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Elevated temperature-driven coordinative reconstruction of an unsaturated single-Ni-atom structure with low valency on a polymer-derived matrix for the electrolytic oxygen evolution reaction

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Nanoscale 2024年第15期16卷 7467-7479页

作者： Patil, Rahul Rajput, Anubha Matsagar, Babasaheb M. Chen, Norman C. R. Ujihara, Masaki Salunkhe, Rahul R. Yadav, Praveen Wu, Kevin C.-W. Chakraborty, Biswarup Dutta, Saikat Electrochemical Energy & Sensor Research Laboratory Amity Institute of Click Chemistry Research & Studies Amity University Noida India Department of Chemistry Indian Institute of Technology New Delhi India Department of Chemical Engineering National Taiwan University Taipei10617 Taiwan Molecular Science and Technology Program Taiwan International Graduate Program Academia Sinica Taiwan National Taiwan University Taiwan Graduate Institute of Applied Science and Technology National Taiwan University of Science and Technology Taipei Taiwan Materials Research Laboratory Department of Physics Indian Institute of Technology Jammu India Synchrotron X-ray Facility Raja Ramanna Centre for Advanced Technology Rajendra Nagar Madhya Pradesh 452013 Indore India

A high-temperature pyrolysis-controlled coordination reconstruction resulted in a single-Ni-atom structure with a Ni-Nx-C structural unit (x = N atom coordinated to Ni). Pyrolysis of Ni-phen@ZIF-8-RF at 700 °C resulted in NiNP-NC-700 with predominantly Ni nanoparticles. Upon elevating the pyrolysis temperature from 700 to 900 °C, a coordination reconstruction offers Ni-Nx atomic sites in NiSA-NC-900. A combined investigation with X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, and soft X-ray L3-edge spectroscopy suggests the stabilization of low-valent Niδ+ (0 −2 was achieved. The cell potential recorded with Pt(−)/(+)NiSA-NC-900/NF was much lower than that obtained for other cells, i.e., Pt(−)/NF and NF(−)/(+)NF, which enhances the potentials of low-valent NiSAs for insightful understanding of the OER. At a constant applied potential of 1.61 V (vs. RHE) for 12 h, an small increase in current for initial 0.6 h followed by a constant current depicts the fair stability of catalyst for 12 h. Our results offer an insightful angle into the OER with a coordinatively reconstructed single-Ni-atom structure at lower valency ( © 2024 The Royal Society of chemistry.

关键词： Reaction kinetics

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Active loading of cyanine 5.5 derivatives into liposomes for deep self-quenching and their applications in deep tissue imaging

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Sensors and Diagnostics 2024年第6期3卷 1028-1038页

作者： Chen, Chong-Yan Jian, Cheng-Bang Gao, Hua-De Yu, Xu-En Chang, Yuan-Chih Leong, Shwee Khuan Shie, Jiun-Jie Lee, Hsien-Ming Institute of Chemistry Academia Sinica Taipei 11529 Taiwan Nano Science and Technology Program Taiwan International Graduate Program Academia Sinica and National Taiwan University Taipei 11529 Taiwan Department of Chemistry National Taiwan University Taipei 10617 Taiwan Institute of Biological Chemistry Academia Sinica Taipei 11529 Taiwan Academia Sinica Cryo-EM Center Academia Sinica Taipei 11529 Taiwan Sustainable Chemical Science & Technology Taiwan International Graduate Program Academia Sinica Taipei 11529 Taiwan Department of Applied Chemistry National Yang Ming Chiao Tung University (NYCU) Hsinchu 30050 Taiwan

