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arXiv 2023年

作者： Fang, Yan Rumyantsev, Artem M. Neitzel, Angelika E. Liang, Heyi Heller, William T. Nealey, Paul F. Tirrell, Matthew V. de Pablo, Juan J. Pritzker School of Molecular Engineering University of Chicago ChicagoIL60637 United States Center for Molecular Engineering and Materials Science Division Argonne National Laboratory LemontIL60439 United States Department of Chemical and Biomolecular Engineering North Carolina State University RaleighNC27695 United States Department of Materials Science & Engineering University of Florida GainesvilleFL32611 United States Neutron Scattering Division Oak Ridge National Laboratory Oak RidgeTN37831 United States

Polyelectrolyte complexation plays an important role in materials science and biology. The internal structure of the resultant polyelectrolyte complex (PEC) phase dictates properties such as physical state, response to external stimuli, and dynamics. Small-angle scattering experiments with X-rays and neutrons have revealed structural similarities between PECs and semidilute solutions of neutral polymers, where the total scattering function exhibits an Ornstein-Zernike form. In spite of consensus among different theoretical predictions, the existence of positional correlations between polyanion and polycation charges has not been confirmed experimentally. Here, we present small-angle neutron scattering profiles where the polycation scattering length density is matched to that of the solvent to extract positional correlations among anionic monomers. The polyanion scattering functions exhibit a peak at the inverse polymer screening radius of Coulomb interactions, q∗ ≈ 0.2 Å−1. This peak, attributed to Coulomb repulsions between the fragments of polyanions and their attractions to polycations, is even more pronounced in the calculated charge scattering function that quantifies positional correlations of all polymer charges within the PEC. Screening of electrostatic interactions by adding salt leads to the gradual disappearance of this correlation peak, and the scattering functions regain an Ornstein-Zernike form. Experimental scattering results are consistent with those calculated from the random phase approximation, a scaling analysis, and molecular simulations. © 2023, CC BY.

关键词： Approximation algorithms

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Bacterial Mobility and Motility in Porous Media Mimicked By Microspheres

SSRN

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SSRN 2022年

作者： Shrestha, Diksha Ou, Jun Rogers, Ariel Jereb, Amani Wang, Yong Department of Physics Cell and Molecular Graduate Program Materials Science and Engineering Program University of Arkansas FayettevilleAR72701 United States Department of Environmental Resources Engineering Mechanical Engineering Program California State Polytechnic University Humboldt ArcataCA95521 United States

Bacterial motion in porous media are essential for their survival, proper functioning, and variousapplications. Here we investigated the motion of Escherichia coli bacteria in microsphere-mimicked porousmedia. We observed reduced bacterial velocity and enhanced directional changes of bacteria as the densityof microspheres increased, while such changes happened mostly around the microspheres and due to thecollisions with the microspheres. More importantly, we established and quantified the correlation betweenthe bacterial trapping in porous media and the geometric confinement imposed by the microspheres. In addition,numerical simulations showed that the active Brownian motion model in the presence of microspheresresulted in bacterial motion that are consistent with the experimental observations. Our study suggested thatit is important to distinguish the ability of bacteria to move easily – bacterial mobility – from the abilityof bacteria to move independently – bacteria motility. Our results showed that bacterial motility remainssimilar in porous media, but bacterial mobility was significantly affected by the pore-scale confinement. © 2022, The Authors. All rights reserved.

关键词： Microspheres

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Low-temperature sintering of Li0.33La0.55TiO3 electrolyte for all-solid-state Li batteries

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Journal of the European Ceramic Society 2023年第16期43卷 7543-7552页

