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Translocation of ssDNA through Charged Graphene Nanopores:Effect of the Charge Density

Chinese Journal of polymer science 2024年第12期42卷 2048-2058,I0013页

作者： Yuan-Shuo Zhang Zhi-Ya Qi Ming-Ming Ding Ming-Lun Li Tong-Fei Shi School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou510006China Jieyang Branch of Chemistry and Chemical Engineering Guangdong Laboratory Jieyang515200China Department of Polymer Science and Engineering University of Massachusetts Amherst120 Governors DriveAmherstMassachusetts01003USA

Nanopore sequencing harnesses changes in ionic current as nucleotides traverse a nanopore,enabling real-time decoding of DNA/RNA *** instruments for the dynamic behavior of substances in the nanopore on the molecular scale are still very limited *** study employs all-atom molecular dynamics(MD)simulations to explore the impact of charge densities on graphene nanopore in the translocation of single-stranded DNA(ssDNA).We find that the magnitude of graphene’s charge,rather than the charge disparity between ssDNA and graphene,significantly influences ssDNA adsorption and translocation ***,high negative charge densities on graphene nanopores are shown to substantially slow down ssDNA translocation,highlighting the importance of hydrodynamic effects and electrostatic *** indicates translocation is crucial for achieving distinct ionic current blockades,which plays a central role for DNA sequencing *** findings suggest that negatively charged graphene nanopores hold considerable potential for optimizing DNA sequencing,marking a critical advancement in this field.

关键词： Nanopore sequencing Graphene nanoslit DNA translocation Electroosmotic flow

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Sulfur-doped hard carbon hybrid anodes with dual lithium-ion/metal storage bifunctionality for high-energy-density lithium-ion batteries

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Carbon Energy 2023年第1期5卷 71-81页

作者： Sungmin Cho Jong Chan Hyun Son Ha Yeonhua Choi Honggyu Seong Jaewon Choi Hyoung-Joon Jin Young Soo Yun Program in Environmental and Polymer Engineering Inha UniversityIncheonSouth Korea KU-KIST Graduate School of Converging Science and Technology Korea UniversitySeoulSouth Korea Departmant of Chemistry and Research Institute of Natural Science Gyeongsang National UniversityJinjuSouth Korea Department of Polymer Science and Engineering Inha UniversityIncheonSouth Korea Division of Energy Engineering Kangwon National UniversityGangwon-doSouth Korea

Bifunctional hybrid anodes(BHAs),which are both a high-performance active host material for lithium-ion storage as well as a guiding agent for homogeneous lithium metal nucleation and growth,exhibit significant potential as anodes for next-generation high-energy-density lithium-ion batteries(LIBs).In this study,sulfur-doped hard carbon nanosphere assemblies(S-HCNAs)were prepared through a hydrothermal treatment of a liquid organic precursor,followed by high-temperature thermal annealing with elemental sulfur for application as BHAs for *** a carbonate-based electrolyte containing fluoroethylene carbonate additive,the S-HCNAs showed high lithium-ion storage capacities in sloping as well as plateau voltage sections,good rate capabilities,and stable *** addition,high average Coulombic efficiencies(CEs)of~96.9%were achieved for dual lithium-ion and lithium metal storage *** the LIB full-cell tests with typical NCM811 cathodes,the S-HCNA-based BHAs containing~400 mA h g^(−1) of excess lithium led to high energy and power densities of~500Wh kg^(−1) and~1695Wkg^(−1),respectively,and a stable cycling performance with~100%CEs was achieved.

关键词： hard carbon hybrid anode lithium-ion batteries lithium metal anode lithium metal batteries sulfur-doped carbon

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Dense carbon nanofiber self-supporting electrode fabricated by orientation/compaction strategy for high volumetric lithium storage capacity

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Progress in Natural science:Materials International 2025年第1期35卷 229-237页

作者： Haihui Liu Chaoqun Chen Qiang Xu Yan Song Xiangwu Zhang Chang Ma Tianjin Municipal Key Lab of Advanced Fiber and Energy Storage Technology Tiangong University CAS Key Laboratory of Carbon Materials Institute of Coal Chemistry Chinese Academy of Sciences Fiber and Polymer Science Program Department of Textile Engineering Chemistry and Science Wilson College of Textiles North Carolina State University

