diamond Proposal Number(s):
[31642]
Open Access
Abstract: Metal–organic framework (MOF) glasses combine the structural tunability of crystalline MOFs with the processability of amorphous materials, offering exciting opportunities for functional hybrid materials. Here, a one-pot, solvent-free synthesis is reported of an Fe2+-based MOF glass, gFe-tBubipy, with the composition [Fe2(im)3.12(bim)0.88(tBubipy)0.11]·[Fe(Cp)2]0.09 (im− = imidazolate, bim− = benzimidazolate, tBubipy = 4,4′-di-tert-butyl-2,2′-bipyridine, Cp− = cyclopentadienyl anion). This material forms a continuous random network structure of four-connected tetrahedral and octahedral Fe2+ nodes and exhibits an exceptionally low glass transition temperature (Tg = 87 °C). Despite its amorphous nature and complex composition, gFe-tBubipy exhibits a high degree of local structural order that enables strong antiferromagnetic exchange interactions between Fe2+ centers. Remarkably, it exhibits clear signatures of spin-glass behavior, with a well-defined magnetic freezing transition ≈14 K. This combination of a MOF glass exhibiting a distinct glass transition with spin-glass magnetism arising from topological disorder and frustrated, short-range magnetic interactions represent a significant advance. This discovery underscores the transformative potential of MOF glasses as a versatile platform for exploring the interplay between structural disorder and cooperative magnetic phenomena in hybrid materials.
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Aug 2025
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B07-B1-Versatile Soft X-ray beamline: High Throughput ES1
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Mark A.
Isaacs
,
Charalampos
Drivas
,
Arthur
Graf
,
Sasha
Kroon
,
Santosh
Kumar
,
Junxi
Liu
,
Antonio
Torres‐lopez
,
Cameron
Price
,
Edward
Garland
,
Ines
Lezcano-Gonzalez
,
Christopher M. A.
Parlett
,
Vannia C.
Dos Santos-Durndell
,
Lee J.
Durndell
Diamond Proposal Number(s):
[40403]
Open Access
Abstract: 2.5% of global carbon emissions result from air travel, underscoring the need for sustainable aviation fuels (SAF) derived from second-generation lignocellulosic biomass to enhance the green credentials of the aviation sector. This study demonstrates the first solvent-free photocatalytic conversion of furfural (FAL) and cyclopentanone (CPO) to produce 2,5-bis(2-furylmethylidene)cyclopentanone (F2Cp), a jet fuel precursor, using Ti-SBA-15 catalysts, synthesized via alkoxide grafting and controlled titanium surface coverage. Sub-monolayer titania films on SBA-15 supports are achieved with tuneable Ti content, confirmed by XPS (X-ray photoelectron spectroscopy), UPS (ultraviolet photoelectron spectroscopy), REELS (reflectance electron energy loss spectroscopy), ISS (ion scattering spectroscopy), and Raman analysis. XPS analyses reveal coverage-dependent Ti speciation, transitioning from isolated Ti atoms to interconnected Ti-O-Ti networks, with corresponding shifts in Auger parameters, indicating increased surface polarizability and Lewis acidity. Optimized Ti-SBA-15 catalysts exhibit a fourfold activity enhancement in photocatalytic activity over bulk TiO₂, attributed to improved mass transport, active site accessibility, and surface stability. This work highlights the potential of rationally designed hierarchical catalysts for scalable, energy-efficient biomass valorization into SAF precursors, offering a scalable, energy-efficient pathway for sustainable jet fuel production. By elucidating the structure-function relationships in sub-monolayer Ti-SBA-15 materials, this study provides critical insights for advancing photocatalytic technologies in renewable energy applications.
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Jul 2025
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I10-Beamline for Advanced Dichroism - scattering
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Hetian
Chen
,
Xiaofu
Qiu
,
Zenghui
Jin
,
Dingsong
Jiang
,
Ting
Lin
,
Yujun
Zhang
,
Yuhan
Liang
,
Xiaoyu
Jiang
,
Yiming
Yang
,
Chao
Li
,
Fangyuan
Zhu
,
Jing
Ma
,
Qinghua
Zhang
,
Jheng-Cyuan
Lin
,
Qing
He
,
Yuanhua
Lin
,
Tianxiang
Nan
,
Di
Yi
Abstract: Magnon spin current, which delivers spin angular momentum without charge flow, has garnered considerable interest for next-generation spintronic applications. Antiferromagnetic insulators have been shown to be the ideal material platform for magnonics. However, it remains a challenge to effectively control the antiferromagnetic magnon transport. Here, the control over both transmissivity and anisotropy of antiferromagnetic magnon transport in magnetic multilayers is reported, achieved through the delicate interplay between interfacial coupling and magnetocrystalline anisotropy. In La0.7Sr0.3MnO3 (LSMO)/LaFeO3 (LFO)/Pt heterostructures, a Néel vector reorientation as temperature decreases is observed through soft X-ray magnetic linear dichroism. Temperature- and angular-dependent spin pump data reveal three regions with distinct antiferromagnetic magnon transport characteristics, evolving from a magnon-conducting state with uniaxial anisotropy to an intermediate state with reduced transmissivity and weak anisotropy, and ultimately to a magnon-insulating state. Theoretical modeling reveals that this modulation is likely attributed to the evolution of both antiferromagnetic axis and domain structure of LFO, determined by the competition between exchange coupling across the interface and the intrinsic magnetic anisotropy of LFO. These findings provide fundamental insights into the critical role of the interface in controlling the magnon transport in magnetic multilayers and offer a new toolkit for developing magnonic devices.
