Pub Date : 2024-11-15DOI: 10.1016/j.matt.2024.10.016
Xiaoyu Hou, Kaiyue Zhang, Xintao Lai, Liwei Hu, Florian Vogelbacher, Yanlin Song, Lei Jiang, Mingzhu Li
Passive daytime radiative cooling is regarded as a promising technology to achieve all-day subambient cooling without energy consumption and pollution. The installation of monotonous white radiative cooling coating on the facades of buildings poses challenges in terms of aesthetic integration. Fabricating radiative cooling coatings with different colors and high cooling efficiency at a low cost is an optimal solution for their broad adoption and commercialization. Here, inspired by the elytra of the scarab beetle, we design a hierarchically porous nested structured radiative cooling film with high subambient cooling efficiency and flexible color tunability. This film exhibits both high solar reflectance (93.4%) and superior thermal emissivity (92.3%), realizing subambient cooling of ∼10.2°C at night and ∼7.2°C at midday. Its color is brilliant, stable, and flexible. Additionally, this film is self-cleaning and can reduce noise, which suggests possibilities for the development of multifunctional radiative cooling surfaces in building envelopes, automobile coatings, and clothes.
{"title":"Brilliant colorful daytime radiative cooling coating mimicking scarab beetle","authors":"Xiaoyu Hou, Kaiyue Zhang, Xintao Lai, Liwei Hu, Florian Vogelbacher, Yanlin Song, Lei Jiang, Mingzhu Li","doi":"10.1016/j.matt.2024.10.016","DOIUrl":"https://doi.org/10.1016/j.matt.2024.10.016","url":null,"abstract":"Passive daytime radiative cooling is regarded as a promising technology to achieve all-day subambient cooling without energy consumption and pollution. The installation of monotonous white radiative cooling coating on the facades of buildings poses challenges in terms of aesthetic integration. Fabricating radiative cooling coatings with different colors and high cooling efficiency at a low cost is an optimal solution for their broad adoption and commercialization. Here, inspired by the elytra of the scarab beetle, we design a hierarchically porous nested structured radiative cooling film with high subambient cooling efficiency and flexible color tunability. This film exhibits both high solar reflectance (93.4%) and superior thermal emissivity (92.3%), realizing subambient cooling of ∼10.2°C at night and ∼7.2°C at midday. Its color is brilliant, stable, and flexible. Additionally, this film is self-cleaning and can reduce noise, which suggests possibilities for the development of multifunctional radiative cooling surfaces in building envelopes, automobile coatings, and clothes.","PeriodicalId":388,"journal":{"name":"Matter","volume":"46 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637609","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 : 2024-11-12DOI: 10.1016/j.matt.2024.10.024
Yunna Guo, Hantao Cui, Peng Jia, Zhangran Ye, Lei Deng, Hui Li, Baiyu Guo, Xuedong Zhang, Jie Huang, Yong Su, Jianyu Huang, Bin Wen, Yang Lu, Liqiang Zhang
(Matter 7, ◼◼◼–◼◼◼; December 4, 2024)
(事项 7，◼◼◼-◼◼◼；2024 年 12 月 4 日）
{"title":"Nanoscale cold welding of glass","authors":"Yunna Guo, Hantao Cui, Peng Jia, Zhangran Ye, Lei Deng, Hui Li, Baiyu Guo, Xuedong Zhang, Jie Huang, Yong Su, Jianyu Huang, Bin Wen, Yang Lu, Liqiang Zhang","doi":"10.1016/j.matt.2024.10.024","DOIUrl":"https://doi.org/10.1016/j.matt.2024.10.024","url":null,"abstract":"(Matter <em>7</em>, ◼◼◼–◼◼◼; December 4, 2024)","PeriodicalId":388,"journal":{"name":"Matter","volume":"16 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142601770","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 : 2024-11-12DOI: 10.1016/j.matt.2024.10.015
Kourosh Darvish, Marta Skreta, Yuchi Zhao, Naruki Yoshikawa, Sagnik Som, Miroslav Bogdanovic, Yang Cao, Han Hao, Haoping Xu, Alán Aspuru-Guzik, Animesh Garg, Florian Shkurti