作者： Lin, Che-an Ihrig, Martin Kung, Kuan-chen Chen, Hsiang-ching Scheld, Walter Sebastian Ye, Ruijie Finsterbusch, Martin Guillon, Olivier Lin, Shih-kang Department of Materials Science and Engineering National Cheng Kung University Tainan70101 Taiwan Institute of Energy and Climate Research – Materials Synthesis and Processing Forschungszentrum Jülich GmbH Jülich52425 Germany Department of Chemical Engineering National Taiwan University of Science and Technology No. 43 Keelung Rd. Section 4 Da'an Dist Taipei City106 Taiwan Helmholtz Institute Münster: Ionics in Energy Storage Corrensstr. 46 Münster48149 Germany Research Center National Cheng Kung University Tainan70101 Taiwan Program on Smart and Sustainable Manufacturing Academy of Innovative Semiconductor and Sustainable Manufacturing National Cheng Kung University Tainan70101 Taiwan Core Facility Center National Cheng Kung University Tainan70101 Taiwan

Ceramic solid-state Li batteries have promising electrochemical properties. However, their device integration is hampered by the required high sintering temperature step to obtain good ionic conductivity. The sintering temperature often leads to thermal decomposition of the cathode active material. Advanced sintering techniques, such as field-assisted sintering technology/spark plasma sintering (FAST/SPS), utilizing applied mechanical pressure to achieve a lower sintering temperature and shorter dwell time, are helpful in overcoming thermal stability challenges. While thermal stability issues are overcome by a lower sintering temperature, new challenges in the form of surface impurities arise. Low-temperature sintering does not thermally decompose surface impurities which causes low grain boundary conductivity and thus low total ionic conductivity. In this work, a cleaning method and a low-temperature sintering process is exemplarily developed for Li0.33La0.55TiO3 (LLTO) and the impact of applied mechanical pressure during FAST/SPS on the total ionic conductivity and the phase stability of LLTO is revealed. © 2023 Elsevier Ltd

关键词： Spark plasma sintering

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Selective Ligase-Based Sample Processing-Free Discrimination and Detection of Site-Specific DNA 5-Hydroxymethylcytosine

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Analytical chemistry 2024年第32期96卷 13285-13290页

作者： Jiahui Zhao Jingli Yan Jing Li Guoyu Shi Ming Su Chenghui Liu Guifang Jia Key Laboratory of Medicinal Chemistry and Molecular Diagnosis of the Ministry of Education Key Laboratory of Analytical Science and Technology of Hebei Province (Project Number: 22567620H) State Key Laboratory of New Pharmaceutical Preparations and Excipients College of Chemistry and Materials Science Hebei University Baoding 071002 China. Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education Key Laboratory of Analytical Chemistry for Life Science of Shaanxi Province School of Chemistry & Chemical Engineering Shaanxi Normal University Xi'an 710119 China. Department of Chemical Biology Synthetic and Functional Biomolecules Center Beijing National Laboratory for Molecular Sciences Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of Education College of Chemistry and Molecular Engineering Beijing Advanced Innovation Center for Genomics Peking University Beijing 100871 China.

Accurate detection of site-specific 5-hydroxymethylcytosine (5hmC) in genomic DNA is of great significance, but it is technically challenging to directly distinguish very low levels of 5hmC from their abundant cytosine/5-methylcytosine (C/5mC) analogues. Herein, we wish to propose a selective ligase-mediated mechanism (SLim) that can directly discriminate 5hmC from C/5mC with a high specificity without the use of any sample processing protocol. In this new design, we discovered that HiFi Taq DNA Ligase can well tolerate the mismatched 5hmC/A base-pairing and then effectively ligate the associated nicking site while the mismatched 5mC/A or C/A pairs cannot be recognized by HiFi Taq DNA Ligase, providing a new way for direct and selective discriminating 5hmC from its similar analogues. Ultrasensitive and selective quantification of site-specific 5hmC is realized by coupling the SLim with polymerase chain reaction (PCR) or loop-mediated isothermal amplification (LAMP).

