Taegyun Park, Jihun Kim, Young Jae Kwon, Han Joon Kim, Seong Pil Yim, Dong Hoon Shin, Yeong Rok Kim, Hae Jin Kim, Cheol Seong Hwang
The self‐rectifying memristor with a bilayer of trap‐rich HfO2 and insulating Ta2O5 oxide layers is considered one of the most promising candidates for the memristive crossbar array due to its superior switching performance, scalability with 3D stacking, and low operating power. However, the output current variation due to the electron detrapping from trap states can cause the failure of critical operations in neuromorphic applications. This work suggests two solutions to mitigate the switching variations and insufficient data retention time by embedding gold nanodots and modifying the bias voltage application methods for read, write, and erase operations in the crossbar array. The switching mechanism is studied by varying the embedded position of the gold nanodots across the thickness direction of the bilayered oxides, which helped to optimize device performance further. Combining the two solutions into the proposed self‐rectifying memristor enables a single device to have the 7‐possible, stable states by preventing interstate overlap and securing the retention. Consequently, the hardware neural network consisting of self‐rectifying memristors with gold nanodots with the modified bias voltage application methods demonstrates a high inference accuracy of 93.1% in MNIST handwritten digit classification, comparable to the software‐based accuracy of 93.4%, benefiting from the enhanced multi‐state uniformity.
{"title":"Au‐Nanodots Embedded Self‐Rectifying Analog Charge Trap Memristor with Modified Bias Voltage Application Method for Stable Multi‐Bit Hardware‐Based Neural Network","authors":"Taegyun Park, Jihun Kim, Young Jae Kwon, Han Joon Kim, Seong Pil Yim, Dong Hoon Shin, Yeong Rok Kim, Hae Jin Kim, Cheol Seong Hwang","doi":"10.1002/admt.202400965","DOIUrl":"https://doi.org/10.1002/admt.202400965","url":null,"abstract":"The self‐rectifying memristor with a bilayer of trap‐rich HfO<jats:sub>2</jats:sub> and insulating Ta<jats:sub>2</jats:sub>O<jats:sub>5</jats:sub> oxide layers is considered one of the most promising candidates for the memristive crossbar array due to its superior switching performance, scalability with 3D stacking, and low operating power. However, the output current variation due to the electron detrapping from trap states can cause the failure of critical operations in neuromorphic applications. This work suggests two solutions to mitigate the switching variations and insufficient data retention time by embedding gold nanodots and modifying the bias voltage application methods for read, write, and erase operations in the crossbar array. The switching mechanism is studied by varying the embedded position of the gold nanodots across the thickness direction of the bilayered oxides, which helped to optimize device performance further. Combining the two solutions into the proposed self‐rectifying memristor enables a single device to have the 7‐possible, stable states by preventing interstate overlap and securing the retention. Consequently, the hardware neural network consisting of self‐rectifying memristors with gold nanodots with the modified bias voltage application methods demonstrates a high inference accuracy of 93.1% in MNIST handwritten digit classification, comparable to the software‐based accuracy of 93.4%, benefiting from the enhanced multi‐state uniformity.","PeriodicalId":7200,"journal":{"name":"Advanced Materials & Technologies","volume":"42 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142252317","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The surface of hard carbon is rich in micropores, disordered graphene layers, defects, and various functional groups that can serve as reactive sites. However, these reaction sites are non‐equivalent sites both electronically and geometrically. Consequently, the solid electrolyte interface (SEI) formed on the hard carbon electrode exhibits instability in the organic electrolyte system, resulting in a continuous depletion of LiPF6 within the electrolyte, thereby compromising its cycling stability. Herein, the formation of stable SEI is induced by modulating the surface structure of hard carbon fibers. The transition metal nickel is utilized to convert the disordered structure on the surface of hard carbon fibers into graphitic crystallites at high temperatures. This also reduces the functional groups, micropores, defects, and disordered graphene layers on the surface of the hard carbon fibers, making the active sites equiv. Meanwhile, the highly active graphene edges are uniformly exposed as nucleation sites on the fibers surface, which induces the formation of a uniform and dense SEI and inhibits the continuous decomposition of LiPF6, thus improving the rate performance and cycling stability of the hard carbon.