Visualizing liposome release profiles in small animals is important for evaluating the pharmacokinetic influence of vesicles. Encapsulating near-infrared (NIR) fluorescent dyes to visualize and report liposomal cargo release in vivo, which necessitates high encapsulation with deep self-quenching, is highly desirable in advanced (such as targeting or trigger-release) liposome development. However, passive loading of NIR dyes usually yields low encapsulation efficiencies (1-5%), causing significant wastage and cost-ineffectiveness while using expensive NIR fluorescent dyes. It would be highly beneficial if an active loading method, which typically has an encapsulation efficiency of nearly 100%, is developed. This research describes an active loading approach for two cyanine 5.5 (Cy5.5) derivatives. We discovered that using ammonium sucrose octasulfate (ASO) as a trapping agent allows for nearly 100% encapsulation for both Cy5.5 dyes, accompanied by the formation of nanoprecipitates inside the liposome, as evidenced by cryogenic electron microscopy. Fluorescence spectroscopy confirmed deep fluorescence self-quenching after active loading and a 60-100-fold fluorescence enhancement upon full content release via liposome rupture. Cellular uptake experiments showed that the fluorescence of Cy5.5-loaded liposomes recovered and plateaued after 9 hours of incubation with cells. In vivo fluorescence imaging (IVIS) demonstrated the same fluorescence activation in tumor-bearing mice intratumorally injected with the liposome. We believe that the developed active loading method will enable Cy5.5-loaded liposomes to be a deep tissue-compatible and cost-effective NIR fluorescence release-reporting platform. © 2024 RSC.

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Ordered and disordered stealthy hyperuniform point patterns across spatial dimensions

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Physical Review Research 2024年第3期6卷 033260页

作者： Peter K. Morse Paul J. Steinhardt Salvatore Torquato Department of Chemistry Department of Physics Princeton Institute of Materials Princeton Center for Theoretical Science Program in Applied and Computational Mathematics

In previous work [Phys. Rev. X 5, 021020 (2015)] it was shown that stealthy hyperuniform systems can be regarded as hard spheres in Fourier space in the sense that the structure factor is exactly zero in a spherical region around the origin in analogy with the pair-correlation function of real-space hard spheres. While this earlier work focused on spatial dimensions d=1–4, here we extend the analysis to higher dimensions in order to make connections to high-dimensional sphere packings and the mean-field theory of glasses. We exploit this correspondence to confirm that the densest Fourier-space hard-sphere system is that of a Bravais lattice in contrast to real-space hard spheres, whose densest configuration is conjectured to be disordered. In passing, we give a concise form for the position of the first Bragg peak. We also extend the virial series previously suggested for disordered stealthy hyperuniform systems to higher dimensions in order to predict spatial decorrelation as a function of dimension. This prediction is then borne out by numerical simulations of disordered stealthy hyperuniform ground states in dimensions d=2–8, which have only recently been made possible due to a highly parallelized algorithm.

关键词： Classical statistical mechanics Disordered systems

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Advances in data-independent acquisition mass spectrometry towards comprehensive digital proteome landscape

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Mass Spectrometry Reviews 2023年第6期42卷 2324-2348页

作者： Kitata, Reta Birhanu Yang, Jhih-Ci Chen, Yu-Ju Institute of Chemistry Academia Sinica Taipei Taiwan Sustainable Chemical Science and Technology Taiwan International Graduate Program Academia Sinica and National Yang Ming Chiao Tung University Taipei Taiwan Department of Applied Chemistry National Yang Ming Chiao Tung University Hsinchu Taiwan Department of Chemistry National Taiwan University Taipei Taiwan

The data-independent acquisition mass spectrometry (DIA-MS) has rapidly evolved as a powerful alternative for highly reproducible proteome profiling with a unique strength of generating permanent digital maps for retrospective analysis of biological systems. Recent advancements in data analysis software tools for the complex DIA-MS/MS spectra coupled to fast MS scanning speed and high mass accuracy have greatly expanded the sensitivity and coverage of DIA-based proteomics profiling. Here, we review the evolution of the DIA-MS techniques, from earlier proof-of-principle of parallel fragmentation of all-ions or ions in selected m/z range, the sequential window acquisition of all theoretical mass spectra (SWATH-MS) to latest innovations, recent development in computation algorithms for data informatics, and auxiliary tools and advanced instrumentation to enhance the performance of DIA-MS. We further summarize recent applications of DIA-MS and experimentally-derived as well as in silico spectra library resources for large-scale profiling to facilitate biomarker discovery and drug development in human diseases with emphasis on the proteomic profiling coverage. Toward next-generation DIA-MS for clinical proteomics, we outline the challenges in processing multi-dimensional DIA data set and large-scale clinical proteomics, and continuing need in higher profiling coverage and sensitivity. © 2022 The Authors. Mass Spectrometry Reviews published by John Wiley & Sons Ltd.

