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Substitution Index-Prediction Rules for Low-Potential Plateau of Hard Carbon Anodes in Sodium-Ion Batteries
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-25 DOI: 10.1002/adma.202417886
Yunfei Xue, Yaxin Chen, Yazhang Liang, Liluo Shi, Rui Ma, Xia Qiu, Ying Li, Nannan Guo, Quanchao Zhuang, Baojuan Xi, Zhicheng Ju, Shenglin Xiong
Establishing prediction rules for the low-potential plateau (LPP) of hard carbon (HC) anodes is crucial for constructing high-energy-density sodium-ion batteries (SIBs). While current studies suggest that the closed pores of HC can enhance the LPP performance, the rules for directly predicting the LPP from precursors have yet to be established. Here, prediction rules for the LPP of HC anodes in SIBs—the substitution index (Δ) of precursor are introduced. Three carbon models (disordered carbon, closed-pore-dominated carbon, and turbostratic carbon) are constructed to verify the accuracy of Δ and to explore the closed-pore formation and LPP mechanism. In detail, as the Δ increases from 0.06 to 0.22, the LPP capacity rises from 25 to 278 mAh g⁻¹, revealing a strong linear correlation between Δ of precursor and LPP capacity. In situ XRD, Raman, and ex situ SAXS, EPR further confirm that sodium storage in HC can be categorized into adsorption (>0.4 V), interlayer storage (0.4 to 0.15 V), and pore-filling (below 0.15 V). This work not only elucidates the sodium storage mechanisms, but also provides one efficient design guideline for advanced carbon anodes in SIBs.
{"title":"Substitution Index-Prediction Rules for Low-Potential Plateau of Hard Carbon Anodes in Sodium-Ion Batteries","authors":"Yunfei Xue, Yaxin Chen, Yazhang Liang, Liluo Shi, Rui Ma, Xia Qiu, Ying Li, Nannan Guo, Quanchao Zhuang, Baojuan Xi, Zhicheng Ju, Shenglin Xiong","doi":"10.1002/adma.202417886","DOIUrl":"https://doi.org/10.1002/adma.202417886","url":null,"abstract":"Establishing prediction rules for the low-potential plateau (LPP) of hard carbon (HC) anodes is crucial for constructing high-energy-density sodium-ion batteries (SIBs). While current studies suggest that the closed pores of HC can enhance the LPP performance, the rules for directly predicting the LPP from precursors have yet to be established. Here, prediction rules for the LPP of HC anodes in SIBs—the substitution index (<i>Δ</i>) of precursor are introduced. Three carbon models (disordered carbon, closed-pore-dominated carbon, and turbostratic carbon) are constructed to verify the accuracy of <i>Δ</i> and to explore the closed-pore formation and LPP mechanism. In detail, as the <i>Δ</i> increases from 0.06 to 0.22, the LPP capacity rises from 25 to 278 mAh g⁻¹, revealing a strong linear correlation between <i>Δ</i> of precursor and LPP capacity. In situ XRD, Raman, and ex situ SAXS, EPR further confirm that sodium storage in HC can be categorized into adsorption (&gt;0.4 V), interlayer storage (0.4 to 0.15 V), and pore-filling (below 0.15 V). This work not only elucidates the sodium storage mechanisms, but also provides one efficient design guideline for advanced carbon anodes in SIBs.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"71 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872578","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
Modulating Coupled Polyhedral Distortion in Li-Rich Cathodes for Synergistically Inhibiting Capacity and Voltage Decay
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-25 DOI: 10.1002/adma.202505616
Qinwen Cui, Songlin Yu, Yi Li, Xingyu Li, Xiaolin Zhao, Wujie Qiu, Jianjun Liu
Achieving significant enhancements in both capacity and voltage stability remains a formidable challenge for Li-rich layered cathodes. The severe performance degradation is attributed to large lattice strain, irreversible oxygen release and transition metal migration, but the most critical factor responsible for structural destabilization is still elusive. Here, based on density functional theory calculations, machine learning and experimental validation, a multi-hierarchy screening of complex multi-element doping systems is developed from electrochemical activity, lattice strain, oxygen stability and transition metal migration barrier. It is further identified that the coupled polyhedral distortion parameter D+σ2 of the substitution element is the most significant feature that affects the structural stability during cycling. The Li-rich layered cathode developed based on the predicted results exhibits remarkable long-term capacity stability (95.8% capacity retention over 300 cycles) and negligible voltage loss (0.02% voltage decay per cycle). This study provides a general approach by modulating coupled polyhedral distortion for the rational design of cathode materials and can be expanded to the discovery of other advanced electrodes.