Chemistry experiments can be resource- and labor-intensive, often requiring manual tasks like polishing electrodes in electrochemistry. Traditional lab automation infrastructure faces challenges adapting to new experiments. To address this, we introduce ORGANA, an assistive robotic system that automates diverse chemistry experiments using decision-making and perception tools. It makes decisions with chemists in the loop to control robots and lab devices. ORGANA interacts with chemists using large language models (LLMs) to derive experiment goals, handle disambiguation, and provide experiment logs. ORGANA plans and executes complex tasks with visual feedback while supporting scheduling and parallel task execution. We demonstrate ORGANA’s capabilities in solubility, pH measurement, recrystallization, and electrochemistry experiments. In electrochemistry, it executes a 19-step plan in parallel to characterize quinone derivatives for flow batteries. Our user study shows ORGANA reduces frustration and physical demand by over 50%, with users saving an average of 80.3% of their time when using it.
{"title":"ORGANA: A robotic assistant for automated chemistry experimentation and characterization","authors":"Kourosh Darvish, Marta Skreta, Yuchi Zhao, Naruki Yoshikawa, Sagnik Som, Miroslav Bogdanovic, Yang Cao, Han Hao, Haoping Xu, Alán Aspuru-Guzik, Animesh Garg, Florian Shkurti","doi":"10.1016/j.matt.2024.10.015","DOIUrl":"https://doi.org/10.1016/j.matt.2024.10.015","url":null,"abstract":"Chemistry experiments can be resource- and labor-intensive, often requiring manual tasks like polishing electrodes in electrochemistry. Traditional lab automation infrastructure faces challenges adapting to new experiments. To address this, we introduce ORGANA, an assistive robotic system that automates diverse chemistry experiments using decision-making and perception tools. It makes decisions with chemists in the loop to control robots and lab devices. ORGANA interacts with chemists using large language models (LLMs) to derive experiment goals, handle disambiguation, and provide experiment logs. ORGANA plans and executes complex tasks with visual feedback while supporting scheduling and parallel task execution. We demonstrate ORGANA’s capabilities in solubility, pH measurement, recrystallization, and electrochemistry experiments. In electrochemistry, it executes a 19-step plan in parallel to characterize quinone derivatives for flow batteries. Our user study shows ORGANA reduces frustration and physical demand by over 50%, with users saving an average of 80.3% of their time when using it.","PeriodicalId":388,"journal":{"name":"Matter","volume":"95 1","pages":""},"PeriodicalIF":18.9,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142599874","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 : 2024-11-06DOI: 10.1016/j.matt.2024.08.008
Yaning Ma , Zihan Zhao , Zhiran Zheng , Jiawei Li , Min-Hui Li , Jun Hu
Polymers constructed from natural thioctic acid (TA) provide a solution for the development of sustainable materials. However, their inherent weak networks make them difficult to use in engineering materials featuring high durability and mechanical robustness. In this work, the autocatalytic dual-dynamic covalent adaptable networks (CANs) are devised by curing diglycidyl 4,5-epoxycyclohexane-1,2-dicarboxylate (DGEDC) with TA and bis(p-aminocyclohexyl)methane (PACM). The resulting DGEDC/TA/PACM thermosets exhibit good mechanical and thermal properties (Tg of 145°C, Td5% of 289°C, tensile strength of 70 MPa, Young’s modulus of 2.25 GPa), higher than previous poly(thioctic acid)-based materials. Due to topological network rearrangements induced by the exchange of disulfide bonds and tertiary amine-catalyzed transesterification reactions, they can be easily reshaped and repaired. Furthermore, they can be degraded mildly and upcycled into polyurethane foam by in situ foaming. This strategy of autocatalytic dual-dynamic CANs will inspire the development of practical applications of poly(thioctic acid).
