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Tuning water-cellulose interactions via copper-coordinated mercerization for hydro-actuated, shape-memory cellulosic hydroplastics 通过铜配位丝光处理调节水与纤维素之间的相互作用,实现水动形状记忆纤维素水塑料
IF 18.9 1区 材料科学 Q1 Materials Science Pub Date : 2024-05-15 DOI: 10.1016/j.matt.2024.04.033
Zhi Zeng, Le Yu, Shanchen Yang, Kunkun Guo, Chao Xu, Chaoji Chen, Zhaohui Wang

Innovative biopolymers emulating natural organisms’ reversible water-induced deformations hold great potential across various domains. Here, we create a biopolymer that unifies actuation, hydrosetting, and shape-memory capabilities through copper-coordinated mercerization of nanocellulose paper. This method transforms the inherently hydrophilic, porous nanocellulose network into a compact amphiphilic membrane, distinguished by Cu2+-crosslinked hydrophobic domains acting as tough “net points,” ensuring exceptional water stability and ultrahigh wet mechanical performance (94.9 MPa and 3.50 GPa). Upon hydration, the membrane swiftly establishes reversible hydrogen-bonding “switches,” enabling a rapid plastic-elastic transition. The interplay between the net points and switches resolves the inherent trade-off between rapid, reversible hydrogen-bonding networks and mechanical robustness in cellulosic materials, thereby facilitating remarkable water-induced actuation, hydrosetting, and shape memory. Notably, the membrane demonstrates complex morphing and swift recovery in water, serving as a smart encrypted information carrier. Our study offers a molecular structural engineering paradigm for the rational design of advanced responsive materials.

仿效自然生物的可逆水诱导变形的创新生物聚合物在各个领域都具有巨大潜力。在这里,我们通过对纳米纤维素纸进行铜配位丝光处理,创造出了一种集驱动、水凝和形状记忆功能于一体的生物聚合物。这种方法将固有的亲水性多孔纳米纤维素网络转变成了一种紧凑的两亲膜,其特点是Cu2+交联的疏水域可作为坚韧的 "网点",确保了优异的水稳定性和超高的湿机械性能(94.9 兆帕和 3.50 千兆帕)。水化时,薄膜会迅速建立可逆的氢键 "开关",实现快速的塑性-弹性转换。网点和开关之间的相互作用解决了纤维素材料中快速、可逆氢键网络和机械坚固性之间固有的权衡问题,从而促进了显著的水诱导致动、水凝和形状记忆。值得注意的是,这层膜在水中具有复杂的变形和快速恢复能力,可作为智能加密信息载体。我们的研究为合理设计先进的响应材料提供了分子结构工程范例。
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引用次数: 0
Integration of kinks and creases enables tunable folding in meta-ribbons 将扭结和折痕整合在一起可实现元带的可调折叠
IF 18.9 1区 材料科学 Q1 Materials Science Pub Date : 2024-05-15 DOI: 10.1016/j.matt.2024.04.031
Weicheng Huang, Tian Yu, K. Jimmy Hsia, Sigrid Adriaenssens, Mingchao Liu

Foldable structures find diverse applications. Folding of thin structures into compact shapes involves the interplay of nonlinear mechanics and topology. In this study, we employ discrete models, theoretical analysis, and tabletop experiments to systematically investigate the geometrically nonlinear folding process of ring-shape elastic ribbons through in-plane kinks and out-of-plane creases. We find that kinks initiate continuous folding through supercritical bifurcation, while creases trigger abrupt snapping via subcritical bifurcation. Master curves that summarize energy landscapes for ribbons with varying numbers of kinks and creases are obtained. By integrating kinks and creases, a “meta-ribbon” can be created, which shows the tunable folding behavior, transitioning from continuous to snapping, or vice versa, by strategically engineering the in-plane and out-of-plane angles guided by the constructed energy map. As a product of folding, we demonstrate the snapping-induced vibration accomplished with dynamic folding, as well as the multistability of meta-ribbons with saddle-like configurations and their transformation.