{"title":"Modulating Coupled Polyhedral Distortion in Li-Rich Cathodes for Synergistically Inhibiting Capacity and Voltage Decay","authors":"Qinwen Cui, Songlin Yu, Yi Li, Xingyu Li, Xiaolin Zhao, Wujie Qiu, Jianjun Liu","doi":"10.1002/adma.202505616","DOIUrl":"https://doi.org/10.1002/adma.202505616","url":null,"abstract":"Achieving significant enhancements in both capacity and voltage stability remains a formidable challenge for Li-rich layered cathodes. The severe performance degradation is attributed to large lattice strain, irreversible oxygen release and transition metal migration, but the most critical factor responsible for structural destabilization is still elusive. Here, based on density functional theory calculations, machine learning and experimental validation, a multi-hierarchy screening of complex multi-element doping systems is developed from electrochemical activity, lattice strain, oxygen stability and transition metal migration barrier. It is further identified that the coupled polyhedral distortion parameter D+σ<sup>2</sup> of the substitution element is the most significant feature that affects the structural stability during cycling. The Li-rich layered cathode developed based on the predicted results exhibits remarkable long-term capacity stability (95.8% capacity retention over 300 cycles) and negligible voltage loss (0.02% voltage decay per cycle). This study provides a general approach by modulating coupled polyhedral distortion for the rational design of cathode materials and can be expanded to the discovery of other advanced electrodes.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"91 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872579","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
Enhancing Room-Temperature Spin Lifetimes in Molecular Semiconductors by Designing Intramolecular Dipole Orientations
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-25 DOI: 10.1002/adma.202500521
Yang Qin, Meng Wu, Junjun Xiang, Tingting Yang, Lidan Guo, Xianrong Gu, Rui Zhang, Xiangpeng Zhang, Ke Meng, Shunhua Hu, Ruiheng Zheng, Min Li, Yong Wang, Ye Zou, Jianqi Zhang, Xike Gao, Xiangnan Sun
In spintronics, achieving long spin lifetimes, particularly at room temperature (RT), is a key objective for spin transport materials. Molecular semiconductors (MSCs), with their inherently weak spin relaxation mechanisms, have emerged as promising candidates for realizing long RT spin lifetimes. However, effective strategies to suppress spin relaxation through the design of molecular structures in MSCs are still not well understood, and as a result, spin lifetimes remain limited (≈ 10-µs level at RT). In this study, the impact of intramolecular dipole orientations on spin lifetimes in MSCs has been explored for the first time. Both theoretical and experimental results have demonstrated that dipole orientation influences the hyperfine interaction (HFI) effect (a main causation for spin relaxation), and thus, spin lifetime. By adjusting dipole arrangements through molecular design, it is demonstrated that the poly(2,6-azuleneethynylene) with a regular dipole orientation served to reduce the HFI strength and ultimately extended the spin lifetime to 106 µs in a spintronic device, much higher than that of the random arrangement, setting a new RT record. This work provides new insights into the spin relaxation mechanism and offers a valuable strategy for extending spin lifetimes in MSCs for future RT spintronic applications.