Low bulk density greatly restricts the large-scale application of electrospun carbon-based fiber membrane as electrode in energy storage devices. To solve the above challenges, herein an orientation-compaction densification strategy is proposed to enhance the bulk density and volumetric capacity of PAN-based carbon nanofiber membranes as self-supporting electrode used in lithium-ion batteries（LIBs）. Specifically, highly-oriented fibers are achieved by high-speed roller collecting during electrospinning, and compaction densification is conducted by hot-pressing treatment. The effects of collecting speed and hot-pressing pressure on the morphology, conductivity,bulk density, tensile strength, and flexibility of the obtained carbon nanofiber membrane are *** to conventional fiber membranes, of which fibers are disorderly stacked, the oriented fiber membrane is much easier to achieve dense stacking by compaction. The obtained dense carbon nanofiber membrane demonstrates a bulk density of 0.566 g cm-3, and shows a significantly-enhanced volumetric capacity(318.3 mA h cm-3), high-rate performance(86.6 mA h cm-3at 5 A g-1), and satisfactory cycling stability when used as selfsupporting electrode of LIBs.

关键词： Bulk density Densification Electrospinning Orientation-compaction Volumetric capacity

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Thermal stability and secondary aggregation of self-limiting, geometrically frustrated assemblies: Chain assembly of incommensurate polybricks

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Physical Review E 2024年第1期109卷 014608-014608页

作者： Michael Wang Gregory Grason Department of Polymer Science and Engineering University of Massachusetts Amherst Massachusetts 01003 USA

In geometrically frustrated assemblies, equilibrium self-limitation manifests in the form of a minimum in the free energy per subunit at a finite, multisubunit size which results from the competition between the elastic costs of frustration within an assembly and the surface energy at its boundaries. Physical realizations—from ill-fitting particle assemblies to self-twisting protein superstructures—are capable of multiple mechanisms of escaping the cumulative costs of frustration, resulting in unlimited equilibrium assembly, including elastic modes of “shape flattening” and the formation of weak, defective bonds that screen intra-assembly stresses. Here we study a model of one-dimensional chain assembly of incommensurate “polybricks” and determine its equilibrium assembly as a function of temperature, concentration, degree of shape frustration, elasticity, and interparticle binding, notably focusing on how weakly cohesive, defective bonds give rise to strongly temperature-dependent assembly. Complex assembly behavior derives from the competition between multiple distinct local minima in the free-energy landscape, including self-limiting chains, weakly bound aggregates of self-limiting chains, and strongly bound, elastically defrustrated assemblies. We show that this scenario, in general, gives rise to anomalous multiple aggregation behavior, in which disperse subunits (stable at low concentration and high temperature) first exhibit a primary aggregation transition to self-limiting chains (at intermediate concentration and temperature) which are ultimately unstable to condensation into unlimited assembly of finite-chains through weak binding beyond a secondary aggregation transition (at low temperature and high concentration). We show that window of stable self-limitation is determined both by the elastic costs of frustration in the assembly as well as energetic and entropic features of intersubunit binding.

关键词： Aggregation Self-assembly Biomolecules Colloids Patchy particles Series expansions & exact enumeration

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Harnessing Multiple Surface Deformation Modes for Switchable Conductivity Surfaces

Harnessing Multiple Surface Deformation Modes for Switchable...

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2023 AIChE Annual Meeting

作者： Ouchi, Tetsu Hayward, Ryan C. Department of Polymer Science and Engineering University of Massachusetts Amherst AmherstMA01003 United States

Surface deformation modes, such as wrinkling, creasing, and cracking, enable a plethora of surface morphologies under mechanical loading, which have been widely exploited to provide flexibility and stretchability to electronic devices. As each phenomenon offers a distinct set of potential advantages, controlling the types and spatial locations of deformation modes is key for their successful application. In this study, we demonstrate a method to simultaneously harness multiple surface deformation modes-wrinkles, creases, and cracks-in patterned multilayer films. The wrinkling of metal-coated stiff patterned films provides flexibility and stretchability, while the reversible formation of creases in the intervening regions of the bare elastomer is used to template the formation of patterned cracks in the metal. While conventional cracks can be difficult to precisely control, the patterned cracks demonstrated here remain straight over long distances and show tunable lateral spacings from hundreds of micrometers to centimeters. Finally, the reversible opening and closing of these cracks under mechanical loading provides mechanically gated electrical switches with small and tunable critical switching strains of 0.05−0.18 and high on/off ratios of >107, enabling the preparation of mechanical NAND and NOR logic gates each composed of multiple patterned switches on a single elastomer surface. © 2020 American Chemical Society.