由天然硫辛酸（TA）制成的聚合物为开发可持续材料提供了一种解决方案。然而，其固有的弱网络使其难以用于具有高耐久性和机械坚固性的工程材料。在这项工作中，通过将 4,5-环氧环己烷-1,2-二甲酸二缩水甘油酯（DGEDC）与 TA 和双（对氨基环己基）甲烷（PACM）固化，设计出了自催化双动力共价适应网络（CANs）。由此产生的 DGEDC/TA/PACM 热固性材料具有良好的机械性能和热性能（Tg 为 145°C，Td5% 为 289°C，拉伸强度为 70 兆帕，杨氏模量为 2.25 GPa），高于以前的聚硫辛酸基材料。由于二硫键交换和叔胺催化的酯交换反应引起的拓扑网络重排，它们可以很容易地重塑和修复。此外，它们还能被温和降解，并通过原位发泡被再生为聚氨酯泡沫。这种自催化双动力 CAN 的策略将为聚硫辛酸的实际应用开发带来启发。
{"title":"High-performance poly(thioctic acid)-based thermosets featuring upcycling ability for in situ foaming enabled by dual-dynamic networks","authors":"Yaning Ma , Zihan Zhao , Zhiran Zheng , Jiawei Li , Min-Hui Li , Jun Hu","doi":"10.1016/j.matt.2024.08.008","DOIUrl":"10.1016/j.matt.2024.08.008","url":null,"abstract":"<div><div>Polymers constructed from natural thioctic acid (TA) provide a solution for the development of sustainable materials. However, their inherent weak networks make them difficult to use in engineering materials featuring high durability and mechanical robustness. In this work, the autocatalytic dual-dynamic covalent adaptable networks (CANs) are devised by curing diglycidyl 4,5-epoxycyclohexane-1,2-dicarboxylate (DGEDC) with TA and bis(<em>p</em>-aminocyclohexyl)methane (PACM). The resulting DGEDC/TA/PACM thermosets exhibit good mechanical and thermal properties (<em>T</em><sub><em>g</em></sub> of 145°C, <em>T</em><sub><em>d5%</em></sub> of 289°C, tensile strength of 70 MPa, Young’s modulus of 2.25 GPa), higher than previous poly(thioctic acid)-based materials. Due to topological network rearrangements induced by the exchange of disulfide bonds and tertiary amine-catalyzed transesterification reactions, they can be easily reshaped and repaired. Furthermore, they can be degraded mildly and upcycled into polyurethane foam by <em>in situ</em> foaming. This strategy of autocatalytic dual-dynamic CANs will inspire the development of practical applications of poly(thioctic acid).</div></div>","PeriodicalId":388,"journal":{"name":"Matter","volume":"7 11","pages":"Pages 4046-4058"},"PeriodicalIF":17.3,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142158695","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 : 2024-11-06DOI: 10.1016/j.matt.2024.08.002
Xun Guo , Hu Hong , Qing Li , Jiaxiong Zhu , Zhuoxi Wu , Yanbo Wang , Shuo Yang , Zhaodong Huang , Yan Huang , Nan Li , Chunyi Zhi
Rechargeable zinc metal batteries (ZMBs) are promising for fabricating low-cost, safe, and high-energy-density storage systems. However, ZMBs typically undergo interfacial side reactions and cathode dissolution during cycling, resulting in the depletion of active materials and performance decay of batteries. Here, we develop a localized high-concentration fluorinated electrolyte featuring a high fluorine/oxygen atomic ratio (388.72%) with beneficial solvation chemistry, fostering the simultaneous formation of a cathode-electrolyte interphase (CEI) enriched with C–F bonds and a ZnF2-dominant solid-electrolyte interphase (SEI). The constructed robust electrode-electrolyte interfaces (EEIs) contribute to dendrite-free zinc deposition and a highly stable cathode, demonstrating soft-packed Zn||Mn-doped V2O5 batteries with an exceptional energy density (91.25 Wh kg−1cathode+anode) and capacity retention (90.5%) over 500 cycles employing a limited zinc supply. The anode-free ZMBs deliver a record power density of 153.9 Wh kg−1cathode+anode with a high capacity retention of 80.2% over 1,500 cycles. This research provides significant insights for interface construction in multivalent ion batteries.
