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Bio-Templated Chiral Zeolitic Imidazolate Framework for Enantioselective Chemoresistive Sensing

Angewandte Chemie 2023年第30期135卷

作者： Minkyu Kim Moon Jong Han Hansol Lee Paraskevi Flouda Daria Bukharina Kellina J. Pierce Katarina M. Adstedt Madeline L. Buxton Young Hee Yoon William T. Heller Srikanth Singamaneni Vladimir V. Tsukruk School of Materials Science & Engineering Georgia Institute of Technology Atlanta GA 30332 USA Contribution: Conceptualization (equal) Data curation (lead) Validation (lead) Visualization (lead) Writing - original draft (lead) Writing - review & editing (equal) Contribution: Conceptualization (supporting) Data curation (supporting) Formal analysis (supporting) Visualization (supporting) Contribution: Data curation (supporting) Investigation (supporting) Contribution: Investigation (supporting) School of Chemical & Biomolecular Engineering Georgia Institute of Technology Atlanta GA 30332 USA Neutron Scattering Division Oak Ridge National Laboratory Oak Ridge TN 37831 USA Contribution: Investigation (supporting) Validation (supporting) Department of Mechanical Engineering and Materials Science Institute of Materials Science and Engineering Washington University in St. Louis St Louis MO 63130 USA Contribution: Conceptualization (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (supporting) Funding acquisition (lead) Investigation (supporting) Project administration (lead) Writing - original draft (supporting) Writing - review & editing (equal)

Chiral metal–organic frameworks (MOFs) have gained rising attention as ordered nanoporous materials for enantiomer separations, chiral catalysis, and sensing. Among those, chiral MOFs are generally obtained through complex synthetic routes by using a limited choice of reactive chiral organic precursors as the primary linkers or auxiliary ligands. Here, we report a template-controlled synthesis of chiral MOFs from achiral precursors grown on chiral nematic cellulose-derived nanostructured bio-templates. We demonstrate that chiral MOFs, specifically, zeolitic imidazolate framework (ZIF), unc -[Zn(2-MeIm) 2 , 2-MeIm=2-methylimidazole], can be grown from regular precursors within nanoporous organized chiral nematic nanocelluloses via directed assembly on twisted bundles of cellulose nanocrystals. The template-grown chiral ZIF possesses tetragonal crystal structure with chiral space group of P 4 1 , which is different from traditional cubic crystal structure of I -43 m for freely grown conventional ZIF-8. The uniaxially compressed dimensions of the unit cell of templated ZIF and crystalline dimensions are signatures of this structure. We observe that the templated chiral ZIF can facilitate the enantiotropic sensing. It shows enantioselective recognition and chiral sensing abilities with a low limit of detection of 39 μM and the corresponding limit of chiral detection of 300 μM for representative chiral amino acid, D- and L- alanine.

关键词： Chiral bio-templates chiral metal–organic frameworks enantioselective chemoresistive sensors

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Neutron Scattering Signature of Phonon Renormalization in Nickel (II) Oxide

arXiv

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arXiv 2021年

作者： Sun, Qiyang Wei, Bin Su, Yaokun Smith, Hillary Lin, Jiao Y.Y. Abernathy, Douglas L. Li, Chen Department of Mechanical Engineering University of California Riverside RiversideCA92521 United States Materials Science and Engineering University of California Riverside RiversideCA92521 United States Henan Key Laboratory of Materials on Deep-Earth Engineering School of Materials Science and Engineering Henan Polytechnic University Jiaozuo454000 China Department of Physics and Astronomy Swarthmore College SwarthmorePA19081 United States Neutron Data Analysis and Visualization Division Oak Ridge National Laboratory Oak RidgeTN37830 United States Neutron Scattering Division Oak Ridge National Laboratory Oak RidgeTN37830 United States