可折叠结构的应用多种多样。将薄结构折叠成紧凑形状涉及非线性力学和拓扑学的相互作用。在这项研究中,我们采用离散模型、理论分析和桌面实验,系统地研究了环形弹性带通过平面内扭结和平面外折痕的几何非线性折叠过程。我们发现,扭结通过超临界分岔引发连续折叠,而折痕则通过亚临界分岔引发突然折断。我们还获得了主曲线,该曲线概括了具有不同数量折痕和折皱的带的能量景观。通过整合扭结和折痕,可以创建一个 "元带",它显示了可调的折叠行为,在所构建的能量图的指导下,通过对平面内和平面外角度的战略性工程设计,可以从连续过渡到折断,反之亦然。作为折叠的产物,我们展示了通过动态折叠实现的由折断引起的振动,以及具有鞍状构型的元带的多态性及其转变。
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引用次数: 0
ChemOS 2.0: An orchestration architecture for chemical self-driving laboratories ChemOS 2.0:化学自驱动实验室的协调架构
IF 18.9 1区 材料科学 Q1 Materials Science Pub Date : 2024-05-14 DOI: 10.1016/j.matt.2024.04.022
Malcolm Sim, Mohammad Ghazi Vakili, Felix Strieth-Kalthoff, Han Hao, Riley J. Hickman, Santiago Miret, Sergio Pablo-García, Alán Aspuru-Guzik

Self-driving laboratories (SDLs), which combine automated experimental hardware with computational experiment planning, have emerged as powerful tools for accelerating materials discovery. The intrinsic complexity created by their multitude of components requires an effective orchestration platform to ensure the correct operation of diverse experimental setups. Existing orchestration frameworks, however, are either tailored to specific setups or have not been implemented for real-world synthesis. To address these issues, we introduce ChemOS 2.0, an orchestration architecture that efficiently coordinates communication, data exchange, and instruction management among modular laboratory components. By treating the laboratory as an “operating system,” ChemOS 2.0 combines ab initio calculations, experimental orchestration, and statistical algorithms to guide closed-loop operations. To demonstrate its capabilities, we showcase ChemOS 2.0 in a case study focused on discovering organic laser molecules. The results confirm ChemOS 2.0’s prowess in accelerating materials research and demonstrate its potential as a valuable design for future SDL platforms.

自动驾驶实验室(SDL)结合了自动化实验硬件和计算实验计划,已成为加速材料发现的强大工具。其众多组件造成的内在复杂性需要一个有效的协调平台来确保各种实验装置的正确运行。然而,现有的协调框架要么是为特定设置量身定制的,要么尚未在实际合成中实施。为了解决这些问题,我们推出了 ChemOS 2.0,这是一种协调架构,可有效协调模块化实验室组件之间的通信、数据交换和指令管理。通过将实验室视为 "操作系统",ChemOS 2.0 将原子序数计算、实验协调和统计算法结合起来,指导闭环操作。为了展示ChemOS 2.0的能力,我们在一个以发现有机激光分子为重点的案例研究中展示了ChemOS 2.0。研究结果证实了ChemOS 2.0在加速材料研究方面的能力,并证明了它作为未来SDL平台的重要设计的潜力。
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引用次数: 0
Protein dynamics inform protein structure: An interdisciplinary investigation of protein crystallization propensity 蛋白质动力学为蛋白质结构提供信息:蛋白质结晶倾向的跨学科研究
IF 18.9 1区 材料科学 Q1 Materials Science Pub Date : 2024-05-10 DOI: 10.1016/j.matt.2024.04.023
Mohammad Madani, Anna Tarakanova

The classical central paradigm of structural biology links a protein’s sequence to its structure and function but overlooks conformational fluctuation that is integral to protein function. We propose a graph neural network model based on gated attention that explicitly incorporates protein dynamics via physics-based models to predict protein crystallization propensity. We compare results to all-atom molecular dynamics simulations of flexible, disordered human tropoelastin and ordered, globular human lysyl oxidase-like protein. Our findings show that fluctuating residues correlate with locally maximal attention scores in the neural network. By methodically truncating the sequences, we establish correlations between dynamical and physicochemical molecular properties and protein crystallization propensity. Accounting for comprehensive biological mechanisms, our tool can facilitate the rational design of protein sequences that lead to diffraction-quality crystals. Our study showcases the integration of physics-based and machine learning models for structure and property prediction, expanding the classical paradigm of structural biology.