{"title":"Enhancing Room-Temperature Spin Lifetimes in Molecular Semiconductors by Designing Intramolecular Dipole Orientations","authors":"Yang Qin, Meng Wu, Junjun Xiang, Tingting Yang, Lidan Guo, Xianrong Gu, Rui Zhang, Xiangpeng Zhang, Ke Meng, Shunhua Hu, Ruiheng Zheng, Min Li, Yong Wang, Ye Zou, Jianqi Zhang, Xike Gao, Xiangnan Sun","doi":"10.1002/adma.202500521","DOIUrl":"https://doi.org/10.1002/adma.202500521","url":null,"abstract":"In spintronics, achieving long spin lifetimes, particularly at room temperature (RT), is a key objective for spin transport materials. Molecular semiconductors (MSCs), with their inherently weak spin relaxation mechanisms, have emerged as promising candidates for realizing long RT spin lifetimes. However, effective strategies to suppress spin relaxation through the design of molecular structures in MSCs are still not well understood, and as a result, spin lifetimes remain limited (≈ 10-µs level at RT). In this study, the impact of intramolecular dipole orientations on spin lifetimes in MSCs has been explored for the first time. Both theoretical and experimental results have demonstrated that dipole orientation influences the hyperfine interaction (HFI) effect (a main causation for spin relaxation), and thus, spin lifetime. By adjusting dipole arrangements through molecular design, it is demonstrated that the poly(2,6-azuleneethynylene) with a regular dipole orientation served to reduce the HFI strength and ultimately extended the spin lifetime to 106 µs in a spintronic device, much higher than that of the random arrangement, setting a new RT record. This work provides new insights into the spin relaxation mechanism and offers a valuable strategy for extending spin lifetimes in MSCs for future RT spintronic applications.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"28 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872572","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
Shape Memory Networks With Tunable Self-Stiffening Kinetics Enabled by Polymer Melting-Recrystallization
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-25 DOI: 10.1002/adma.202500295
Xing Zhang, Yichen Zhou, Haoran Chen, Ying Zheng, Junfeng Liu, Yongzhong Bao, Guorong Shan, Chengtao Yu, Pengju Pan
Shape memory polymers (SMPs) are deformable materials capable of recovering from a programmed temporary shape to a permanent shape under specific stimuli. However, shape recovery of SMPs is often accompanied by the evolution of materials from a stiff to soft state, leading to a significant decrease in strength/modulus and thereby impacting their practical applications. Although some attempts are made to pursue the SMPs with self-stiffening capability after shape recovery, the modulus increase ratio is much limited. Inspired by the recrystallization process of CaCO3 during crab molting, a novel and universal strategy is developed to construct water-free self-stiffening SMPs by using a single thermal stimulus through harnessing the polymer melting-recrystallization. The shape recovery is achieved through the melting of polymer primary crystals, followed by the self-stiffening via polymer recrystallization at the same recovery temperature, in which the modulus increase rate and ratio can be programmed in a wide range. Additionally, conceptual applications of these self-stiffening SMPs as artificial stents with self-enhancing supporting function are successfully demonstrated. This work is believed to provide new insights for developing the advanced shape memory devices.
{"title":"Shape Memory Networks With Tunable Self-Stiffening Kinetics Enabled by Polymer Melting-Recrystallization","authors":"Xing Zhang, Yichen Zhou, Haoran Chen, Ying Zheng, Junfeng Liu, Yongzhong Bao, Guorong Shan, Chengtao Yu, Pengju Pan","doi":"10.1002/adma.202500295","DOIUrl":"https://doi.org/10.1002/adma.202500295","url":null,"abstract":"Shape memory polymers (SMPs) are deformable materials capable of recovering from a programmed temporary shape to a permanent shape under specific stimuli. However, shape recovery of SMPs is often accompanied by the evolution of materials from a stiff to soft state, leading to a significant decrease in strength/modulus and thereby impacting their practical applications. Although some attempts are made to pursue the SMPs with self-stiffening capability after shape recovery, the modulus increase ratio is much limited. Inspired by the recrystallization process of CaCO<sub>3</sub> during crab molting, a novel and universal strategy is developed to construct water-free self-stiffening SMPs by using a single thermal stimulus through harnessing the polymer melting-recrystallization. The shape recovery is achieved through the melting of polymer primary crystals, followed by the self-stiffening via polymer recrystallization at the same recovery temperature, in which the modulus increase rate and ratio can be programmed in a wide range. Additionally, conceptual applications of these self-stiffening SMPs as artificial stents with self-enhancing supporting function are successfully demonstrated. This work is believed to provide new insights for developing the advanced shape memory devices.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"8 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872576","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
Synergistic Interface Engineering via o-Difluorobenzene-Mediated HPWO Crystallization and ITO Fluorination for 20.57% Efficiency Organic Solar Cells
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-25 DOI: 10.1002/adma.202503072
Xingjian Dai, Ben Fan, Xiaopeng Xu, Qiang Peng
Interfacial energy loss is a critical challenge in achieving high-efficiency organic solar cells (OSCs), primarily due to mismatched energy levels and inefficient charge collection. Herein, a bifunctional interface engineering strategy is proposed, employing an ethanol/o-difluorobenzene (EtOH/o-DFB) dual-solvent system for phosphotungstic acid (HPWO) processing. During film formation, o-DFB regulates HPWO crystallization by suppressing excessive aggregation, while enabling in situ ITO fluorination through the adsorbed o-DFB. This synergistic approach simultaneously mitigates the trap-assisted nonradiative recombination at the hole transport layer while enhancing the electrode work function, resulting in better ohmic contact, minimized trap-state densities, and improved energy level alignment at the electrode/active layer interface. The effectiveness of this strategy is demonstrated across multiple active layer systems. Remarkable power conversion efficiencies of 19.55%, 20.07%, and 20.57% are achieved for PM6/L8-BO, D18/L8-BO, and D18/BTP-eC9-based OSCs, respectively. Notably, the 20.57% PCE represents one of the highest efficiencies reported to date for OSCs, highlighting the potential of this bifunctional interface engineering strategy in advancing high-performance organic photovoltaics.