{"title":"Enhanced Electrochemical Performances of Hard Carbon via Nickel‐Metal Catalyzed Surface Conversion Graphitic Crystallites","authors":"Junsheng Yuan, Muxuan Li, Mengjing Jin, Yanting Wang, Guowen Sun, Jianqiao Song, Jinyuan Zhou, Xia Ni, Xiaojun Pan","doi":"10.1002/admt.202400907","DOIUrl":"https://doi.org/10.1002/admt.202400907","url":null,"abstract":"The surface of hard carbon is rich in micropores, disordered graphene layers, defects, and various functional groups that can serve as reactive sites. However, these reaction sites are non‐equivalent sites both electronically and geometrically. Consequently, the solid electrolyte interface (SEI) formed on the hard carbon electrode exhibits instability in the organic electrolyte system, resulting in a continuous depletion of LiPF<jats:sub>6</jats:sub> within the electrolyte, thereby compromising its cycling stability. Herein, the formation of stable SEI is induced by modulating the surface structure of hard carbon fibers. The transition metal nickel is utilized to convert the disordered structure on the surface of hard carbon fibers into graphitic crystallites at high temperatures. This also reduces the functional groups, micropores, defects, and disordered graphene layers on the surface of the hard carbon fibers, making the active sites equiv. Meanwhile, the highly active graphene edges are uniformly exposed as nucleation sites on the fibers surface, which induces the formation of a uniform and dense SEI and inhibits the continuous decomposition of LiPF<jats:sub>6</jats:sub>, thus improving the rate performance and cycling stability of the hard carbon.","PeriodicalId":7200,"journal":{"name":"Advanced Materials & Technologies","volume":"40 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142252322","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In this study, a tri‐layer Pt/Al/TiOx/HfOx/Al2O3/Pt memristor device is fabricated and analyze its electrical characteristics for reservoir computing and neuromorphic systems applications. This device incorporates an oxygen reservoir of a TiOx and a barrier layer of an Al2O3, enabling stable bipolar switching characteristics without the need for an electroforming process over 103 cycles. It also exhibits self‐rectifying properties under a negative bias. Based on these characteristics, it is investigated essential synaptic functions such as long‐term potentiation (LTP), long‐term depression (LTD), paired‐pulse facilitation (PPF), spike‐rate‐dependent plasticity (SRDP), spike‐duration‐dependent plasticity (SDDP), spike‐number‐dependent plasticity (SNDP), and spike‐amplitude‐dependent plasticity (SADP), to assess their suitability for neuromorphic applications that mimic biological synapses. Furthermore, utilizing the short‐term memory characteristics of the device, reservoir computing (RC) measurement from [0000] to [1111] in 4‐bit representation is conducted. This capability enables us to achieve a high accuracy of 95.5% in MNIST pattern recognition tasks. Lastly, the natural decay characteristics caused by oxygen ion migration in the device, examining the transition from short‐term to long‐term memory in image memorization tasks is explored. The potential for deployment in high‐density crossbar arrays by calculating the read margin based on the device I–V curve and programming scheme is also evaluated.