结构生物学的经典核心范式将蛋白质序列与其结构和功能联系起来,但忽略了与蛋白质功能密不可分的构象波动。我们提出了一种基于门控注意力的图神经网络模型,该模型通过基于物理的模型明确地将蛋白质动力学纳入其中,从而预测蛋白质的结晶倾向。我们将结果与灵活、无序的人 tropoelastin 和有序、球状的人赖氨酸氧化酶样蛋白的全原子分子动力学模拟结果进行了比较。我们的研究结果表明,波动残基与神经网络中局部最大注意力得分相关。通过有条不紊地截断序列,我们建立了动态和物理化学分子特性与蛋白质结晶倾向之间的相关性。考虑到全面的生物机制,我们的工具有助于合理设计蛋白质序列,从而获得衍射质量的晶体。我们的研究展示了基于物理学和机器学习的结构与性质预测模型的整合,拓展了结构生物学的经典范式。
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引用次数: 0
Post-synthesis tuning of dielectric constant via ferroelectric domain wall engineering 通过铁电畴壁工程在合成后调整介电常数
IF 18.9 1区 材料科学 Q1 Materials Science Pub Date : 2024-05-09 DOI: 10.1016/j.matt.2024.04.024
Lima Zhou, Lukas Puntigam, Peter Lunkenheimer, Edith Bourret, Zewu Yan, István Kézsmárki, Dennis Meier, Stephan Krohns, Jan Schultheiß, Donald M. Evans

A promising mechanism for achieving colossal dielectric constants involves the use of insulating internal barrier layers, such as insulating domain walls in ferroelectrics. A key advantage of domain walls, compared to other stationary interfaces, is their mobility, offering the potential for post-synthesis adjustment of the dielectric constant. In this work, we demonstrate that altering the domain wall density enables the tuning of the dielectric constant in our template material, i.e., hexagonal ErMnO3 single crystals. Through microscopy and macroscopic dielectric spectroscopy, we quantify changes in domain wall density and correlated these with changes in dielectric constant within a single sample. Analysis of the dielectric data suggests that the insulating domain walls act as “ideal” capacitors connected in series. Our approach to engineering the domain wall density can be readily extended to other control methods, e.g., electric fields or mechanical stresses, providing a degree of flexibility to in situ tune the dielectric constant.

实现超大介电常数的一个可行机制是使用绝缘内部阻挡层,如铁电中的绝缘畴壁。与其他固定界面相比,畴壁的一个关键优势在于其流动性,为合成后调整介电常数提供了可能性。在这项工作中,我们证明了改变畴壁密度可以调整模板材料(即六方 ErMnO3 单晶)的介电常数。通过显微镜和宏观介电光谱,我们量化了畴壁密度的变化,并将其与单个样品中介电常数的变化联系起来。对介电数据的分析表明,绝缘畴壁就像一个串联的 "理想 "电容器。我们设计畴壁密度的方法可以很容易地扩展到其他控制方法,如电场或机械应力,从而为原位调节介电常数提供了一定程度的灵活性。
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引用次数: 0
A reconfigurable monolith chip-type microwave gas sensor for ultrasensitive NH3 detection 用于超灵敏 NH3 检测的可重构单片芯片式微波气体传感器
IF 18.9 1区 材料科学 Q1 Materials Science Pub Date : 2024-05-01 DOI: 10.1016/j.matt.2024.04.040
Juhua Xu, Jian Qi, Chang Xu, Nan Zhang, Renshuo Wang, Xin Xu, Ke Wang, Quan Jin, Xiaolong Wang, Geyu Lu
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引用次数: 0
Want for nothing, need for null, useful output from negative results 不求有功,但求无过,从负面结果中获得有益产出
IF 18.9 1区 材料科学 Q1 Materials Science Pub Date : 2024-05-01 DOI: 10.1016/j.matt.2024.04.005
Steve Cranford
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引用次数: 0
Electrically induced directional ion migration in two-dimensional perovskite heterostructures 二维过氧化物异质结构中的电诱导离子定向迁移
IF 18.9 1区 材料科学 Q1 Materials Science Pub Date : 2024-05-01 DOI: 10.1016/j.matt.2024.03.005
Jee Yung Park , Yoon Ho Lee , Md Asaduz Zaman Mamun , Mir Md Fahimul Islam , Shuchen Zhang , Ke Ma , Aalok Uday Gaitonde , Kang Wang , Seok Joo Yang , Amy Marconnet , Jianguo Mei , Muhammad Ashraful Alam , Letian Dou

Understanding ion migration in two-dimensional (2D) perovskite materials is key to enhancing halide perovskite device performance and stability. However, prior studies have been primarily limited to heat- and light-induced ion migration. In this work, to investigate electrically induced ion migration in 2D perovskites, we construct a high-quality, single-crystal, 2D perovskite heterostructure device platform with near-defect-free van der Waals contact. While achieving real-time visualization of halide anions migrating toward the positive bias, defined here as directional ion migration, we also uncover the unique behavior of halide anions interdiffusing toward the opposite direction under prolonged bias. Confocal microscopy imaging reveals a halide migration channel that aligns with the crystal and heterojunction edges. After a sustained ion migration, stable junction diodes exhibiting an up to ∼1,000-fold forward-to-reverse current ratio are realized. This study unveils important fundamental insights into halide migration under electrical bias, paving the way toward high-performance devices.