The physics of mutual interaction of phonon quasiparticles with electronic spin degrees of freedom, leading to unusual transport phenomena of spin and heat, has been a subject of continuing interests for decades. Despite its pivotal role in transport processes, the effect of spin-phonon coupling on the phonon system, especially acoustic phonon properties, has so far been elusive. By means of inelastic neutron scattering and first-principles calculations, anomalous scattering spectral intensity from acoustic phonons was identified in the exemplary collinear antiferromagnetic nickel (II) oxide, unveiling strong spin-lattice correlations that renormalize the polarization of acoustic phonon. In particular, a clear magnetic scattering signature of the measured neutron scattering intensity from acoustic phonons is demonstrated by its momentum transfer and temperature dependences. The anomalous scattering intensity is successfully modeled with a modified magneto-vibrational scattering cross section, suggesting the presence of spin precession driven by phonon. The renormalization of phonon eigenvector is indicated by the observed "geometry-forbidden" neutron scattering intensity from transverse acoustic phonon. Importantly, the eigenvector renormalization cannot be explained by magnetostriction but instead, it could result from the coupling between phonon and local magnetization of ions. Copyright © 2021, The Authors. All rights reserved.

关键词： Eigenvalues and eigenfunctions

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High-Performance Thermoelectric α-Ag9Ga1−xTe6Compounds with Ultralow Lattice Thermal Conductivity Originating from Ag9Te2Motifs

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Angewandte Chemie 2022年第36期134卷

作者： Yingfei Tang Yimeng Yu Na Zhao Keke Liu Haijie Chen Constantinos C. Stoumpos Yixuan Shi Shuo Chen Lingxiao Yu Jinsong Wu Qingjie Zhang Xianli Su Xinfeng Tang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China International School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 China Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Investigation (equal) Methodology (equal) Visualization (equal) Writing - original draft (lead) Nanostructure Research Center Wuhan University of Technology Wuhan 430070 China Contribution: Data curation (equal) Software (equal) Visualization (supporting) Contribution: Investigation (equal) Methodology (equal) Contribution: Investigation (equal) Methodology (equal) Visualization (equal) State Key Laboratory for Modification of Chemical Fibers and Polymer Materials Institute of Functional Materials College of Materials Science and Engineering Donghua University Shanghai 201620 China Contribution: Methodology (equal) Visualization (equal) Writing - review & editing (equal) Department of Materials Science and Technology Voutes Campus University of Crete Iraklio Heraklion 70013 Greece Contribution: Methodology (equal) Visualization (equal) Contribution: Investigation (equal) Visualization (equal) Contribution: Conceptualization (equal) Investigation (equal) Contribution: Methodology (equal) Contribution: Conceptualization (equal) Methodology (equal) Contribution: Conceptualization (equal) Investigation (equal) Methodology (equal) Writing - review & editing (equal) Contribution: Conceptualization (equal) Funding acquisition (lead) Methodology (equal) Supervision (equal) Writing - review & editing (equal)

We have determined the complex atomic structure of high-temperature α-Ag 9 GaTe 6 phase with a hexagonal lattice ( P 6 3 mc space group, a = b =8.2766 Å, c =13.4349 Å). The structure has outer [GaTe 4 ] 5− tetrahedrons and inner [Ag 9 Te 2 ] 5+ clusters. All of the Ag ions are disorderly distributed in the lattice. Seven types of the Ag atoms constitute the cage-like [Ag 9 Te 2 ] 5+ clusters. The highly disordered Ag ions vibrate in-harmonically, producing strong coupling between low frequency optical phonons and acoustic phonons. This in conjunction with a low sound velocity of 1354 m s −1 leads to an ultralow thermal conductivity of 0.20 W m −1 K −1 at 673 K. Meanwhile, the deficiency of Ga in Ag 9 Ga 1− x Te 6 compounds effectively optimizes the electronic transport properties. Ag 9 Ga 0.91 Te 6 attains a highest power factor of 0.40 mW m −1 K −2 at 673 K. All these contribute to a much-improved ZT value of 1.13 at 623 K for Ag 9 Ga 0.95 Te 6 , which is 41 % higher than that of the pristine Ag 9 GaTe 6 sample.