关键词： Mass spectrometry

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Sensing beyond the exceptional point for high detectivity

Sensing beyond the exceptional point for high detectivity

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CLEO: Science and Innovations in CLEO 2024, CLEO: S and I 2024 - Part of Conference on Lasers and Electro-Optics

作者： Li, Zhichao Prasad, Ciril S. Wang, Xielin Zhang, Ding Naik, Gururaj V. Applied Physics Graduate Program Smalley-Curl Institute Rice University HoustonTX77005 United States Department of Electrical and Computer Engineering Rice University HoustonTX77005 United States Department of Physics and Astronomy Rice University HoustonTX77005 United States

Exceptional point (EP)-based optical sensors exhibit exceptional sensitivity but poor detectivity. Slightly off EP operation boosts detectivity without much loss in sensitivity. We experimentally demonstrate a high-detectivity-off-EP plasmonic-photonic hybrid sensor for anti-mouse IgG protein. © Optica Publishing Group 2024

关键词： Hybrid sensors

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Sensing beyond the exceptional point for high detectivity

Sensing beyond the exceptional point for high detectivity

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2024 Conference on Lasers and Electro-Optics, CLEO 2024

ISBN: (纸本)9781957171395

关键词： Laser beams

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Physical limits on chemical sensing in bounded domains

arXiv

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arXiv 2024年

作者： McCusker, Daniel R. Lubensky, David K. Applied Physics Graduate Program University of Michigan United States Department of Physics University of Michigan United States

Cells respond to chemical cues, and the precision with which they can sense these cues is fundamentally limited by the stochastic nature of diffusion and ligand binding. Berg and Purcell famously investigated how well a small sensor in an infinite ligand bath can determine the ligand concentration, and a number of subsequent analyses have refined and built upon their classical estimates. Not all concentration sensing problems, however, occur in such an infinite geometry. At different scales, subcellular sensors and cells in tissues are both often confronted with signals whose diffusion is affected by confining boundaries. It is thus valuable to understand how basic limits on chemosensation depend on the sensor’s size and on its position in the domain in which ligand diffuses. Here we compute how sensor size and proximity to reflecting boundaries affect the diffusion-limited precision of chemosensation for various geometries in one and three dimensions. We derive analytical expressions for the sensing limit in these geometries. Among our conclusions is the surprising result that, in certain circumstances, smaller sensors can be more effective than larger sensors. This effect arises from a trade-off between spatial averaging and time averaging that we analyze in detail. We also find that proximity to confining boundaries can degrade a sensor’s precision significantly compared to the precision of the same sensor far from any boundaries. Copyright © 2024, The Authors. All rights reserved.

关键词： Ligands

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Data Independent Acquisition Mass Spectrometry Enhanced Personalized Glycosylation Profiling of Haptoglobin in Hepatocellular Carcinoma

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Journal of Proteome Research 2024年第8期23卷 3571-3584页

作者： Pradita, Tiara Chen, Yi-Ju Su, Tung-Hung Chang, Kun-Hao Chen, Pei-Jer Chen, Yu-Ju Institute of Chemistry Academia Sinica Taipei 115 Taiwan Taiwan International Graduate Program Academia Sinica Taipei 115 Taiwan Department of Applied Chemistry National Yang Ming Chiao Tung University Hsinchu 300 Taiwan Division of Gastroenterology and Hepatology Department of Internal Medicine National Taiwan University Hospital Taipei 100 Taiwan Hepatitis Research Center National Taiwan University Hospital Taipei 100 Taiwan Molecular Science and Technology Program Taiwan International Graduate Program Academia Sinica Taipei 115 Taiwan Department of Chemistry National Tsing-Hua University Hsinchu 300 Taiwan Graduate Institute of Clinical Medicine National Taiwan University College of Medicine Taipei 100 Taiwan Department of Medical Research National Taiwan University Hospital Taipei 100 Taiwan Department of Chemistry National Taiwan University Taipei 106 Taiwan