了解二维(2D)包晶材料中的离子迁移是提高卤化物包晶器件性能和稳定性的关键。然而,之前的研究主要局限于热和光诱导的离子迁移。在这项工作中,为了研究二维过氧化物中电诱导的离子迁移,我们构建了一个具有近乎无缺陷范德华接触的高质量单晶二维过氧化物异质结构器件平台。在实现卤化阴离子向正偏压方向迁移(此处定义为离子定向迁移)的实时可视化的同时,我们还发现了卤化阴离子在长时间偏压下向相反方向相互扩散的独特行为。共聚焦显微镜成像显示了与晶体和异质结边缘一致的卤化物迁移通道。经过持续的离子迁移,实现了稳定的结二极管,其正向与反向电流比高达 1,000 倍。这项研究揭示了电偏压下卤化物迁移的重要基本观点,为实现高性能器件铺平了道路。
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引用次数: 0
Photo-conversion of carbon monoxide with water and hydrogen: Lowering the carbon footprint of carbon monoxide valorization 一氧化碳与水和氢的光电转换:降低一氧化碳价值化的碳足迹
IF 18.9 1区 材料科学 Q1 Materials Science Pub Date : 2024-05-01 DOI: 10.1016/j.matt.2024.02.013
Jiaqi Zhao , Zhenhua Li , Pu Wang , Peng Miao , Run Shi , Geoffrey I.N. Waterhouse , Li-Zhu Wu , Tierui Zhang

Artificial photo-synthetic carbon fixation utilizing eco-friendly feedstocks, renewable solar energy, and innovative reaction pathways offers a promising route for lowering the carbon footprint of chemical production. Compared to conventional thermal catalytic processes, CO photo-conversion offers many advantages including low-energy-input requirements, reduced infrastructure requirements, and enhanced selectivity for value-added products. Substantial progress has been made recently in the design of catalysts with high activity and selectivity for photo-driven CO conversion with water (water-gas shift) and hydrogen (Fischer-Tropsch synthesis). This perspective overviews these exciting recent advances, describing how CO photo-conversion could potentially contribute to a sustainable chemical manufacturing industry with a low carbon footprint. We dissect the challenges of CO photo-conversion technologies based on green reactant production strategies, improved solar-to-chemical energy conversion efficiencies, and strategies to circumvent CO2 formation, informing the rational design of new catalyst platforms and reactor designs for greener CO valorization with sunlight.

利用生态友好型原料、可再生太阳能和创新反应途径进行人工光合成碳固定,为降低化学品生产的碳足迹提供了一条前景广阔的途径。与传统的热催化过程相比,一氧化碳光转化具有许多优势,包括低能耗输入要求、减少基础设施要求以及提高增值产品的选择性。最近,在设计具有高活性和高选择性的催化剂方面取得了重大进展,这些催化剂可用于水(水气变换)和氢(费托合成)的光驱动 CO 转化。本视角概述了这些令人振奋的最新进展,描述了一氧化碳光转化如何为低碳足迹的可持续化学制造业做出潜在贡献。我们剖析了一氧化碳光转化技术所面临的挑战,这些挑战基于绿色反应物生产策略、改进的太阳能到化学能的转换效率以及规避二氧化碳形成的策略,为合理设计新催化剂平台和反应器设计提供了信息,从而利用阳光实现更绿色的一氧化碳价值化。
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引用次数: 0
Heterojunction structure of cobalt sulfide cathodes for high-performance magnesium-ion batteries 用于高性能镁离子电池的硫化钴阴极的异质结结构
IF 18.9 1区 材料科学 Q1 Materials Science Pub Date : 2024-05-01 DOI: 10.1016/j.matt.2024.03.008
Jianbiao Wang , Tanmay Ghosh , Zhengyu Ju , Man-Fai Ng , Gang Wu , Gaoliang Yang , Xiaofei Zhang , Lei Zhang , Albertus D. Handoko , Sonal Kumar , Wutthikrai Busayaporn , Dechmongkhon Kaewsuwan , Changyun Jiang , Mingdeng Wei , Guihua Yu , Zhi Wei Seh