关键词： α-Ag9GaTe6 Crystal Structure Ga Deficiency Thermoelectrics Ultralow Lattice Thermal Conductivity

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Clustered conflicts in disturbed lowlands characterize human–tiger interactions in Aceh, Indonesia

Wildlife Letters

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Wildlife Letters 2023年第2期1卷

作者： Joe J. Figel Renaldi Safriansyah Said F. Baabud Zulfan Herman Leuser International Foundation Banda Aceh Sumatra Indonesia Department of Conservation and Research Memphis Zoo Memphis Tennessee USA Contribution: Conceptualization (lead) Formal analysis (lead) Funding acquisition (lead) Visualization (lead) Writing - original draft (lead) Department of Political Science Universitas Islam Negeri Ar-Raniry Banda Aceh Sumatra Indonesia Contribution: Conceptualization (supporting) Data curation (lead) Project administration (equal) Writing - review & editing (supporting) Contribution: Conceptualization (supporting) Project administration (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (supporting) Data curation (supporting) Writing - review & editing (supporting)

Conflict with humans is a severe threat to critically endangered Sumatran tigers Panthera tigris sumatrae . To better inform human-tiger conflict (HTC) management in Aceh, Sumatra, we analysed 96 cases of HTC reported to, and verified by, local government authorities between 2017 and 2021. Livestock depredation (49%) and people reporting fear or anxiety upon tiger sightings (39%) comprised most incidents. We found significant differences in the frequency of HTC cases among land cover types in Aceh ( x 2 = 160.4, df = 4, p < 0.001). During our study period, oil palm plantations covered 9.5% of Aceh's land surface but represented the dominant habitat type in 46.9% of the province's HTC cases. By enabling a better understanding of landscape variables and patterns associated with HTC, this study will help to develop management strategies to advance tiger conservation and support rural livelihoods in Aceh, one of the last remaining Sumatran tiger strongholds. 人虎冲突是威胁极度濒危的苏门答腊虎（ Panthera tigris sumatrae ）的重要因素。为了更好地为苏门答腊亚齐省的人虎冲突（HTC）管理提供信息，我们分析了2017-2021年间向当地政府报告并经过核实的96起人虎冲突事件。捕食家畜（49%）和导致人们恐惧或焦虑的目击虎事件（39%）是人虎冲突的主要类型。我们发现亚齐省人虎冲突事件的发生频率在不同土地覆盖类型之间具有显著差异 = 160.4, df = 4, p < .001)。在我们的研究期间，油棕种植园仅占亚齐省土地面积的9.5%，却是46.9%的人虎冲突事件的主要栖息地类型。本研究通过更好地理解与人虎冲突相关的景观变量与模式，有助于亚齐省作为苏门答腊虎最后的避难所之一来制定管理策略，以促进苏门答腊虎的保护并维持农民的生计。 Implement systematic, landscape-scale camera-trap surveys to better understand relationships between tiger population dynamics and human-tiger conflict (HTC). Develop early warning systems to put forest-edge communities on alert and help prevent tiger presence from escalating to HTC. Collaborate with local government and media to facilitate more accurate, science-based portrayal of Sumatran tigers.

关键词： Aceh conflict livestock depredation oil palm Sumatra tiger 亚齐省冲突捕食家畜油棕苏门答腊虎

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Quantitative Point of Care Tests for Timely Diagnosis of Early-Onset Preeclampsia with High Sensitivity and Specificity

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Angewandte Chemie 2023年第26期135卷

作者： Sahar Masoumeh Ghorbanpour Dr. Shihui Wen Prof. Tu'uhevaha J Kaitu'u-Lino Prof. Natalie J. Hannan Prof. Dayong Jin Assoc. Prof. Lana McClements School of Life Sciences & Institute for Biomedical Materials and Devices Faculty of Science University of Technology Sydney Sydney NSW 2007 Australia Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Methodology (lead) Validation (lead) Visualization (lead) Writing - original draft (lead) Institute for Biomedical Materials and Devices School of Mathematical and Physical Sciences Faculty of Science University of Technology Sydney Sydney NSW 2007 Australia ARC Research Hub for Integrated Device for End-user Analysis at Low-levels (IDEAL) Faculty of Science University of Technology Sydney Sydney NSW 2007 Australia Department of Obstetrics & Gynaecology Mercy Hospital for Women The University of Melbourne Heidelberg Australia Mercy Perinatal Mercy Hospital for Women Heidelberg Australia Contribution: Data curation (supporting) Formal analysis (supporting) Resources (supporting) Writing - review & editing (supporting) Contribution: Conceptualization (lead) Funding acquisition (lead) Supervision (lead) Visualization (supporting) Writing - review & editing (supporting)