{"title":"Dual robust electrode-electrolyte interfaces enabled by fluorinated electrolyte for high-performance zinc metal batteries","authors":"Xun Guo , Hu Hong , Qing Li , Jiaxiong Zhu , Zhuoxi Wu , Yanbo Wang , Shuo Yang , Zhaodong Huang , Yan Huang , Nan Li , Chunyi Zhi","doi":"10.1016/j.matt.2024.08.002","DOIUrl":"10.1016/j.matt.2024.08.002","url":null,"abstract":"<div><div>Rechargeable zinc metal batteries (ZMBs) are promising for fabricating low-cost, safe, and high-energy-density storage systems. However, ZMBs typically undergo interfacial side reactions and cathode dissolution during cycling, resulting in the depletion of active materials and performance decay of batteries. Here, we develop a localized high-concentration fluorinated electrolyte featuring a high fluorine/oxygen atomic ratio (388.72%) with beneficial solvation chemistry, fostering the simultaneous formation of a cathode-electrolyte interphase (CEI) enriched with C–F bonds and a ZnF<sub>2</sub>-dominant solid-electrolyte interphase (SEI). The constructed robust electrode-electrolyte interfaces (EEIs) contribute to dendrite-free zinc deposition and a highly stable cathode, demonstrating soft-packed Zn||Mn-doped V<sub>2</sub>O<sub>5</sub> batteries with an exceptional energy density (91.25 Wh kg<sup>−1</sup><sub>cathode+anode</sub>) and capacity retention (90.5%) over 500 cycles employing a limited zinc supply. The anode-free ZMBs deliver a record power density of 153.9 Wh kg<sup>−1</sup><sub>cathode+anode</sub> with a high capacity retention of 80.2% over 1,500 cycles. This research provides significant insights for interface construction in multivalent ion batteries.</div></div>","PeriodicalId":388,"journal":{"name":"Matter","volume":"7 11","pages":"Pages 4014-4030"},"PeriodicalIF":17.3,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142221114","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 : 2024-11-06DOI: 10.1016/j.matt.2024.09.009
Yizhe Shao , Chao Dang , Haobo Qi , Ziyang Liu , Haoran Pei , Tongqing Lu , Wei Zhai
Eutectogels, consisting of three-dimensional polymeric networks saturated with deep eutectic solvents (DESs), present a promising option for soft ionic conductors. Instead of modifying polymer chains, we propose a new DES system comprising phytic acid (PA) and choline chloride (ChCl), which enhances dynamic and interactive bonding with polymeric networks to create innovative eutectogels. Here, we develop polyfunctional eutectogels (PETGs) by encapsulating polyvinyl alcohol (PVA) networks with our DES using an evaporation-induced confinement strategy. Experimental validation and numerical calculations demonstrate that PA forms high-density dynamic hydrogen bonds with PVA while shielding hydrogen bonds between PVA chains. This results in a multiple hydrogen-bond-shielded amorphous network (MHSN) with undetectable crystalline regions, thereby promoting ion migration to ensure high conductivity. Moreover, our PETG exhibits rapid self-healing, freeze resistance, self-adhesion, antibacterial properties, and dual sensitivities attributable to the MHSN. We demonstrate the potential of PETGs for applications in motion sensing, machine learning, human-machine interaction, and energy harvesting.