Transition metal chalcogenides (TMCs) with 3d orbitals have been intensively studied for use as cathodes in magnesium-ion batteries. However, their poor electronic conductivities and sluggish electrochemical kinetics severely restrict their electrochemical performance, preventing wide applicability for these materials. Here, we propose a heterointerface structure of cobalt sulfide (Co3S4/CoS2) hollow nanospheres to enable built-in electric fields generated in heterointerfaces, as verified in density functional theory, finite-element simulations, and ab initio molecular dynamics results. Compared to other TMCs, our cathode exhibited a substantial capacity of 597 mAh g−1 after 120 cycles at 50 mA g−1. When evaluated in a pouch cell, the electrode can sustain 100 deep cycles at 40 mA g−1 with an energy density of 203 Wh kg−1 that displays potential for practical applications. Finally, rational heterostructure engineering of transition-metal-based sulfides provides insights into developing cathodes for high-performance sustainable Mg batteries.

为了在镁离子电池中用作阴极,人们对具有 3d 轨道的过渡金属瑀(TMCs)进行了深入研究。然而,它们较差的电子传导性和迟缓的电化学动力学严重限制了它们的电化学性能,阻碍了这些材料的广泛应用。在此,我们提出了一种硫化钴(Co3S4/CoS2)空心纳米球的异质界面结构,以实现异质界面中产生的内置电场,密度泛函理论、有限元模拟和 ab initio 分子动力学结果都验证了这一点。与其他 TMC 相比,我们的阴极在 50 mA g-1 的条件下循环 120 次后显示出 597 mAh g-1 的巨大容量。在袋式电池中进行评估时,该电极可以在 40 mA g-1 的条件下维持 100 次深度循环,能量密度为 203 Wh kg-1,具有实际应用的潜力。最后,过渡金属硫化物的合理异质结构工程为开发高性能可持续镁电池阴极提供了启示。
{"title":"Heterojunction structure of cobalt sulfide cathodes for high-performance magnesium-ion batteries","authors":"Jianbiao Wang ,&nbsp;Tanmay Ghosh ,&nbsp;Zhengyu Ju ,&nbsp;Man-Fai Ng ,&nbsp;Gang Wu ,&nbsp;Gaoliang Yang ,&nbsp;Xiaofei Zhang ,&nbsp;Lei Zhang ,&nbsp;Albertus D. Handoko ,&nbsp;Sonal Kumar ,&nbsp;Wutthikrai Busayaporn ,&nbsp;Dechmongkhon Kaewsuwan ,&nbsp;Changyun Jiang ,&nbsp;Mingdeng Wei ,&nbsp;Guihua Yu ,&nbsp;Zhi Wei Seh","doi":"10.1016/j.matt.2024.03.008","DOIUrl":"10.1016/j.matt.2024.03.008","url":null,"abstract":"<div><p>Transition metal chalcogenides (TMCs) with 3d orbitals have been intensively studied for use as cathodes in magnesium-ion batteries. However, their poor electronic conductivities and sluggish electrochemical kinetics severely restrict their electrochemical performance, preventing wide applicability for these materials. Here, we propose a heterointerface structure of cobalt sulfide (Co<sub>3</sub>S<sub>4</sub>/CoS<sub>2</sub>) hollow nanospheres to enable built-in electric fields generated in heterointerfaces, as verified in density functional theory, finite-element simulations, and <em>ab initio</em> molecular dynamics results. Compared to other TMCs, our cathode exhibited a substantial capacity of 597 mAh g<sup>−1</sup> after 120 cycles at 50 mA g<sup>−1</sup>. When evaluated in a pouch cell, the electrode can sustain 100 deep cycles at 40 mA g<sup>−1</sup> with an energy density of 203 Wh kg<sup>−1</sup> that displays potential for practical applications. Finally, rational heterostructure engineering of transition-metal-based sulfides provides insights into developing cathodes for high-performance sustainable Mg batteries.</p></div>","PeriodicalId":388,"journal":{"name":"Matter","volume":null,"pages":null},"PeriodicalIF":18.9,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140595661","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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