Pub Date : 2024-05-15DOI: 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.
{"title":"Tuning water-cellulose interactions via copper-coordinated mercerization for hydro-actuated, shape-memory cellulosic hydroplastics","authors":"Zhi Zeng, Le Yu, Shanchen Yang, Kunkun Guo, Chao Xu, Chaoji Chen, Zhaohui Wang","doi":"10.1016/j.matt.2024.04.033","DOIUrl":"https://doi.org/10.1016/j.matt.2024.04.033","url":null,"abstract":"<p>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 Cu<sup>2+</sup>-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.</p>","PeriodicalId":388,"journal":{"name":"Matter","volume":null,"pages":null},"PeriodicalIF":18.9,"publicationDate":"2024-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140949651","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}
Pub Date : 2024-05-15DOI: 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.
{"title":"Integration of kinks and creases enables tunable folding in meta-ribbons","authors":"Weicheng Huang, Tian Yu, K. Jimmy Hsia, Sigrid Adriaenssens, Mingchao Liu","doi":"10.1016/j.matt.2024.04.031","DOIUrl":"https://doi.org/10.1016/j.matt.2024.04.031","url":null,"abstract":"<p>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.</p>","PeriodicalId":388,"journal":{"name":"Matter","volume":null,"pages":null},"PeriodicalIF":18.9,"publicationDate":"2024-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140949569","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}
Pub Date : 2024-05-14DOI: 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.
{"title":"ChemOS 2.0: An orchestration architecture for chemical self-driving laboratories","authors":"Malcolm Sim, Mohammad Ghazi Vakili, Felix Strieth-Kalthoff, Han Hao, Riley J. Hickman, Santiago Miret, Sergio Pablo-García, Alán Aspuru-Guzik","doi":"10.1016/j.matt.2024.04.022","DOIUrl":"https://doi.org/10.1016/j.matt.2024.04.022","url":null,"abstract":"<p>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 <em>ab initio</em> 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.</p>","PeriodicalId":388,"journal":{"name":"Matter","volume":null,"pages":null},"PeriodicalIF":18.9,"publicationDate":"2024-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140919980","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}
Pub Date : 2024-05-10DOI: 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.
{"title":"Protein dynamics inform protein structure: An interdisciplinary investigation of protein crystallization propensity","authors":"Mohammad Madani, Anna Tarakanova","doi":"10.1016/j.matt.2024.04.023","DOIUrl":"https://doi.org/10.1016/j.matt.2024.04.023","url":null,"abstract":"<p>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.</p>","PeriodicalId":388,"journal":{"name":"Matter","volume":null,"pages":null},"PeriodicalIF":18.9,"publicationDate":"2024-05-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140903391","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}
Pub Date : 2024-05-09DOI: 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.
{"title":"Post-synthesis tuning of dielectric constant via ferroelectric domain wall engineering","authors":"Lima Zhou, Lukas Puntigam, Peter Lunkenheimer, Edith Bourret, Zewu Yan, István Kézsmárki, Dennis Meier, Stephan Krohns, Jan Schultheiß, Donald M. Evans","doi":"10.1016/j.matt.2024.04.024","DOIUrl":"https://doi.org/10.1016/j.matt.2024.04.024","url":null,"abstract":"<p>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 ErMnO<sub>3</sub> 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 <em>in situ</em> tune the dielectric constant.</p>","PeriodicalId":388,"journal":{"name":"Matter","volume":null,"pages":null},"PeriodicalIF":18.9,"publicationDate":"2024-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140903031","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}
Pub Date : 2024-05-01DOI: 10.1016/j.matt.2024.04.005
Steve Cranford
{"title":"Want for nothing, need for null, useful output from negative results","authors":"Steve Cranford","doi":"10.1016/j.matt.2024.04.005","DOIUrl":"https://doi.org/10.1016/j.matt.2024.04.005","url":null,"abstract":"","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":"140816542","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}
Pub Date : 2024-05-01DOI: 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.
{"title":"Electrically induced directional ion migration in two-dimensional perovskite heterostructures","authors":"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","doi":"10.1016/j.matt.2024.03.005","DOIUrl":"10.1016/j.matt.2024.03.005","url":null,"abstract":"<div><p>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.</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":"140565758","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}
Pub Date : 2024-05-01DOI: 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。
{"title":"Photo-conversion of carbon monoxide with water and hydrogen: Lowering the carbon footprint of carbon monoxide valorization","authors":"Jiaqi Zhao , Zhenhua Li , Pu Wang , Peng Miao , Run Shi , Geoffrey I.N. Waterhouse , Li-Zhu Wu , Tierui Zhang","doi":"10.1016/j.matt.2024.02.013","DOIUrl":"https://doi.org/10.1016/j.matt.2024.02.013","url":null,"abstract":"<div><p>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 CO<sub>2</sub> formation, informing the rational design of new catalyst platforms and reactor designs for greener CO valorization with sunlight.</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":"140816622","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}
Pub Date : 2024-05-01DOI: 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 , 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","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}