共晶凝胶由饱和深共晶溶剂（DES）的三维聚合物网络组成，是一种前景广阔的软离子导体。我们提出了一种由植酸（PA）和氯化胆碱（ChCl）组成的新型 DES 系统，而不是对聚合物链进行改性，它能增强与聚合物网络的动态互动结合，从而创造出创新的共晶凝胶。在这里，我们采用蒸发诱导限制策略，将聚乙烯醇（PVA）网络与我们的 DES 一起封装，从而开发出多功能共晶凝胶（PETGs）。实验验证和数值计算表明，聚酰胺与 PVA 形成了高密度的动态氢键，同时屏蔽了 PVA 链之间的氢键。这就形成了一个无法检测到结晶区域的多重氢键屏蔽无定形网络（MHSN），从而促进了离子迁移，确保了高导电性。此外，由于 MHSN 的存在，我们的 PETG 还具有快速自愈合、抗冻性、自粘性、抗菌性和双重敏感性。我们展示了 PETG 在运动传感、机器学习、人机交互和能量收集方面的应用潜力。
{"title":"Polyfunctional eutectogels with multiple hydrogen-bond-shielded amorphous networks for soft ionotronics","authors":"Yizhe Shao , Chao Dang , Haobo Qi , Ziyang Liu , Haoran Pei , Tongqing Lu , Wei Zhai","doi":"10.1016/j.matt.2024.09.009","DOIUrl":"10.1016/j.matt.2024.09.009","url":null,"abstract":"<div><div>Eutectogels, consisting of three-dimensional polymeric networks saturated with deep eutectic solvents (DESs), present a promising option for soft ionic conductors. Instead of modifying polymer chains, we propose a new DES system comprising phytic acid (PA) and choline chloride (ChCl), which enhances dynamic and interactive bonding with polymeric networks to create innovative eutectogels. Here, we develop polyfunctional eutectogels (PETGs) by encapsulating polyvinyl alcohol (PVA) networks with our DES using an evaporation-induced confinement strategy. Experimental validation and numerical calculations demonstrate that PA forms high-density dynamic hydrogen bonds with PVA while shielding hydrogen bonds between PVA chains. This results in a multiple hydrogen-bond-shielded amorphous network (MHSN) with undetectable crystalline regions, thereby promoting ion migration to ensure high conductivity. Moreover, our PETG exhibits rapid self-healing, freeze resistance, self-adhesion, antibacterial properties, and dual sensitivities attributable to the MHSN. We demonstrate the potential of PETGs for applications in motion sensing, machine learning, human-machine interaction, and energy harvesting.</div></div>","PeriodicalId":388,"journal":{"name":"Matter","volume":"7 11","pages":"Pages 4076-4098"},"PeriodicalIF":17.3,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142369529","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 : 2024-11-06DOI: 10.1016/j.matt.2024.06.050
Cong Chen , Zhenjia Chen , Di Liu , Xianghong Zhang , Changsong Gao , Liuting Shan , Lujian Liu , Tianjian Chen , Tailiang Guo , Huipeng Chen
Machine vision enables machines to extract rich information from image or video data and make intelligent decisions. However, approaches using artificial synapse hardware systems significantly limit the real-time and accuracy in machine vision segmentation amid complex environments. Addressing this, we propose a novel three-terminal adaptive artificial-light-emitting synapse (AALS) capable of photoelectric double output along with adaptive behavior. The device uses silver nanowires (AgNWs) as polar conductive bridges to reduce reliance on transparent electrodes, while polyvinyl alcohol (PVA) dielectric layers adaptively modulate charge carrier concentrations in conductive channels. Additionally, we have designed an adaptive parallel neural network (APNN) and applied it to autonomous driving image processing. This innovation significantly reduces adaptation time and notably enhances mean pixel accuracy (MPA) for semantic segmentation under overexposure and low-light conditions by 142.2% and 304.4%, respectively. Therefore, this work introduces new strategies for advanced adaptive vision, promising significant potential in intelligent driving and neuromorphic computing.