{"title":"Self‐Rectifying Short‐Term Memory Phenomena Through Integration of TiOx Oxygen Reservoir and Al2O3 Barrier Layers for Neuromorphic System","authors":"Hyeonseung Ji, Sungjoon Kim, Sungjun Kim","doi":"10.1002/admt.202400895","DOIUrl":"https://doi.org/10.1002/admt.202400895","url":null,"abstract":"In this study, a tri‐layer Pt/Al/TiO<jats:sub>x</jats:sub>/HfO<jats:sub>x</jats:sub>/Al<jats:sub>2</jats:sub>O<jats:sub>3</jats:sub>/Pt memristor device is fabricated and analyze its electrical characteristics for reservoir computing and neuromorphic systems applications. This device incorporates an oxygen reservoir of a TiO<jats:sub>x</jats:sub> and a barrier layer of an Al<jats:sub>2</jats:sub>O<jats:sub>3</jats:sub>, enabling stable bipolar switching characteristics without the need for an electroforming process over 10<jats:sup>3</jats:sup> cycles. It also exhibits self‐rectifying properties under a negative bias. Based on these characteristics, it is investigated essential synaptic functions such as long‐term potentiation (LTP), long‐term depression (LTD), paired‐pulse facilitation (PPF), spike‐rate‐dependent plasticity (SRDP), spike‐duration‐dependent plasticity (SDDP), spike‐number‐dependent plasticity (SNDP), and spike‐amplitude‐dependent plasticity (SADP), to assess their suitability for neuromorphic applications that mimic biological synapses. Furthermore, utilizing the short‐term memory characteristics of the device, reservoir computing (RC) measurement from [0000] to [1111] in 4‐bit representation is conducted. This capability enables us to achieve a high accuracy of 95.5% in MNIST pattern recognition tasks. Lastly, the natural decay characteristics caused by oxygen ion migration in the device, examining the transition from short‐term to long‐term memory in image memorization tasks is explored. The potential for deployment in high‐density crossbar arrays by calculating the read margin based on the device <jats:italic>I–V</jats:italic> curve and programming scheme is also evaluated.","PeriodicalId":7200,"journal":{"name":"Advanced Materials & Technologies","volume":"100 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142252318","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sanghyun Park, Chi Keung Song, Mincheol Jung, Seong Min Jeon, Changhee Chae, Woo‐Jin Song, Kyung Jin Lee
For the next generation of lithium batteries, polymer‐based electrolytes are promising candidates for resolving issues from liquid electrolytes such as leakage, flammability, and explosion. Various attempts have been carried out to develop polymer electrolytes based on poly(ethylene oxide) (PEO), polyacrylonitrile, polyvinylidene fluoride, etc., resulting in suppression for dendrite growth on Li metal and mechanical support against internal or external shock as well. Among these polymer electrolytes, PEO has been widely used due to their relatively high ionic conduction through the hopping of Li ions. Herein, poly(GAP‐co‐THF) diol (PGT) having a similar main chain to PEO while containing azide groups in a side chain is synthesized. To enhance the processability of polymer electrolytes, the thermal crosslinking process is performed via azide‐alkene cycloaddition between PGT and poly(ethylene glycol) diacrylate with lithium bis(trifluoromethanesulfonyl)imide without any initiators and organic solvents. Thickness controllable thin film of polymer electrolyte is obtained after the crosslinking process, resulting in outstanding advantages with respect to stacking of batteries. To check the electrochemical stabilities and cell performances of these polymer electrolytes, cyclic voltammetry, linear symmetric voltammetry, LiFePO4∥Li cell, and Li symmetric cell tests are accomplished.