Preeclampsia is a heterogeneous and multiorgan cardiovascular disorder of pregnancy. Here, we report the development of a novel strip-based lateral flow assay (LFA) using lanthanide-doped upconversion nanoparticles conjugated to antibodies targeting two different biomarkers for detection of preeclampsia. We first measured circulating plasma FKBPL and CD44 protein concentrations from individuals with early-onset preeclampsia (EOPE), using ELISA. We confirmed that the CD44/FKBPL ratio is reduced in EOPE with a good diagnostic potential. Using our rapid LFA prototypes, we achieved an improved lower limit of detection: 10 pg ml −1 for FKBPL and 15 pg ml −1 for CD44, which is more than one order lower than the standard ELISA method. Using clinical samples, a cut-off value of 1.24 for CD44/FKBPL ratio provided positive predictive value of 100 % and the negative predictive value of 91 %. Our LFA shows promise as a rapid and highly sensitive point-of-care test for preeclampsia.

关键词： CD44 FKBPL Point of Care Testing Preeclampsia Upconversion Nanoparticles

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Mapping the Complete Photocycle that Powers a Large Stokes Shift Red Fluorescent Protein

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Angewandte Chemie 2022年第5期135卷

作者： Dr. Ziyu Wang Dr. Ya Zhang Dr. Cheng Chen Dr. Ruixue Zhu Dr. Jiaming Jiang Prof. Tsu-Chien Weng Prof. Quanjiang Ji Prof. Yifan Huang Prof. Chong Fang Prof. Weimin Liu School of Physical Science and Technology ShanghaiTech University 201210 Shanghai China Contribution: Data curation (equal) Formal analysis (lead) Investigation (equal) Methodology (equal) Resources (supporting) Visualization (lead) Writing - original draft (equal) Writing - review & editing (supporting) University of Chinese Academy of Sciences 100049 Beijing China Contribution: Data curation (supporting) Investigation (supporting) Methodology (equal) Resources (supporting) Writing - original draft (supporting) Department of Chemistry Oregon State University 153 Gilbert Hall 97331 Corvallis OR USA Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Validation (supporting) Visualization (supporting) Writing - review & editing (supporting) Contribution: Data curation (supporting) Investigation (supporting) Validation (supporting) Contribution: Investigation (supporting) Validation (supporting) Contribution: Data curation (supporting) Resources (supporting) Supervision (supporting) Validation (supporting) Contribution: Data curation (supporting) Resources (equal) Supervision (supporting) Validation (supporting) Contribution: Data curation (supporting) Funding acquisition (supporting) Resources (equal) Software (lead) Validation (supporting) Visualization (supporting) Contribution: Conceptualization (supporting) Data curation (supporting) Funding acquisition (equal) Investigation (supporting) Project administration (supporting) Resources (supporting) Supervision (supporting) Validation (supporting) Visualization (equal) Writing - review & editing (lead) Contribution: Conceptualization (lead) Data curation (equal) Funding acquisition (lead) Investigation (supporting) Methodology (lead) Project administration (lead) Resources (equal) Supervision (lead) Validation (supporting) Writing - original draft (equal) Writing - review & editing (supporting)

Large Stokes shift (LSS) red fluorescent proteins (RFPs) are highly desirable for bioimaging advances. The RFP mKeima, with coexisting cis- and trans -isomers, holds significance as an archetypal system for LSS emission due to excited-state proton transfer (ESPT), yet the mechanisms remain elusive. We implemented femtosecond stimulated Raman spectroscopy (FSRS) and various time-resolved electronic spectroscopies, aided by quantum calculations, to dissect the cis - and trans -mKeima photocycle from ESPT, isomerization, to ground-state proton transfer in solution. This work manifests the power of FSRS with global analysis to resolve Raman fingerprints of intermediate states. Importantly, the deprotonated trans -isomer governs LSS emission at 620 nm, while the deprotonated cis -isomer's 520 nm emission is weak due to an ultrafast cis -to- trans isomerization. Complementary spectroscopic techniques as a table-top toolset are thus essential to study photochemistry in physiological environments.