{"title":"Three-terminal quantum dot light-emitting synapse with active adaptive photoelectric outputs for complex image processing/parallel computing","authors":"Cong Chen , Zhenjia Chen , Di Liu , Xianghong Zhang , Changsong Gao , Liuting Shan , Lujian Liu , Tianjian Chen , Tailiang Guo , Huipeng Chen","doi":"10.1016/j.matt.2024.06.050","DOIUrl":"10.1016/j.matt.2024.06.050","url":null,"abstract":"<div><div>Machine vision enables machines to extract rich information from image or video data and make intelligent decisions. However, approaches using artificial synapse hardware systems significantly limit the real-time and accuracy in machine vision segmentation amid complex environments. Addressing this, we propose a novel three-terminal adaptive artificial-light-emitting synapse (AALS) capable of photoelectric double output along with adaptive behavior. The device uses silver nanowires (AgNWs) as polar conductive bridges to reduce reliance on transparent electrodes, while polyvinyl alcohol (PVA) dielectric layers adaptively modulate charge carrier concentrations in conductive channels. Additionally, we have designed an adaptive parallel neural network (APNN) and applied it to autonomous driving image processing. This innovation significantly reduces adaptation time and notably enhances mean pixel accuracy (MPA) for semantic segmentation under overexposure and low-light conditions by 142.2% and 304.4%, respectively. Therefore, this work introduces new strategies for advanced adaptive vision, promising significant potential in intelligent driving and neuromorphic computing.</div></div>","PeriodicalId":388,"journal":{"name":"Matter","volume":"7 11","pages":"Pages 3891-3906"},"PeriodicalIF":17.3,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141895932","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 : 2024-11-06DOI: 10.1016/j.matt.2024.07.018
Jingxian Li , Anirudh Appachar , Sabrina L. Peczonczyk , Elisa T. Harrison , Anton V. Ievlev , Ryan Hood , Dongjae Shin , Sangmin Yoo , Brianna Roest , Kai Sun , Karsten Beckmann , Olya Popova , Tony Chiang , William S. Wahby , Robin B. Jacobs-Godrim , Matthew J. Marinella , Petro Maksymovych , John T. Heron , Nathaniel Cady , Wei D. Lu , Yiyang Li
Electronic switches based on the migration of high-density point defects, or memristors, are poised to revolutionize post-digital electronics. Despite significant research, key mechanisms for filament formation and oxygen transport remain unresolved, hindering our ability to predict and design device properties. For example, experiments have achieved 10 orders of magnitude longer retention times than predicted by current models. Here, using electrical measurements, scanning probe microscopy, and first-principles calculations on tantalum oxide memristors, we reveal that the formation and stability of conductive filaments crucially depend on the thermodynamic stability of the amorphous oxygen-rich and oxygen-poor compounds, which undergo composition phase separation. Including the previously neglected effects of this amorphous phase separation reconciles unexplained discrepancies in retention and enables predictive design of key performance indicators such as retention stability. This result emphasizes non-ideal thermodynamic interactions as key design criteria in post-digital devices with defect densities substantially exceeding those of today’s covalent semiconductors.