对于下一代锂电池，聚合物电解质是解决液态电解质泄漏、易燃和爆炸等问题的有前途的候选材料。人们已经进行了各种尝试，开发基于聚环氧乙烷（PEO）、聚丙烯腈、聚偏氟乙烯等的聚合物电解质，从而抑制锂金属上的枝晶生长，并提供机械支持以抵御内部或外部冲击。在这些聚合物电解质中，聚醚砜因其通过锂离子跳跃产生的相对较高的离子传导性而被广泛使用。在此，我们合成了主链与 PEO 相似，但侧链中含有叠氮基团的聚（GAP-co-THF）二元醇（PGT）。为了提高聚合物电解质的加工性能，在不使用任何引发剂和有机溶剂的情况下，通过叠氮-烯环加成法在 PGT 和聚乙二醇二丙烯酸酯与双(三氟甲磺酰基)亚胺锂之间进行热交联。交联后可获得厚度可控的聚合物电解质薄膜，从而在电池堆叠方面具有突出优势。为了检验这些聚合物电解质的电化学稳定性和电池性能，我们完成了循环伏安法、线性对称伏安法、LiFePO4∥Li 电池和 Li 对称电池测试。
{"title":"Initiator‐Free Crosslinking Process Without Organic Solvent for Polymer Gel Electrolyte of Lithium Metal Batteries","authors":"Sanghyun Park, Chi Keung Song, Mincheol Jung, Seong Min Jeon, Changhee Chae, Woo‐Jin Song, Kyung Jin Lee","doi":"10.1002/admt.202400851","DOIUrl":"https://doi.org/10.1002/admt.202400851","url":null,"abstract":"For the next generation of lithium batteries, polymer‐based electrolytes are promising candidates for resolving issues from liquid electrolytes such as leakage, flammability, and explosion. Various attempts have been carried out to develop polymer electrolytes based on poly(ethylene oxide) (PEO), polyacrylonitrile, polyvinylidene fluoride, etc., resulting in suppression for dendrite growth on Li metal and mechanical support against internal or external shock as well. Among these polymer electrolytes, PEO has been widely used due to their relatively high ionic conduction through the hopping of Li ions. Herein, poly(GAP‐co‐THF) diol (PGT) having a similar main chain to PEO while containing azide groups in a side chain is synthesized. To enhance the processability of polymer electrolytes, the thermal crosslinking process is performed via azide‐alkene cycloaddition between PGT and poly(ethylene glycol) diacrylate with lithium bis(trifluoromethanesulfonyl)imide without any initiators and organic solvents. Thickness controllable thin film of polymer electrolyte is obtained after the crosslinking process, resulting in outstanding advantages with respect to stacking of batteries. To check the electrochemical stabilities and cell performances of these polymer electrolytes, cyclic voltammetry, linear symmetric voltammetry, LiFePO<jats:sub>4</jats:sub>∥Li cell, and Li symmetric cell tests are accomplished.","PeriodicalId":7200,"journal":{"name":"Advanced Materials & Technologies","volume":"5 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142252320","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ruiyuan Sun, Qinglu Liu, Qitao Liu, Weilong Qin, Jiabo Le, Xiaopei Ren, Muhammad Bilal Akbar, Yang Zhou, Chonghan Xia, Licheng Sun, Yongbo Kuang
Particle transfer method photoelectrodes show superior photoelectrochemical performance compared to traditional powder‐based methods, making them a promising solution for solar water splitting in sustainable energy. This study introduces an innovative nonvacuum particle transfer method for fabricating photoelectrodes on a conductive carbon substrate, addressing the challenges associated with the high costs and vacuum deposition processes of traditional methods. Utilizing a p‐type CuFeO2 powder semiconductor, a unique substrate is developed by applying a graphene oxide layer mixed with a small amount of silica binder on the particle layer's backside through ultrasonic atomization spraying. This layer is converted into multilayered reduced graphene oxide (ML‐rGO) via wet chemical reduction, resulting in a substrate boasting a high work function (4.8 eV), alongside remarkable chemical stability, mechanical strength, and conductivity. The fabricated CuFeO2 photocathode demonstrated an onset potential of 0.97 V versus RHE and a photocurrent density of 1.5 mA cm−2 at 0.6 V versus RHE for H2O2 reduction. Further enhancement is achieved by depositing Pt as a cocatalyst, which ensured stability for over 20 h in an alkaline medium for water splitting. This study sets a new benchmark for developing CuFeO2‐based photocathodes, paving the way for broader particle transfer method applications.