{"title":"Synergistic Interface Engineering via o-Difluorobenzene-Mediated HPWO Crystallization and ITO Fluorination for 20.57% Efficiency Organic Solar Cells","authors":"Xingjian Dai, Ben Fan, Xiaopeng Xu, Qiang Peng","doi":"10.1002/adma.202503072","DOIUrl":"https://doi.org/10.1002/adma.202503072","url":null,"abstract":"Interfacial energy loss is a critical challenge in achieving high-efficiency organic solar cells (OSCs), primarily due to mismatched energy levels and inefficient charge collection. Herein, a bifunctional interface engineering strategy is proposed, employing an ethanol/o-difluorobenzene (EtOH/o-DFB) dual-solvent system for phosphotungstic acid (HPWO) processing. During film formation, o-DFB regulates HPWO crystallization by suppressing excessive aggregation, while enabling in situ ITO fluorination through the adsorbed o-DFB. This synergistic approach simultaneously mitigates the trap-assisted nonradiative recombination at the hole transport layer while enhancing the electrode work function, resulting in better ohmic contact, minimized trap-state densities, and improved energy level alignment at the electrode/active layer interface. The effectiveness of this strategy is demonstrated across multiple active layer systems. Remarkable power conversion efficiencies of 19.55%, 20.07%, and 20.57% are achieved for PM6/L8-BO, D18/L8-BO, and D18/BTP-eC9-based OSCs, respectively. Notably, the 20.57% PCE represents one of the highest efficiencies reported to date for OSCs, highlighting the potential of this bifunctional interface engineering strategy in advancing high-performance organic photovoltaics.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"79 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872569","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
Processable and Recyclable Covalent Organic Framework Gel Electrolytes
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-25 DOI: 10.1002/adma.202501223
Zhiwen Fan, Juntao Tang, Wei Zhang, Jiayin Yuan, Shuai Gu, Rongyi Huang, Qianpan Guo, Qiujian Xie, Fan Hu, Feng Zhang, Zihao Wang, Chunyue Pan, Guipeng Yu
Covalent organic framework (COF)-based electrolytes with abundant ordered channels and accessible interaction sites have shown great potential in energy storage and transformation, although their practical applications are strongly impeded by their inherent insolubility and non-melt processability. Developing processable COF gel electrolytes and recycling them remains a formidable challenge. In this study, the processing of COF to gels demonstrated through interlayer interaction manipulation and enable solution-reconstruction of COF gel electrolytes for the first time, inspired by the working principle of wedges. Good solution-processability of the COF powders in strong acid mediums is achieved by inserting oxygen atoms into its framework to promote the interlayer charge repulsion. This modification enabled the COF readily dispersable as colloidal nanosheets in an aqueous solution of trifluoroacetic acid (TFA). Starting from here, this is modulated competitive interactions among TFA, COF, and water molecules, to reconfigure COF materials between their gelified and colloidally dispersed states. The reconfigured COF gel maintains their mechanical properties and long cycle life as an electrolyte in the battery (>800 h). This approach realizes solution processing of COF powders and can recycle COF out of gels for repeated use, offering new insights and strategies for their preparation and sustainable recycling.