关键词： Flexible electronics

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Excitations in layered materials from a non-empirical Wannier-localized optimally-tuned screened rangeseparated hybrid functional

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npj Computational Materials 2024年第1期10卷 132-140页

作者： María Camarasa-Gómez Stephen E.Gant Guy Ohad Jeffrey B.Neaton Ashwin Ramasubramaniam Leeor Kronik Department of Molecular Chemistry and Materials Science Weizmann Institute of ScienceRehovoth7610001Israel Department of Physics University of CaliforniaBerkeleyCA94720USA Materials Sciences Division Lawrence Berkeley National LaboratoryBerkeleyCA94720USA Kavli Energy NanoSciences Institute at Berkeley University of CaliforniaBerkeleyCA94720USA Department of Mechanical and Industrial Engineering University of Massachusetts AmherstAmherstMA01003USA Materials Science and Engineering Graduate Program University of MassachusettsAmherstAmherstMA01003USA

Accurate prediction of electronic and optical excitations in van der Waals(vdW)materials is a long-standing challenge for density functional *** recent Wannier-localized optimally-tuned screened range-separated hybrid(WOT-SRSH)functional has proven successful in non-empirical determination of electronic band gaps and optical absorption spectra for covalent and ionic ***,for vdW materials the tuning of the material-and structure-dependent functional parameters has only been attained ***,we present a non-empirical WOT-SRSH approach applicable to vdW materials,with the optimal functional parameters transferable between monolayer and *** apply this methodology to prototypical vdW materials:black phosphorus,molybdenum disulfide,and hexagonal boron nitride(in the latter case including zero-point renormalization).We show that the WOT-SRSH approach consistently achieves accuracy levels comparable to experiments and many-body perturbation theory(MBPT)calculations for band structures and optical absorption spectra,both on its own and as an optimal starting point for MBPT calculations.

关键词： theory optimal functional

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Dispersed, Condensed, and Self-Limiting States of Geometrically Frustrated Assembly

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Physical Review X 2023年第4期13卷 041010-041010页

作者： Nicholas W. Hackney Christopher Amey Gregory M. Grason Department of Polymer Science and Engineering University of Massachusetts Amherst

In self-assembling systems, geometric frustration leads to complex states characterized by internal gradients of shape misfit. Frustrated assemblies have drawn recent interest due to the unique possibility that their thermodynamics can sense and select the finite size of assembly at length scales much larger than constituent building blocks or their interactions. At present, self-limitation is chiefly understood to derive from zero-temperature considerations, specifically the competition between cohesion and scale-dependent elastic costs of frustration. While effects of entropy and finite-temperature fluctuations are necessarily significant for self-assembling systems, their impact on the self-limiting states of frustrated assemblies is not known. We introduce a generic, minimal model of frustrated assembly and establish its finite-temperature and concentration-dependent thermodynamics by way of simulation and continuum theory. The phase diagram is marked by three distinct states of translation order: a dispersed vapor, a defect-riddled condensate, and the self-limiting aggregate state. We show that, at finite temperature, the self-limiting state is stable at intermediate frustration. Furthermore, in contrast to the prevailing picture, its thermodynamic boundaries with the macroscopic disperse and bulk states are temperature controlled, pointing to the essential importance of translational and conformational entropy in their formation.