{"title":"Scalable Reduced Graphene Oxide Conductive Layer‐Based Particulate Photocathodes for Photoelectrochemical Water Splitting","authors":"Ruiyuan Sun, Qinglu Liu, Qitao Liu, Weilong Qin, Jiabo Le, Xiaopei Ren, Muhammad Bilal Akbar, Yang Zhou, Chonghan Xia, Licheng Sun, Yongbo Kuang","doi":"10.1002/admt.202400392","DOIUrl":"https://doi.org/10.1002/admt.202400392","url":null,"abstract":"Particle transfer method photoelectrodes show superior photoelectrochemical performance compared to traditional powder‐based methods, making them a promising solution for solar water splitting in sustainable energy. This study introduces an innovative nonvacuum particle transfer method for fabricating photoelectrodes on a conductive carbon substrate, addressing the challenges associated with the high costs and vacuum deposition processes of traditional methods. Utilizing a p‐type CuFeO<jats:sub>2</jats:sub> powder semiconductor, a unique substrate is developed by applying a graphene oxide layer mixed with a small amount of silica binder on the particle layer's backside through ultrasonic atomization spraying. This layer is converted into multilayered reduced graphene oxide (ML‐rGO) via wet chemical reduction, resulting in a substrate boasting a high work function (4.8 eV), alongside remarkable chemical stability, mechanical strength, and conductivity. The fabricated CuFeO<jats:sub>2</jats:sub> photocathode demonstrated an onset potential of 0.97 V versus RHE and a photocurrent density of 1.5 mA cm<jats:sup>−2</jats:sup> at 0.6 V versus RHE for H<jats:sub>2</jats:sub>O<jats:sub>2</jats:sub> reduction. Further enhancement is achieved by depositing Pt as a cocatalyst, which ensured stability for over 20 h in an alkaline medium for water splitting. This study sets a new benchmark for developing CuFeO<jats:sub>2</jats:sub>‐based photocathodes, paving the way for broader particle transfer method applications.","PeriodicalId":7200,"journal":{"name":"Advanced Materials & Technologies","volume":"7 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142252316","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Suyun Li, Yanbo Shan, Jingyi Chen, Xiaotong Chen, Zengqin Shi, Lisheng Zhao, Rujie He, Ying Li
Piezoelectric composites have received widespread attentions in the fields of biomedicine and in vitro wearable devices due to their ability to convert mechanical forces into charge signals. The preparation of piezoelectric composites with complex structures through 3D printing technology can not only effectively improve their piezoelectric output, but also enable their customized therapeutic applications. This paper first introduces the types of piezoelectric composites and reviews the 3D printing technology commonly used in their preparation, analyzing the advantages and disadvantages of each 3D printing technology. Then, the state‐of‐the‐art of the biomedical applications of piezoelectric composites, including drug sustained‐release, wound healing promotion, bone tissue cells growth promoting, neurorehabilitation stimulating, ultrasonic diagnosis, and in vivo biosensing and in vitro wearable sensing, are emphasized. Finally, the main factors affecting the applications of 3D printed piezoelectric composites are outlooked, and an in‐depth discussion on the challenges toward 3D printed piezoelectric composites are analyzed. This review is believed to provide some fundamental knowledge of 3D printed piezoelectric composites.
压电复合材料能够将机械力转化为电荷信号，因此在生物医学和体外可穿戴设备领域受到广泛关注。通过三维打印技术制备具有复杂结构的压电复合材料，不仅能有效提高其压电输出，还能实现定制化治疗应用。本文首先介绍了压电复合材料的类型，并回顾了制备压电复合材料常用的 3D 打印技术，分析了每种 3D 打印技术的优缺点。然后，重点介绍了压电复合材料在生物医学方面的应用现状，包括药物缓释、促进伤口愈合、促进骨组织细胞生长、刺激神经康复、超声波诊断、体内生物传感和体外可穿戴传感等。最后，展望了影响 3D 打印压电复合材料应用的主要因素，并深入探讨了 3D 打印压电复合材料面临的挑战。相信这篇综述能为读者提供一些有关 3D 打印压电复合材料的基础知识。
{"title":"3D Printing and Biomedical Applications of Piezoelectric Composites: A Critical Review","authors":"Suyun Li, Yanbo Shan, Jingyi Chen, Xiaotong Chen, Zengqin Shi, Lisheng Zhao, Rujie He, Ying Li","doi":"10.1002/admt.202401160","DOIUrl":"https://doi.org/10.1002/admt.202401160","url":null,"abstract":"Piezoelectric composites have received widespread attentions in the fields of biomedicine and in vitro wearable devices due to their ability to convert mechanical forces into charge signals. The preparation of piezoelectric composites with complex structures through 3D printing technology can not only effectively improve their piezoelectric output, but also enable their customized therapeutic applications. This paper first introduces the types of piezoelectric composites and reviews the 3D printing technology commonly used in their preparation, analyzing the advantages and disadvantages of each 3D printing technology. Then, the state‐of‐the‐art of the biomedical applications of piezoelectric composites, including drug sustained‐release, wound healing promotion, bone tissue cells growth promoting, neurorehabilitation stimulating, ultrasonic diagnosis, and in vivo biosensing and in vitro wearable sensing, are emphasized. Finally, the main factors affecting the applications of 3D printed piezoelectric composites are outlooked, and an in‐depth discussion on the