关键词： Chromophore Isomerization Excited- and Ground-State Proton Transfer Femtosecond Raman Spectroscopy Large Stokes Shift Red Fluorescent Proteins

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Distinguishing Protein Chemical Topologies Using Supercharging Ion Mobility Spectrometry-Mass Spectrometry

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Angewandte Chemie 2023年第51期135卷

作者： Jiyeon Lee Dahye Im Yajie Liu Jing Fang Xibao Tian Minsu Kim Prof. Wen-Bin Zhang Prof. Jongcheol Seo Department of Chemistry Pohang University of Science and Technology (POSTECH) 77 Cheongam-ro Nam-gu Pohang 37673 Gyeonsangbuk-do (Republic of Korea Contribution: Data curation (lead) Formal analysis (equal) Visualization (lead) Writing - original draft (lead) Writing - review & editing (supporting) Contribution: Data curation (supporting) Formal analysis (equal) Visualization (supporting) Writing - original draft (supporting) Writing - review & editing (supporting) Beijing National Laboratory for Molecular Sciences Key Laboratory of Polymer Chemistry & Physics of Ministry of Education Center for Soft Matter Science and Engineering College of Chemistry and Molecular Engineering Peking University Beijing 100871 P. R. China Contribution: Resources (equal) Contribution: Data curation (supporting) Validation (supporting) Contribution: Conceptualization (equal) Funding acquisition (equal) Investigation (equal) Project administration (supporting) Writing - review & editing (equal) Contribution: Conceptualization (equal) Funding acquisition (equal) Investigation (lead) Project administration (lead) Validation (lead) Writing - review & editing (lead)

A technique combining ion mobility spectrometry-mass spectrometry (IMS-MS) and supercharging electrospray ionization (ESI) has been demonstrated to differentiate protein chemical topology effectively. Incorporating as many charges as possible into proteins via supercharging ESI allows the protein chains to be largely unfolded and stretched, revealing their hidden chemical topology. Different chemical topologies result in differing geometrical sizes of the unfolded proteins due to constraints in torsional rotations in cyclic domains. By introducing new topological indices, such as the chain-length-normalized collision cross-section (CCS) and the maximum charge state ( z M ) in the extensively unfolded state, we were able to successfully differentiate various protein chemical topologies, including linear chains, ring-containing topologies (lasso, tadpole, multicyclics, etc.), and mechanically interlocked rings, like catenanes.

关键词： Mass Spectrometry Protein Engineering Proteins

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Mesopredators in forest edges森林边缘地带的中级捕食者

Wildlife Letters

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Wildlife Letters 2023年第3期1卷

作者： Matthew Scott Luskin Lindsey Arnold Adia Sovie Zachary Amir Marcus Aik Hwee Chua Bastien Dehaudt Ashlea Dunn Ilyas Nursamsi Jonathan H. Moore Calebe P. Mendes School of the Environment University of Queensland Brisbane Queensland Australia Centre for Biodiversity and Conservation Science University of Queensland Brisbane Queensland Australia Contribution: Conceptualization (lead) Data curation (equal) Formal analysis (equal) Investigation (equal) Methodology (equal) Project administration (lead) Resources (lead) Writing - original draft (equal) Writing - review & editing (lead) Contribution: Formal analysis (equal) Writing - original draft (equal) Department of Fisheries and Wildlife Michigan State University East Lansing Michigan USA School of Environmental Science and Engineering Southern University of Science and Technology Shenzhen China Contribution: Formal analysis (equal) Investigation (equal) Writing - original draft (equal) Writing - review & editing (equal) Contribution: Conceptualization (supporting) Formal analysis (equal) Writing - review & editing (supporting) Lee Kong Chian Natural History Museum National University of Singapore Singapore Singapore Contribution: Writing - original draft (supporting) Contribution: Formal analysis (supporting) Visualization (supporting) Contribution: Formal analysis (supporting) Writing - original draft (supporting) Contribution: Investigation (supporting) Methodology (supporting) Visualization (supporting) School of Environmental Sciences University of East Anglia Norwich UK Contribution: Data curation (equal) Investigation (supporting) Writing - original draft (supporting) Asian School of the Environment Nanyang Technological University Singapore Singapore Contribution: Data curation (equal) Formal analysis (supporting) Investigation (supporting) Visualization (supporting)