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介于二维和三维晶体间的超薄晶态材料的X射线衍射及对称性研究

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science Bulletin 2023年第9期68卷 887-891,M0003页

作者：马恒瑞蒋巧荣南子昂李根贾艳艳宁若昕吉家葆曹振明吕林喆李慧齐戴升林海昕谢兆雄 State Key Laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materialsand Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center Institute of Fine ChemicalsSchool of Chemistry&Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Department of Chemistry and Applied Biosciences Laboratory of Physical ChemistryETH ZürichZürich CH-8093Switzerland Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361005China

为了深入理解超薄晶态材料的结构和对称性的独特性,本文在充分考虑超薄晶态材料堆积自由度的情况下,从数学和晶体学角度对介于二维与三维之间的超薄纳米晶体的对称性和X射线衍射进行了探讨.认为超薄纳米晶体的对称性需要用数学层群(laye... 详细信息

为了深入理解超薄晶态材料的结构和对称性的独特性,本文在充分考虑超薄晶态材料堆积自由度的情况下,从数学和晶体学角度对介于二维与三维之间的超薄纳米晶体的对称性和X射线衍射进行了探讨.认为超薄纳米晶体的对称性需要用数学层群(layer group)来描述;另外,由于其层堆叠方向上不具有周期性结构,超薄纳米晶体可能产生特异衍射特征.为了验证这一观点,研究了三类在层堆叠方向不具有周期性的典型超薄纳米晶体的X射线衍射,从实验上观察到了超薄纳米晶体与其体相三维晶体粉末X射线衍射的不同;针对基于三维晶体的X射线衍射模拟软件不再适用于超薄纳米晶体的情况,发展了超薄纳米晶体的全结构X射线衍射分析方法,很好地模拟了超薄纳米晶粉末X射线衍射图.该研究对超薄纳米晶态材料的结构及对称性提出了新见解,将有益于推动相关材料的构效关系研究和新功能开发.

关键词：纳米晶体周期性结构 X射线衍射纳米晶粉末模拟软件对称性自由度

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engineering “JiaoJiao”(maltose syrup) with chopsticks: From traditional Chinese sweet food to skin-like iontronics

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science China materials 2021年第12期64卷 3059-3068页

作者： Jiahui Huang Peiyi Wu State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular Science and Laboratory for Advanced MaterialsFudan UniversityShanghai 200433China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of ChemistryChemical Engineering and BiotechnologyCenter for Advanced Low-Dimension MaterialsDonghua UniversityShanghai 201620China

The advancement of technology has had a profound impact on all areas of life, with an ever more intimate integration of the digital and biological spheres, but it may also be accompanied by an environmental crisis caused by the abuse of large quantities of electronics and ***-generation "green" electronics or iontronics with high biocompatibility, biodegradation, low cost and mechanical compliance promise to mitigate these adverse effects, but are often limited by the finite choices of materials and ***, maltose syrup, a traditional water-dissolvable saccharide food called "JiaoJiao" in Chinese, is engineered to replace unsustainable conductive components of current electronic devices. After churning and pulling with two chopsticks, known as aeration, the aerated maltose syrup has optimized viscoelasticity, mechanical adaptation, robustness,remodeling and self-healing capability, yet with transient behavior. Moreover, the structural and viscoelastic evolution during aeration is also analyzed to maximize the contribution from structures. As a proof-of-concept, a type of "green" skinlike iontronics is prepared, which exhibits reliable strain sensing ability and is subsequently applied for intelligent information encryption and transmission based on a novel concept of sending Morse code. This work greatly extends the current material choice and is expected to shed light on the development of a sustainable future.

关键词： green electronics skin-like iontronics sustainable viscoelastic transient electronics

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Reduced recombination via tunable surface fields in perovskite thin films (aprl, 10.1038/s41560-024-01470-5, 2024)

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NATURE ENERGY 2024年第6期9卷 762-762页