challenges toward 3D printed piezoelectric composites are analyzed. This review is believed to provide some fundamental knowledge of 3D printed piezoelectric composites.","PeriodicalId":7200,"journal":{"name":"Advanced Materials & Technologies","volume":"6 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142252321","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The next‐generation bionics and, more specifically, wearable and implantable bioelectronics require wireless, battery‐free, long‐term operation and seamless bio‐integration. Design considerations, materials choice, and implementation of efficient architectures have become crucial for the fabrication and deployment of wireless devices, especially if they are flexible or soft. Wireless power and data transfer represent key elements for the development of robust, efficient, and reliable systems for health monitoring, advanced disease diagnosis and treatment, personalized medicine. Here, the recent advances in materials and technologies used for wireless energy sourcing and telemetry in bio‐integrated flexible bionic and bioelectronic systems are reviewed. The study tackles different challenges related to mechanical compliance, low thickness, small footprint, biocompatibility, biodegradability, and in vivo implementation. The work also delves into the main figures of merit that are mostly adopted to quantify the wireless power/data transfer performances. Lastly, the pivotal applications of wearable and implantable wireless bionics/bioelectronics are summarized, such as electrical stimulation/recording, real‐time monitoring of physiological parameters, light delivery trough optical interfaces, electromechanical stimulation via ultrasounds, highlighting their potential for future implementation and the challenges related to their commercialization.
{"title":"Wireless Power and Data Transfer Technologies for Flexible Bionic and Bioelectronic Interfaces: Materials and Applications","authors":"Massimo Mariello, Christopher M. Proctor","doi":"10.1002/admt.202400797","DOIUrl":"https://doi.org/10.1002/admt.202400797","url":null,"abstract":"The next‐generation bionics and, more specifically, wearable and implantable bioelectronics require wireless, battery‐free, long‐term operation and seamless bio‐integration. Design considerations, materials choice, and implementation of efficient architectures have become crucial for the fabrication and deployment of wireless devices, especially if they are flexible or soft. Wireless power and data transfer represent key elements for the development of robust, efficient, and reliable systems for health monitoring, advanced disease diagnosis and treatment, personalized medicine. Here, the recent advances in materials and technologies used for wireless energy sourcing and telemetry in bio‐integrated flexible bionic and bioelectronic systems are reviewed. The study tackles different challenges related to mechanical compliance, low thickness, small footprint, biocompatibility, biodegradability, and in vivo implementation. The work also delves into the main figures of merit that are mostly adopted to quantify the wireless power/data transfer performances. Lastly, the pivotal applications of wearable and implantable wireless bionics/bioelectronics are summarized, such as electrical stimulation/recording, real‐time monitoring of physiological parameters, light delivery trough optical interfaces, electromechanical stimulation via ultrasounds, highlighting their potential for future implementation and the challenges related to their commercialization.","PeriodicalId":7200,"journal":{"name":"Advanced Materials & Technologies","volume":"15 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142194087","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
An e‐nose is built on a single graphene field effect transistor (GFET), based on a graphene/Si3N4/p‐Si stack of layers. Multichannel data acquisition, enabling to mimic the architecture of a sensor array, is achieved by steering the gate potential, thus yielding a virtual array of 2D chemiresistors on a single sensing layer. This setting allows for the detection of volatile compounds with a remarkable discrimination capability, boosted by intensive machine learning analysis and accuracy maximization through the choice of the number of virtual sensors. Sensing of gas phase NH3 is tested, along with a set of possible interferents, and discrimination of NH3+NO2 mixtures is successfully probed. High throughput in terms of sensitivity is achieved by tracking the shift of the minimum of the GFET transfer curve versus NH3 concentration. With this readout scheme, a 20‐fold sensitivity increase over a 5–50 ppm range is registered to the same layer used as a chemiresistor. High discrimination capability is probed by leveraging machine learning algorithms, from principal component analysis (PCA) to Uniform Manifold Approximation and Projection (U‐MAP) and, finally, to a Deep Neural Networks (DNN) where input neurons are the virtual sensors created by the gate voltage driving. For the tested case, the DNN maximum accuracy is achieved with 21 virtual sensors.