Fragments and edges account for most remaining forest habitats globally. Apex predators and megaherbivores often decline in these degraded habitats while smaller generalist omnivores can persist or thrive in forest edges, especially if they can utilize nonnative resources (“cross-boundary food subsidies”). Outcomes for small-medium carnivores (mesopredators) remain unclear or idiosyncratic. We tested responses of a widespread and common forest mesopredator to edges and the composition of the adjacent nonforested areas using 91 camera trapping surveys in Southeast Asia. Leopard cats ( Prionailurus bengalensis and Prionailurus javanensis ) showed a hump-shaped relationship with forest cover and a positive association with oil palm plantations, but they did not increase near other types of nonnative land cover. Leopard cats' success in edges appears due to their hunting abundant rodent prey inside oil palm plantations, providing natural pest management for farmers. Abundant leopard cats also hunt and suppress native small vertebrates, which may trigger negative ecological cascades and suppress biodiversity in forest edges. 全球大部分残留的森林栖息地都是破碎化和边缘性的。在生境退化的栖息地中，顶级捕食者和大型草食动物种群数量通常会减少，而普适性的杂食动物则可以在森林边缘地带生存或持续发展，尤其是当这些杂食动物可以利用非本土资源（称为“跨界食物补充”）时。而中小型食肉动物（中级捕食者）在这些区域的种群趋势尚不明确或因种而异。我们在东南亚利用91 个自动相机监测位点，检验了一种常见的广泛分布的森林中级捕食者对于边缘地区以及邻近非森林区域复合景观的反应。豹猫（ Prionailurus bengalensis and P. javanensis ）丰富度与森林覆盖率呈单峰形关系，与油棕榈种植园呈正相关，然而，在其他非原生植被覆盖的生境附近，豹猫的数量并没有增加。豹猫在森林边缘地带的成功分布是因为它们在油棕榈种植园内捕食大量的啮齿类猎物，这起到帮助农民管理自然害兽的作用。豹猫还捕食并抑制了本地小型脊椎动物，这可能会引发生物多样性的级联效应。 The rise of native mesopredators in forest edges provides pest control ecosystem services by regulating rodent proliferation in cultivated lands and natural forest edges, benefiting people and conservation. Native mesopredators can be managed by farmers (e.g., oil palm plantation managers) through the retention of natural forest patches and the selective cultivation of preferred microhabitats (e.g., shade trees and understory vegetation). Abunda

关键词： camera trapping carnivore deforestation felid leopard cat mesopredator release oil palm pest control Prionailurus bengalensis wildlife conservation 相机陷阱食肉动物森林砍伐猫科动物豹猫 Prionailurus bengalensis 中级捕食者释放油棕榈害兽控制野生动物保护

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Temperature-dependent phonon lifetimes and thermal conductivity of silicon by inelastic neutron scattering and ab initio calculations

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Physical Review B 2020年第17期102卷 174311-174311页

作者： D. S. Kim O. Hellman N. Shulumba C. N. Saunders J. Y. Y. Lin H. L. Smith J. E. Herriman J. L. Niedziela D. L. Abernathy C. W. Li B. Fultz Department of Applied Physics and Materials Science California Institute of Technology Pasadena California 91125 USA Department of Mechanical and Civil Engineering California Institute of Technology Pasadena California 91125 USA Neutron Data Analysis and Visualization Division Oak Ridge National Laboratory Oak Ridge Tennessee 37831 USA Physics and Astronomy Department Swarthmore University Swarthmore Pennsylvania 19081 USA Division of Materials Science and Technology Oak Ridge National Laboratory Oak Ridge Tennessee 37831 USA Division of Neutron Scattering Oak Ridge National Laboratory Oak Ridge Tennessee 37831 USA Department of Mechanical Engineering University of California Riverside California 92521 USA