{"title":"Processable and Recyclable Covalent Organic Framework Gel Electrolytes","authors":"Zhiwen Fan, Juntao Tang, Wei Zhang, Jiayin Yuan, Shuai Gu, Rongyi Huang, Qianpan Guo, Qiujian Xie, Fan Hu, Feng Zhang, Zihao Wang, Chunyue Pan, Guipeng Yu","doi":"10.1002/adma.202501223","DOIUrl":"https://doi.org/10.1002/adma.202501223","url":null,"abstract":"Covalent organic framework (COF)-based electrolytes with abundant ordered channels and accessible interaction sites have shown great potential in energy storage and transformation, although their practical applications are strongly impeded by their inherent insolubility and non-melt processability. Developing processable COF gel electrolytes and recycling them remains a formidable challenge. In this study, the processing of COF to gels demonstrated through interlayer interaction manipulation and enable solution-reconstruction of COF gel electrolytes for the first time, inspired by the working principle of wedges. Good solution-processability of the COF powders in strong acid mediums is achieved by inserting oxygen atoms into its framework to promote the interlayer charge repulsion. This modification enabled the COF readily dispersable as colloidal nanosheets in an aqueous solution of trifluoroacetic acid (TFA). Starting from here, this is modulated competitive interactions among TFA, COF, and water molecules, to reconfigure COF materials between their gelified and colloidally dispersed states. The reconfigured COF gel maintains their mechanical properties and long cycle life as an electrolyte in the battery (&gt;800 h). This approach realizes solution processing of COF powders and can recycle COF out of gels for repeated use, offering new insights and strategies for their preparation and sustainable recycling.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"171 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872571","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
Tunable Bipolar Photothermoelectric Response from Mott Activation for In-Sensor Image Preprocessing
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-25 DOI: 10.1002/adma.202502915
Bowen Li, Ning Lin, Zhaowu Wang, Baojie Chen, Changyong Lan, Xiaocui Li, You Meng, Weijun Wang, Mingqi Ding, Pengshan Xie, Yuxuan Zhang, Zenghui Wu, Dengji Li, Fu-Rong Chen, Chi Hou Chan, Zhongrui Wang, Johnny C. Ho
In-sensor image preprocessing, a subset of edge computing, offers a solution to mitigate frequent analog-digital conversions and the von Neumann bottleneck in conventional digital hardware. However, an efficient in-sensor device array with large-scale integration capability for high-density and low-power sensory processing is still lacking and highly desirable. This work introduces an adjustable broadband photothermoelectric detector based on a phase-change vanadium dioxide thin-film transistor. This transistor employs a vanadium dioxide/gallium nitride three-terminal structure with a gate-tunable phase transition at the gate-source junctions. This design allows for modulable photothermoelectric responsivities and alteration of the short-circuit photocurrent's polarities. The devices exhibit linear gate dependence for the broadband photoresponse and linear light-intensity dependence for both positive and negative photoresponsivities. The device's energy consumption is as low as 8 pJ per spike, which is one order of magnitude lower than that of previous Mott materials-based in-sensor preprocessing devices. A wafer-scale bipolar phototransistor array has also been fabricated by standard micro-/nano-fabrication techniques, exhibiting excellent stability and endurance (over 5000 cycles). More importantly, an integrated in-sensor convolutional network is successfully designed for simultaneous broadband image classification, medical image denoising, and retinal vessel segmentation, delivering exceptional performance and paving the way for future smart edge sensors.
{"title":"Tunable Bipolar Photothermoelectric Response from Mott Activation for In-Sensor Image Preprocessing","authors":"Bowen Li, Ning Lin, Zhaowu Wang, Baojie Chen, Changyong Lan, Xiaocui Li, You Meng, Weijun Wang, Mingqi Ding, Pengshan Xie, Yuxuan Zhang, Zenghui Wu, Dengji Li, Fu-Rong Chen, Chi Hou Chan, Zhongrui Wang, Johnny C. Ho","doi":"10.1002/adma.202502915","DOIUrl":"https://doi.org/10.1002/adma.202502915","url":null,"abstract":"In-sensor image preprocessing, a subset of edge computing, offers a solution to mitigate frequent analog-digital conversions and the von Neumann bottleneck in conventional digital hardware. However, an efficient in-sensor device array with large-scale integration capability for high-density and low-power sensory processing is still lacking and highly desirable. This work introduces an adjustable broadband photothermoelectric detector based on a phase-change vanadium dioxide thin-film transistor. This transistor employs a vanadium dioxide/gallium nitride three-terminal structure with a gate-tunable phase transition at the gate-source junctions. This design allows for modulable photothermoelectric responsivities and alteration of the short-circuit photocurrent's polarities. The devices exhibit linear gate dependence for the broadband photoresponse and linear light-intensity dependence for both positive and negative photoresponsivities. The device's energy consumption is as low as 8 pJ per spike, which is one order of magnitude lower than that of previous Mott materials-based in-sensor preprocessing devices. A wafer-scale bipolar phototransistor array has also been fabricated by standard micro-/nano-fabrication techniques, exhibiting excellent stability and endurance (over 5000 cycles). More importantly, an integrated in-sensor convolutional network is successfully designed for simultaneous broadband image classification, medical image denoising, and retinal vessel segmentation, delivering exceptional performance and paving the way for future smart edge sensors.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"8 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872549","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