{"title":"Physical Virtualization of a GFET for a Versatile, High‐Throughput, and Highly Discriminating Detection of Target Gas Molecules at Room Temperature","authors":"Michele Zanotti, Sonia Freddi, Luigi Sangaletti","doi":"10.1002/admt.202400985","DOIUrl":"https://doi.org/10.1002/admt.202400985","url":null,"abstract":"An e‐nose is built on a single graphene field effect transistor (GFET), based on a graphene/Si<jats:sub>3</jats:sub>N<jats:sub>4</jats:sub>/p‐Si stack of layers. Multichannel data acquisition, enabling to mimic the architecture of a sensor array, is achieved by steering the gate potential, thus yielding a virtual array of 2D chemiresistors on a single sensing layer. This setting allows for the detection of volatile compounds with a remarkable discrimination capability, boosted by intensive machine learning analysis and accuracy maximization through the choice of the number of virtual sensors. Sensing of gas phase NH<jats:sub>3</jats:sub> is tested, along with a set of possible interferents, and discrimination of NH<jats:sub>3</jats:sub>+NO<jats:sub>2</jats:sub> mixtures is successfully probed. High throughput in terms of sensitivity is achieved by tracking the shift of the minimum of the GFET transfer curve versus NH<jats:sub>3</jats:sub> concentration. With this readout scheme, a 20‐fold sensitivity increase over a 5–50 ppm range is registered to the same layer used as a chemiresistor. High discrimination capability is probed by leveraging machine learning algorithms, from principal component analysis (PCA) to Uniform Manifold Approximation and Projection (U‐MAP) and, finally, to a Deep Neural Networks (DNN) where input neurons are the virtual sensors created by the gate voltage driving. For the tested case, the DNN maximum accuracy is achieved with 21 virtual sensors.","PeriodicalId":7200,"journal":{"name":"Advanced Materials & Technologies","volume":"164 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142194053","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Esther E. Jaekel, Rubina Ajdary, Nathan Holwell, Sean Mathew, Brian G. Amsden, Kevin J. De France, Orlando J. Rojas, Markus Antonietti, Svitlana Filonenko
Direct ink writing is especially relevant to the biomedical field due to the customizable extrusion and the possibility of creating pre‐designed architectures. Abundant natural polymers are sustainable and biocompatible alternatives to synthetic and persistent polymers. The printing of pure nanocellulose suspensions proves difficult due to low solid loadings, high shrinkage, as well as non‐fitting rheology. Emulsion gels (emulgel) alternatives gain attention in the field owing to their favorable viscoelastic properties and the possibility of creating multiphase systems. The authors’ sulfur‐free cationic cellulose nanocrystals (CNC) of low degree of substitution enable straightforward deployment in Pickering emulsions. An emulgel ink co‐stabilized by cationic CNC and α‐cyclodextrin is introduced as an interfacial inclusion complex. All ink components are natural and biodegradable compounds. The produced emulgel inks allow for high fidelity printing and minimum shrinkage upon drying that relaxes the need for supports, even in complex overhanging structures. A low yield stress (230–270 Pa) facilitates the inclusion of cells for biomedical applications into the formulation. The emulgel can be tuned to the desired rheological properties and be equipped with both polar and apolar compounds due to the biphasic system, making it a promising platform for biocompatible additive manufacturing.