Inelastic neutron scattering on a single crystal of silicon was performed at temperatures from 100 to 1500 K. These experimental data were reduced to obtain phonon spectral intensity at all wave vectors Q⃗ and frequencies ω in the first Brillouin zone. Thermal broadenings of the phonon peaks were obtained by fitting and by calculating with an iterative ab initio method that uses thermal atom displacements on an ensemble of superlattices. Agreement between the calculated and experimental broadenings was good, with possible discrepancies at the highest temperatures. Distributions of phonon widths versus phonon energy had similar shapes for computation and experiment. These distributions grew with temperature but maintained similar shapes. Parameters from the ab initio calculations were used to obtain the thermal conductivity from the Boltzmann transport equation, which was in good agreement with experimental data. Despite the high group velocities of longitudinal acoustic phonons, their shorter lifetimes reduced their contribution to the thermal conductivity, which was dominated by transverse acoustic modes.

关键词： Lattice thermal conductivity Semiconductors Neutron scattering Time-of-flight neutron spectroscopy

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Glucose-Responsive Charge-Switchable Lipid Nanoparticles for Insulin Delivery

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Angewandte Chemie 2023年第20期135卷

作者： Yun Liu Yanfang Wang Yuejun Yao Juan Zhang Wei Liu Kangfan Ji Xinwei Wei Yuanwu Wang Prof. Xiangsheng Liu Prof. Shiming Zhang Prof. Jinqiang Wang Prof. Zhen Gu Key Laboratory of Advanced Drug Delivery Systems of Zhejiang Province College of Pharmaceutical Sciences Zhejiang University 310058 Hangzhou China Jinhua Institute of Zhejiang University 321299 Jinhua China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Software (lead) Validation (lead) Visualization (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Data curation (supporting) Investigation (supporting) Visualization (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Contribution: Formal analysis (supporting) Investigation (supporting) Methodology (supporting) Contribution: Formal analysis (supporting) Investigation (supporting) Contribution: Writing - review & editing (supporting) Contribution: Investigation (supporting) Zhejiang Cancer Hospital Hangzhou Institute of Medicine (HIM) Chinese Academy of Sciences 310022 Hangzhou China Department of Electrical and Electronic Engineering The University of Hong Kong 999077 Hong Kong SAR China Second Affiliated Hospital Zhejiang University School of Medicine 310009 Hangzhou China Contribution: Conceptualization (lead) Data curation (equal) Formal analysis (equal) Funding acquisition (lead) Investigation (lead) Methodology (equal) Project administration (lead) Resources (lead) Software (lead) Supervision (lead) Validation (supporting) Visualization (supporting) Writing - review & editing (lead) Department of General Surgery Sir Run Run Shaw Hospital School of Medicine Zhejiang University 310009 Hangzhou China Zhejiang Laboratory of Systems & Precision Medicine Zhejiang University Medical Center 310009 Hangzhou China MOE Key Laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University 310009 Hangzhou China Contribution: Funding acquisition (lead) Project administration (lead) Resources (lead) Softwar

Lipid nanoparticle-based drug delivery systems have a profound clinical impact on nucleic acid-based therapy and vaccination. Recombinant human insulin, a negatively-charged biomolecule like mRNA, may also be delivered by rationally-designed positively-charged lipid nanoparticles with glucose-sensing elements and be released in a glucose-responsive manner. Herein, we have designed phenylboronic acid-based quaternary amine-type cationic lipids that can self-assemble into spherical lipid nanoparticles in an aqueous solution. Upon mixing insulin and the lipid nanoparticles, a heterostructured insulin complex is formed immediately arising from the electrostatic attraction. In a hyperglycemia-relevant glucose solution, lipid nanoparticles become less positively charged over time, leading to reduced attraction and subsequent insulin release. Compared with native insulin, this lipid nanoparticle-based glucose-responsive insulin shows prolonged blood glucose regulation ability and blood glucose-triggered insulin release in a type 1 diabetic mouse model.

关键词： Diabetes Drug Delivery Glucose-Responsive Insulin Delivery Lipid Nanoparticles

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