作者： deQuilettes, Dane W. Yoo, Jason J. Brenes, Roberto Kosasih, Felix Utama Laitz, Madeleine Dou, Benjia Dak Graham, Daniel J. Ho, Kevin Shi, Yangwei Shin, Seong Sik Ducati, Caterina Bawendi, Moungi G. Bulovic, Vladimir Massachusetts Institute of Technology Research Laboratory of Electronics Cambridge USA (GRID:grid.116068.8) (ISNI:0000 0001 2341 2786) Massachusetts Institute of Technology Department of Chemistry Cambridge USA (GRID:grid.116068.8) (ISNI:0000 0001 2341 2786) Division of Advanced Materials Korea Research Institute of Chemical Technology Daejeon Republic of Korea (GRID:grid.29869.3c) (ISNI:0000 0001 2296 8192) Massachusetts Institute of Technology Research Laboratory of Electronics Cambridge USA (GRID:grid.116068.8) (ISNI:0000 0001 2341 2786) Massachusetts Institute of Technology Department of Electrical Engineering and Computer Science Cambridge USA (GRID:grid.116068.8) (ISNI:0000 0001 2341 2786) University of Cambridge Department of Materials Science and Metallurgy Cambridge UK (GRID:grid.5335.0) (ISNI:0000 0001 2188 5934) University of Washington Department of Bioengineering Seattle USA (GRID:grid.34477.33) (ISNI:0000 0001 2298 6657) University of Washington Department of Chemistry Seattle USA (GRID:grid.34477.33) (ISNI:0000 0001 2298 6657) University of Washington Department of Chemistry Seattle USA (GRID:grid.34477.33) (ISNI:0000 0001 2298 6657) University of Washington Molecular Engineering and Sciences Institute Seattle USA (GRID:grid.34477.33) (ISNI:0000 0001 2298 6657) Division of Advanced Materials Korea Research Institute of Chemical Technology Daejeon Republic of Korea (GRID:grid.29869.3c) (ISNI:0000 0001 2296 8192) Sungkyunkwan University Department of Nano Engineering and Department of Nano Science and Technology SKKU Advanced Institute of Nanotechnology (SAINT) Suwon Republic of Korea (GRID:grid.264381.a) (ISNI:0000 0001 2181 989X) Sungkyunkwan University SKKU Institute of Energy Science and Technology (SIEST) Suwon Republic of Korea (GRID:grid.264381.a) (ISNI:0000 0001 2181 989X) Massachusetts Institute of Technology Department of Chemistry Cambridge USA (GRID:grid.116068.8) (ISNI:0000 0001 2341 2786)

The ability to reduce energy loss at semiconductor surfaces through passivation or surface field engineering is an essential step in the manufacturing of efficient photovoltaic (PV) and optoelectronic devices. Similarly, surface modification of emerging halide perovskites with quasi-two-dimensional (2D) heterostructures is now ubiquitous to achieve PV power conversion efficiencies (PCEs) >25%, yet a fundamental understanding to how these treatments function is still generally lacking. Here we use a unique combination of depth-sensitive nanoscale characterization techniques to uncover a tunable passivation strategy and mechanism found in perovskite PV devices that were the first to reach the >25% PCE milestone. Namely, treatment with hexylammonium bromide leads to the simultaneous formation of an iodide-rich 2D layer along with a Br halide gradient that extends from defective surfaces and grain boundaries into the bulk three-dimensional (3D) layer. This interface can be optimized to extend the charge carrier lifetime to record values >30 μs and to reduce interfacial recombination velocities to values as low as <7 cm s−*** et al. show that hexylammonium bromide forms an iodide-rich 2D structure and bromide gradient at the surface of 3D perovskite, both of which limit interfacial charge and energy losses in perovskite solar cells.

关键词： Passivation

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Electric field manipulation enhanced by strong spin-orbit coupling: promoting rare-earth ions as qubits

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National science Review 2020年第10期7卷 1557-1563页

作者： Zheng Liu Ye-Xin Wang Yu-Hui Fang Si-Xue Qin Zhe-Ming Wang Shang-Da Jiang Song Gao Beijing National Laboratory of Molecular Science State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsBeijing Key Laboratory of Magnetoelectric Materials and Devices College of Chemistry and Molecular Engineering Peking University Department of Physics Chongqing University Beijing Academy of Quantum Information Sciences School of Chemistry and Chemical Engineering South China University of Technology

Quantum information processing based on magnetic ions has potential for applications as the ions can be modified in their electronic properties and assembled by a variety of chemical methods. For these systems to achieve individual spin addressability and high energy efficiency, we exploited the electric field as a tool to manipulate the quantum behaviours of the rare-earth ion which has strong spin-orbit coupling. A Ce:YAG single crystal was employed with considerations to the dynamics and the symmetry requirements. The Stark effect of the Ce;ion was observed and measured. When demonstrated as a quantum phase gate, the electric field manipulation exhibited high efficiency which allowed up to 57 π/2 operations before decoherence with optimized field direction. It was also utilized to carry out quantum bang-bang control, as a method of dynamic decoupling, and the refined Deutsch-Jozsa algorithm. Our experiments highlighted rare-earth ions as potentially applicable qubits because they offer enhanced spin-electric coupling which enables high-efficiency quantum manipulation.