Aberrant glycosylation has gained significant interest for biomarker discovery. However, low detectability, complex glycan structures, and heterogeneity present challenges in glycoprotein assay development. Using haptoglobin (Hp) as a model, we developed an integrated platform combining functionalized magnetic nanoparticles and zwitterionic hydrophilic interaction liquid chromatography (ZIC-HILIC) for highly specific glycopeptide enrichment, followed by a data-independent acquisition (DIA) strategy to establish a deep cancer-specific Hp-glycosylation profile in hepatitis B virus (HBV, n = 5) and hepatocellular carcinoma (HCC, n = 5) patients. The DIA strategy established one of the deepest Hp-glycosylation landscapes (1029 glycopeptides, 130 glycans) across serum samples, including 54 glycopeptides exclusively detected in HCC patients. Additionally, single-shot DIA searches against a DIA-based spectral library outperformed the DDA approach by 2-3-fold glycopeptide coverage across patients. Among the four N-glycan sites on Hp (N-184, N-207, N-211, N-241), the total glycan type distribution revealed significantly enhanced detection of combined fucosylated-sialylated glycans, which were the most dominant glycoforms identified in HCC patients. Quantitation analysis revealed 48 glycopeptides significantly enriched in HCC (p < 0.05), including a hybrid monosialylated triantennary glycopeptide on the N-184 site with nearly none-to-all elevation to differentiate HCC from the HBV group (HCC/HBV ratio: 2462 ± 766, p < 0.05). In summary, DIA-MS presents an unbiased and comprehensive alternative for targeted glycoproteomics to guide discovery and validation of glyco-biomarkers. © 2024 The Authors. Published by American Chemical Society.

关键词： data-independent acquisition (DIA) glycoprotein haptoglobin hepatocellular carcinoma (HCC)

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High-definition microprint of metal-nanoparticles by optical vortex induced forward transfer

High-definition microprint of metal-nanoparticles by optical...

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2023 Conference on Lasers and Electro-Optics, CLEO 2023

作者： Kawaguchi, Haruki Takahashi, Kanta Wei, Rong Yamane, Keisaku Morita, Ryuji Yuyama, Ken-Ichi Kawano, Satoyuki Miyamoto, Katsuhiko Aoki, Nobuyuki Omatsu, Takashige Graduate School of Engineering Chiba University Japan Department of Applied Physics Hokkaido University Japan Department of Chemistry Osaka Metropolitan University Japan Graduate School of Engineering Science Osaka University Japan Molecular Chirality Research Center Chiba University Japan

We present the first demonstration of 2-dimensional direct-microprint of ultrafine circle metallic dots, consisting of close-packed gold nanoparticles, with ultrahigh definition by employing optical vortex induced for... 详细信息

ISBN: (纸本)9781957171258

关键词： Metal nanoparticles

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Field-driven cluster formation in two-dimensional colloidal binary mixtures

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Physical Review E 2023年第4期107卷 044605-044605页

作者： Dingwen Qian Monica Olvera de la Cruz Applied Physics Program Department of Materials Science and Engineering Department of Chemistry and Department of Physic and Astronomy Northwestern University Evanston Illinois 60208 USA

We study size- and charge-asymmetric oppositely charged colloids driven by an external electric field. The large particles are connected by harmonic springs, forming a hexagonal-lattice network, while the small particles are free of bonds and exhibit fluidlike motion. We show that this model exhibits a cluster formation pattern when the external driving force exceeds a critical value. The clustering is accompanied with stable wave packets in vibrational motions of the large particles.

关键词： Transport phenomena Charged colloids

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