{"title":"Thermodynamic origin of nonvolatility in resistive memory","authors":"Jingxian Li , Anirudh Appachar , Sabrina L. Peczonczyk , Elisa T. Harrison , Anton V. Ievlev , Ryan Hood , Dongjae Shin , Sangmin Yoo , Brianna Roest , Kai Sun , Karsten Beckmann , Olya Popova , Tony Chiang , William S. Wahby , Robin B. Jacobs-Godrim , Matthew J. Marinella , Petro Maksymovych , John T. Heron , Nathaniel Cady , Wei D. Lu , Yiyang Li","doi":"10.1016/j.matt.2024.07.018","DOIUrl":"10.1016/j.matt.2024.07.018","url":null,"abstract":"<div><div>Electronic switches based on the migration of high-density point defects, or memristors, are poised to revolutionize post-digital electronics. Despite significant research, key mechanisms for filament formation and oxygen transport remain unresolved, hindering our ability to predict and design device properties. For example, experiments have achieved 10 orders of magnitude longer retention times than predicted by current models. Here, using electrical measurements, scanning probe microscopy, and first-principles calculations on tantalum oxide memristors, we reveal that the formation and stability of conductive filaments crucially depend on the thermodynamic stability of the amorphous oxygen-rich and oxygen-poor compounds, which undergo composition phase separation. Including the previously neglected effects of this amorphous phase separation reconciles unexplained discrepancies in retention and enables predictive design of key performance indicators such as retention stability. This result emphasizes non-ideal thermodynamic interactions as key design criteria in post-digital devices with defect densities substantially exceeding those of today’s covalent semiconductors.</div></div>","PeriodicalId":388,"journal":{"name":"Matter","volume":"7 11","pages":"Pages 3970-3993"},"PeriodicalIF":17.3,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142085334","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 : 2024-11-06DOI: 10.1016/j.matt.2024.08.010
Alissa C. Johnson , Alice S. Fontaine , Emily A. Beeman , William J. Townsend , James H. Pikul
Human circulatory systems store large concentrations of oxygen and provide it continuously and simultaneously to trillions of cells without the need for each cell to access the surrounding environment. Inspired by biological circulatory systems, we envision future robotic systems with multifunctional, fully integrated, air-rechargeable energy delivery and storage. We present an aqueous air catholyte emulsion (ACE) with high oxygen solubility that can derive energy entirely from dissolved oxygen. With only 20% silicone oil by volume, ACEs can store twice as much dissolved oxygen (15 mg/L) as pure KOH samples, remain stable for several months, and show superior oxygen reduction reaction kinetics compared to KOH. Zinc-air flow cells with fully submerged electrodes can achieve 4.6 mW/cm2 at 5.6 mA/cm2. A multifunctional actuator flow cell configuration employs an ACE as both a hydraulic actuator and an energy storage fluid, demonstrating the feasibility of ACEs as multifunctional, flexible power sources for soft robotic systems.
{"title":"Emulsions that store oxygen for fast ORR kinetics and multifunctional robotic and mobility systems","authors":"Alissa C. Johnson , Alice S. Fontaine , Emily A. Beeman , William J. Townsend , James H. Pikul","doi":"10.1016/j.matt.2024.08.010","DOIUrl":"10.1016/j.matt.2024.08.010","url":null,"abstract":"<div><div>Human circulatory systems store large concentrations of oxygen and provide it continuously and simultaneously to trillions of cells without the need for each cell to access the surrounding environment. Inspired by biological circulatory systems, we envision future robotic systems with multifunctional, fully integrated, air-rechargeable energy delivery and storage. We present an aqueous air catholyte emulsion (ACE) with high oxygen solubility that can derive energy entirely from dissolved oxygen. With only 20% silicone oil by volume, ACEs can store twice as much dissolved oxygen (15 mg/L) as pure KOH samples, remain stable for several months, and show superior oxygen reduction reaction kinetics compared to KOH. Zinc-air flow cells with fully submerged electrodes can achieve 4.6 mW/cm<sup>2</sup> at 5.6 mA/cm<sup>2</sup>. A multifunctional actuator flow cell configuration employs an ACE as both a hydraulic actuator and an energy storage fluid, demonstrating the feasibility of ACEs as multifunctional, flexible power sources for soft robotic systems.</div></div>","PeriodicalId":388,"journal":{"name":"Matter","volume":"7 11","pages":"Pages 4059-4075"},"PeriodicalIF":17.3,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142161142","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}
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