关键词： quantum coherent manipulation spin-orbit coupling spin-electric coupling rare-earth ions qubits

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Cascaded Charge-Transfer Organic Alloys for the Controlled Hierarchical Self-Assembly of Low-Dimensional Heterostructures

SSRN

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SSRN 2023年

作者： Su, Yang Zhuo, Ming-Peng Wu, Bin Zhao, Yu-Dong Chen, Min Wang, Zuo-Shan Wang, Xue-Dong College of Chemistry Chemical Engineering and Materials Science Soochow University Jiangsu Suzhou215123 China Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices Soochow University Jiangsu Suzhou215123 China College of Textile and Clothing Engineering Soochow University Jiangsu Suzhou215123 China Department of Materials Science State Key Laboratory of Molecular Engineering of Polymers Fudan University Shanghai200433 China

Organic alloys integrating intrinsic alloys characters and organic semiconductor advantages demonstrate the multi-component synergistic and collective effects for possessing more desirable structural or functional properties. However, their finely rational design and the controlled self-assembly of their corresponding heterostructure materials remain yet to be explored. Herein, we successfully fabricated the novel organic CT alloys with tunable energy structures and the hierarchical heterostructures via a self-assembly process of the cascade CT interaction, which is rationally designed by finely regulating the weak electron donation and affinity of isomorphic 1,2,4,5-tetracyanobenzene (TCNB)-based CT complexes. The high chemical/structural compatibility between isomorphic CT complexes and their alloys is conducive to the excellent lattice matching requirement for the precise preparation of the triblock or core/shell-type organic heterostructures via the sequential or stepwise self-assembly processes. Impressively, these as-prepared organic heterostructures achieve the controlled exciton conversion and the tunable active/passive photon propagation modes, benefiting for the optical logic gate with nanoscale multiple input/out. Significantly, this strategy could be generalized to other organic CT alloys and hierarchical heterostructures, affording fresh comprehension to materials foundation for integrated optoelectronics. © 2023, The Authors. All rights reserved.

关键词： Charge transfer

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Regioselectively electrochemical C_sp3-H alkoxylation for functionalized indanone

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Green Synthesis and Catalysis 2025年

作者： Guo, Xue-Yang Yao, Bo-Xuan Wen, Li-Rong Guo, Weisi Li, Ming Ni, Shao-Fei Zhang, Lin-Bao State Key Laboratory Base of Eco-Chemical Engineering College of Chemistry and Molecular Engineering Qingdao University of Science & Technology Qingdao 266042 China Department of Chemistry and Key Laboratory for Preparation and Application of Ordered Structural Materials of Guangdong Province Shantou University Shantou 515063 China

An electrochemical regioselective Csp3-H alkoxylation has been developed to synthesize functionalized 1-indanone. In this process, electricity serves as the formal terminal oxidant, while the molecular hydrogen produc... 详细信息

An electrochemical regioselective C_sp3-H alkoxylation has been developed to synthesize functionalized 1-indanone. In this process, electricity serves as the formal terminal oxidant, while the molecular hydrogen produced by cathodic proton reduction acts as the sole by-product. This setup optimizes the economics of the oxidizing agent and contributes to the efficient production of valuable functionalized indanone. The use of mild reaction conditions and high regioselectivity makes the process highly practical. Furthermore, functionalized indanones can be synthesized through a one-pot method that involves the continuous oxidation of indan. The methodology can be easily executed on a gram scale, underscoring its potential applications. © 2024 Fudan University

关键词： Alkoxylation Electrocatalysis Functionalized indanone Metal-free Regioselective

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