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Jul 2025
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B23-Circular Dichroism
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Martyna
Wasiluk
,
Claire
Goldmann
,
Maciej
Bagiński
,
Mateusz
Pawlak
,
Pawel W.
Majewski
,
Julia
Abramowicz
,
Piotr
Roszkowski
,
Lukas
Rebholz
,
Carsten
Rockstuhl
,
Cyrille
Hamon
,
Wiktor
Lewandowski
Open Access
Abstract: Thin films exhibiting plasmonic circular dichroism (PCD) represent a promising class of materials for technologies based on light processing. However, their potential is limited by the relatively low selectivity of interactions with circularly polarized photons of a given handedness and restricted tunability of the chiroptical properties. This article aims to resolve these problems with two innovations. First, it assembles gold nanobipyramids (NBPs), a promising building block for plasmonics, and arrange them in helical assemblies using a liquid-crystalline (LC) template. By optimizing the organic coating of NBPs, their size, and loading in the thin film, it achieves PCD films with state-of-the-art dissymmetry, g-factor on the order of 10−2. This study unequivocally evidence the properties by Mueller Matrix polarimetry and identify plasmonic coupling between particles as the driving force for the origin of the PCD properties using T-matrix theoretical modeling. Second, spectral and dynamic PCD engineering is achieved by varying particle sizes, co-assembling NBPs with nanospheres, and reversible melting and crystallization of the thin film. Overall, this work unlocks the potential of NBPs and binary assemblies based on NBPs for chiral plasmonics, providing a strategy for thin film materials displaying spectral and temporal PCD response with high dissymmetry factors.
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Jun 2025
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B18-Core EXAFS
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Weifeng
Su
,
Tao‐jing
Huang
,
Haoliang
Huang
,
Zhipeng
Yu
,
Fei
Lin
,
Chenyue
Zhang
,
Hao
Tan
,
Kaiyang
Xu
,
Run
Ran
,
Weimian
Zhang
,
Yaowen
Xu
,
Chao
Song
,
Guang-Jie
Xia
,
Zuxin
Chen
,
Lifeng
Liu
Diamond Proposal Number(s):
[36104]
Open Access
Abstract: Direct seawater electrolysis for hydrogen production is hindered by high energy consumption and the competing chlorine evolution reaction (CER), which compromises efficiency and generates corrosive byproducts. Replacing oxygen evolution reaction (OER) with sulfion oxidation reaction (SOR) is promising to circumvent CER, but practical applications demand high-efficiency powdery, supported SOR catalysts operating at high current densities. Herein, we report the synthesis of FeCoNiMnCuO high-entropy oxide nanoparticles (HEO NPs) supported on carbon through an ultrafast Joule-heating method, which show outstanding SOR performance in natural seawater, achieving 500 mA cm⁻2 at 0.545 V versus the reversible hydrogen electrode and demonstrating stability over 100 h. Operando X-ray absorption spectroscopy and in-situ Raman spectroscopy studies reveal that in-situ formed metal sulfides, particularly Fe−S and Cu−S species, serve as active sites. Density functional theory calculations confirm the high-entropy effect lowers the energy cost of the potential-determining step by increasing intrinsic charge stability. Furthermore, a membrane electrode assembly incorporating the HEO catalysts operates stably at 500 mA cm⁻2 over 500 h with low energy consumption and no chlorine evolution, showcasing substantial potential for low-cost, energy-saving, and chlorine-free hydrogen production from seawater.
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Jun 2025
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B18-Core EXAFS
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Mei
Han
,
Jieshu
Zhou
,
Shaojun
Xu
,
Honggang
Sun
,
Xin
Zi
,
Ning
Wang
,
Jingrui
Han
,
Weijia
Zhou
,
Haibin
Wang
,
Kangning
Liu
,
Emiliano
Cortés
,
Songhua
Chen
,
Mingchuan
Luo
,
Jieqiong
Shan
,
Min
Liu
,
Ziyun
Wang
,
Hongyan
Liang
,
Yongchang
Liu
Diamond Proposal Number(s):
[19850]
Abstract: Neutral water electrolysis faces challenges due to insufficient OH− supply, which leads to inefficient oxygen evolution reaction (OER). Constructing a localized OH−-enriched reaction environment is crucial for enhancing the neutral OER activity. Here, an integrated catalyst design aimed at optimizing the local reaction environment is presented to improve catalytic activity. Specifically, a high-curvature needle morphology is constructed to strengthen the local electric field, which induces localized OH− accumulation and mitigates OH− deficiency in the neutral electrolyte. Moreover, implanting Ag cores not only improves the conductivity and long-term stability of the NiCo-based catalytic shells but also enables Ag diffusion to dope the catalytic layer. At the atomic scale, Ag dopants modify the activity of oxygen ligands and the polarity of metal-oxygen (M─O) bonds within the symmetric spinel structure. This modification facilitates surface reconstruction, resulting in the formation of a distorted Ag-O-Ni/Co-OH network. The elongation of the Ni/Co−O bond generates an inhomogeneous charge distribution that optimizes water polarization and deprotonation, accelerating water dissociation and *OH formation. The multiscale catalyst design results in a unique interface featuring a high-curvature surface and atomic-scale polarized M─O networks, synergistically enhancing local *OH accumulation. Therefore, the optimal Ag@NiCo2O4 catalyst delivers a η10 = 295 mV in an H-cell electrolyzer and 2.1 V @1 A cm−2 in a membrane electrode assembly electrolyzer. This finding provides a practical design for OER electrocatalysts in neutral electrolytes and opens a new avenue for optimizing catalytic performance by integrating multiple strategies.
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May 2025
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