Super-Wide Color Tunability from a Single Electrochromic Device through In Situ Reconstruction of Optical Cavity
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-25 DOI: 10.1002/adma.202417511
Xueqing Tang, Zishou Hu, Zhenyong Wang, Xinzhou Wu, Zhen Wang, Wenming Su, Shan Cong, Fengxia Geng, Zhigang Zhao
Electrochromic (EC) displays, as non-emissive (passive) displays with low energy consumption, have garnered significant attention from both industry and academia in recent years. Nevertheless, traditional EC technology faces challenges in achieving full-color displays within a single device due to its limited color gamut, even though full-color capability is highly desirable for eliminating the need for complex RGB subpixel mosaics. Herein, a new strategy is proposed utilizing in situ, electrically driven reconstruction of optical cavities on an electrochromic electrode surface to fabricate EC devices with super-wide color tunability. The device fabricated by this approach can create a wide variety of colors from yellow, orange, red, violet, blue, and cyan to green in a single EC device that almost spans the entire visible region (Δhue approaches 360°). Apart from the super-wide color tunability, the devices also have small working voltage window (0.2-1.8 V), outstanding bistability (>8 h), extremely low power consumption (≈2.3 mW cm−2) and good cycling ability (≈4.3% decay rate after 1,000 cycles). Moreover, the super-wide color tunability of these EC devices has been demonstrated in diverse applications, including shifting rainbow flower images, color palettes, and information displays.
{"title":"Super-Wide Color Tunability from a Single Electrochromic Device through In Situ Reconstruction of Optical Cavity","authors":"Xueqing Tang, Zishou Hu, Zhenyong Wang, Xinzhou Wu, Zhen Wang, Wenming Su, Shan Cong, Fengxia Geng, Zhigang Zhao","doi":"10.1002/adma.202417511","DOIUrl":"https://doi.org/10.1002/adma.202417511","url":null,"abstract":"Electrochromic (EC) displays, as non-emissive (passive) displays with low energy consumption, have garnered significant attention from both industry and academia in recent years. Nevertheless, traditional EC technology faces challenges in achieving full-color displays within a single device due to its limited color gamut, even though full-color capability is highly desirable for eliminating the need for complex RGB subpixel mosaics. Herein, a new strategy is proposed utilizing in situ, electrically driven reconstruction of optical cavities on an electrochromic electrode surface to fabricate EC devices with super-wide color tunability. The device fabricated by this approach can create a wide variety of colors from yellow, orange, red, violet, blue, and cyan to green in a single EC device that almost spans the entire visible region (Δhue approaches 360°). Apart from the super-wide color tunability, the devices also have small working voltage window (0.2-1.8 V), outstanding bistability (&gt;8 h), extremely low power consumption (≈2.3 mW cm<sup>−2</sup>) and good cycling ability (≈4.3% decay rate after 1,000 cycles). Moreover, the super-wide color tunability of these EC devices has been demonstrated in diverse applications, including shifting rainbow flower images, color palettes, and information displays.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"56 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143872582","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
Ultrahigh Conductive MXene Films for Broadband Electromagnetic Interference Shielding
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-25 DOI: 10.1002/adma.202502443
Ju-Hyoung Han, Jaeeun Park, Mincheal Kim, Sungwoo Lee, Jin Myeong Heo, Young Ho Jin, Yujin Chae, Juwon Han, Jaewon Wang, Shi-Hyun Seok, Yeoseon Sim, Gangil Byun, Gun-Do Lee, EunMi Choi, Soon-Yong Kwon
Broadband and ultrathin electromagnetic interference (EMI)-shielding materials are crucial for efficient high-frequency data transmission in emerging technologies. MXenes are renowned for their outstanding electrical conductivity and EMI-shielding capability. While substituting nitrogen (N) for carbon (C) atoms in the conventional MXene structure is theoretically expected to enhance these properties, synthesis challenges have hindered progress. Here, it is demonstrated that TixCyNx-y-1Tz MXene films with optimized N content achieve a record-high electrical conductivity of 35 000 S cm−1 and exceptional broadband EMI shielding across the X (8–12.4 GHz), Ka (26.5–40 GHz), and W (75–110 GHz) bands—outperforming all previously reported materials even at reduced thicknesses. By synthesizing a full series of high-stoichiometric TixAlCyNx-y-1 MAX phases without intermediate phases, the impact of N substitution on the physical and electrical properties of TixCyNx-y-1Tz MXene flakes is systematically explored, achieving complete composition tunability in both dispersion and film forms. These findings position TixCyNx-y-1Tz MXenes as promising candidates for applications spanning from conventional lower-frequency domains to next-generation sub-THz electronics.