关键词： Phase behavior Self-assembly Geometry

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Polyacrylonitrile Nanofber‑Reinforced Flexible Single‑Ion Conducting polymer Electrolyte for High‑Performance,Room‑Temperature All‑Solid‑State Li‑Metal Batteries

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Advanced Fiber Materials 2022年第3期4卷 532-546页

作者： Hui Cheng Chaoyi Yan Raphael Orenstein Mahmut Dirican Shuzhen Wei Nakarin Subjalearndee Xiangwu Zhang Fiber and Polymer Science Program Department of Textile EngineeringChemistry and ScienceWilson College of TextilesNorth Carolina State UniversityRaleighNC 27695USA

Single-ion conducting polymer electrolytes(SIPEs)can be formed by anchoring charge delocalized anions on the side chains of a crosslinked polymer matrix,thereby eliminating the severe concentration polarization efect in conventional dual-ion polymer *** of a plasticizer into the polymer matrix confers advantages of both liquid and solid ***,plasticized SIPEs usually face a trade-of between conductivity and mechanical *** insufcient strength,potentially there is short-circuiting failure during *** address this challenge,a simple and mechanicallyrobust SIPE was developed by crosslinking monomer lithium(4-styrenesulfonyl)(trifuoromethylsulfonyl)imide(LiSTFSI)and crosslinker poly(ethylene glycol)diacrylate(PEGDA),with plasticizer propylene carbonate(PC),on electrospun polyacrylonitrile nanofbers(PAN-NFs).The well-fabricated polymer matrix provided fast and efective Li^(+) conductive pathways with a remarkable ionic conductivity of 8.09×10^(-4) S cm^(−1) and a superior lithium-ion transference number close to unity(t_(Li+)=0.92).The introduction of PAN-NFs not only improved the mechanical strength and fexibility but also endowed the plasticized SIPE with a wide electrochemical stability window(4.9 V ***^(+)/Li)and better cycling *** longterm lithium cycling stability and dynamic interfacial compatibility were demonstrated by lithium symmetric cell *** importantly,the assembled all-solid-state Li metal batteries showed stable cycling performance and remarkable rate capability both in low and high current ***,this straightforward and mechanically reinforced SIPE exhibits great potential in the development of advanced all-solid-state Li-metal batteries.

关键词： Single-ion conducting polymer electrolyte Electrospun nanofbers Mechanical properties All-solid-state batteries Rate capability

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Bio-inspired Smart Composites with Multi-scale Architecture and Surface engineering 23

Bio-inspired Smart Composites with Multi-scale Architecture ...

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23rd International Conference on Composite Materials, ICCM 2023

作者： Zeng, Songshan Shen, Kuangyu Li, Rui Smith, Andrew Zhang, Dianyun Sun, Luyi Polymer Program Institute of Materials Science Department of Chemical & Biomolecular Engineering University of Connecticut United States

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Fluorinated Functional Units for Li+ Flux Homogenization in Silica Framework-Based Zwitterionic Single Ion Conductors for Stable Lithium Metal Batteries

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Advanced Energy Materials 2025年第21期15卷

作者： Handayani, Puji Lestari Yun, Susung Kim, Gihyeon Choi, U Hyeok Department of Polymer Science and Engineering and Program in Environmental and Polymer Engineering Inha University Incheon22212 Korea Republic of

Progress in commercializing solid polymer electrolytes (SPEs) for lithium metal batteries (LMBs) has been impeded by challenges, like concentration polarization, non-uniform Li+ flux, and an unstable solid electrolyte interface (SEI), which contribute to dendrite formation. To address these issues, silica framework (SF)-based single-ion conductors are proposed, featuring a unique solvation channel composed of a fluorinated segment, a high-dipole zwitterion, and a rotation-motion-driven ion-hopping medium. This design promotes low resistance at the cathode/electrode interface, suppresses dendrite growth at the anode/electrolyte interface, and maintains a uniform Li+ flux. This results show that continuous ion channels within a robust framework enhance Li-ion dissociation and transport, achieving high ionic conductivity (σDC = 8.8 × 10−4 S cm−1), a modulus of 0.9 GPa, a high lithium transference number (≈0.83), and an extended electrochemical stability window (up to 5.2 V) at 25 °C. This design fosters the formation of a hybrid organic/inorganic SEI layer composed of Li2CO3, LiF, and Li2O, enabling ultra-stable Li plating/stripping for over 4000 h at 0.1 mA cm−2. Furthermore, the full cells demonstrate excellent rate performance and long-term cycling stability and capacity retention (81% for Li||LFP and 86% for Li||NCM811 after 400 cycles at 1 C) and high coulombic efficiency, offering a promising strategy to stable LMBs. © 2025 The Author(s). Advanced Energy Materials published by Wiley-VCH GmbH.

关键词： Solid electrolytes

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