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引用次数: 0
Toward Switching and Fusing Neuromorphic Computing: Vertical Bulk Heterojunction Transistors with Multi-Neuromorphic Functions for Efficient Deep Learning
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-04-24 DOI: 10.1002/adma.202419245
Yi Zou, Di Liu, Xinyan Gan, Rengjian Yu, Xianghong Zhang, Chansong Gao, Zhenjia Chen, Chenhui Xu, Yun Ye, Yuanyuan Hu, Tailiang Guo, Huipeng Chen
The combination of artificial neural networks (ANN) and spiking neural networks (SNN) holds great promise for advancing artificial general intelligence (AGI). However, the reported ANN and SNN computational architectures are independent and require a large number of auxiliary circuits and external algorithms for fusion training. Here, a novel vertical bulk heterojunction neuromorphic transistor (VHNT) capable of emulating both ANN and SNN computational functions is presented. TaOx-based electrochemical reactions and PDVT-10/N2200-based bulk heterojunctions are used to realize spike coding and voltage coding, respectively. Notably, the device exhibits remarkable efficiency, consuming a mere 0.84 nJ of energy consumption for a single multiply accumulate (MAC) operation with excellent linearity. Moreover, the device can be switched to spiking neuron and self-activation neuron by simply changing the programming without auxiliary circuits. Finally, the VHNT-based artificial spiking neural network (ASNN) fusion simulation architecture is demonstrated, achieving 95% accuracy for Canadian-Institute-For-Advanced-ResearchResearch-10 (CIFARResearch-10) dataset while significantly enhancing training speed and efficiency. This work proposes a novel device strategy for developing high-performance, low-power, and environmentally adaptive AGI.
{"title":"Toward Switching and Fusing Neuromorphic Computing: Vertical Bulk Heterojunction Transistors with Multi-Neuromorphic Functions for Efficient Deep Learning","authors":"Yi Zou, Di Liu, Xinyan Gan, Rengjian Yu, Xianghong Zhang, Chansong Gao, Zhenjia Chen, Chenhui Xu, Yun Ye, Yuanyuan Hu, Tailiang Guo, Huipeng Chen","doi":"10.1002/adma.202419245","DOIUrl":"https://doi.org/10.1002/adma.202419245","url":null,"abstract":"The combination of artificial neural networks (ANN) and spiking neural networks (SNN) holds great promise for advancing artificial general intelligence (AGI). However, the reported ANN and SNN computational architectures are independent and require a large number of auxiliary circuits and external algorithms for fusion training. Here, a novel vertical bulk heterojunction neuromorphic transistor (VHNT) capable of emulating both ANN and SNN computational functions is presented. TaO<sub>x</sub>-based electrochemical reactions and PDVT-10/N2200-based bulk heterojunctions are used to realize spike coding and voltage coding, respectively. Notably, the device exhibits remarkable efficiency, consuming a mere 0.84 nJ of energy consumption for a single multiply accumulate (MAC) operation with excellent linearity. Moreover, the device can be switched to spiking neuron and self-activation neuron by simply changing the programming without auxiliary circuits. Finally, the VHNT-based artificial spiking neural network (ASNN) fusion simulation architecture is demonstrated, achieving 95% accuracy for Canadian-Institute-For-Advanced-ResearchResearch-10 (CIFARResearch-10) dataset while significantly enhancing training speed and efficiency. This work proposes a novel device strategy for developing high-performance, low-power, and environmentally adaptive AGI.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"23 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143867152","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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Advanced Materials
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