{"title":"Bioinks from All‐Natural Pickering Emulgels Co‐Stabilized by Cationic CNC and Inclusion Complexes Formed by α‐Cyclodextrin","authors":"Esther E. Jaekel, Rubina Ajdary, Nathan Holwell, Sean Mathew, Brian G. Amsden, Kevin J. De France, Orlando J. Rojas, Markus Antonietti, Svitlana Filonenko","doi":"10.1002/admt.202400549","DOIUrl":"https://doi.org/10.1002/admt.202400549","url":null,"abstract":"Direct ink writing is especially relevant to the biomedical field due to the customizable extrusion and the possibility of creating pre‐designed architectures. Abundant natural polymers are sustainable and biocompatible alternatives to synthetic and persistent polymers. The printing of pure nanocellulose suspensions proves difficult due to low solid loadings, high shrinkage, as well as non‐fitting rheology. Emulsion gels (emulgel) alternatives gain attention in the field owing to their favorable viscoelastic properties and the possibility of creating multiphase systems. The authors’ sulfur‐free cationic cellulose nanocrystals (CNC) of low degree of substitution enable straightforward deployment in Pickering emulsions. An emulgel ink co‐stabilized by cationic CNC and α‐cyclodextrin is introduced as an interfacial inclusion complex. All ink components are natural and biodegradable compounds. The produced emulgel inks allow for high fidelity printing and minimum shrinkage upon drying that relaxes the need for supports, even in complex overhanging structures. A low yield stress (230–270 Pa) facilitates the inclusion of cells for biomedical applications into the formulation. The emulgel can be tuned to the desired rheological properties and be equipped with both polar and apolar compounds due to the biphasic system, making it a promising platform for biocompatible additive manufacturing.","PeriodicalId":7200,"journal":{"name":"Advanced Materials & Technologies","volume":"82 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142194080","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sayoni Sarkar, Diksha Malhotra, Monalisha Debnath, Gopal C. Kundu, Rohit Srivastava, Ajit R. Kulkarni
Semiconductor nanostructures with surface defect‐mediated chemistry have garnered pronounced interest due to their exceptional photo‐induced intracellular bio‐catalytic (enzyme‐mimicking) responses. However, designing defective nanozymes with pH‐responsive multi‐bio‐catalytic functions without any dopants is challenging. Herein, oxygen‐deficient “trojan horse‐like” folate‐functionalized, L‐arginine‐coated ceria (FA‐L‐arg‐CeO2) nanozymes with synergistic multi‐enzyme‐mimicking and anti‐cancer potential are introduced. Intrinsic surface oxygen vacancies (VO●) are strategically created in the nanozymes under kinetically favorable synthesis conditions. Increased surface VO● promotes band structure reconstruction and amplified photochemical‐response efficacy under single laser irradiation (808 nm), outperforming the defect‐free commercial nano‐CeO2 in rapid anti‐tumorigenic activities. Through folate receptor‐mediated endocytosis, these biostable nanozymes localized in MDA‐MB‐231 cells (84% in 48 h) and demonstrated NIR‐accelerated enzymatic functions depending on the pH of the biological milieu. The reduced band gap energy facilitated effective electron‐hole separation, up‐regulating in vitro photo‐redox reactions that impart exceptional therapeutic potential and inhibit 62% cell metastasis within only 12 h. By perturbing intratumoural redox homeostasis, VO●‐rich FA‐L‐arg‐CeO2 nanozymes unanimously killed 86% of MDA‐MB‐231 cancer cells while preferentially shielding benign L929 cells. Transcending beyond conventional drug‐loaded or dopant‐incorporated‐CeO2 nanoplatforms, these defective multi‐modal nanozymes unravel a new avenue for developing smart, low‐cost, bio‐active agents with enhanced efficacy and bio‐safety.
{"title":"Rationalizing Defective Biomimetic Ceria: In Vitro Demonstration of a Potential “Trojan Horse” Nanozyme Based‐Platform Leveraging Photo‐Redox Activities for Minimally Invasive Therapy","authors":"Sayoni Sarkar, Diksha Malhotra, Monalisha Debnath, Gopal C. Kundu, Rohit Srivastava, Ajit R. Kulkarni","doi":"10.1002/admt.202400556","DOIUrl":"https://doi.org/10.1002/admt.202400556","url":null,"abstract":"Semiconductor nanostructures with surface defect‐mediated chemistry have garnered pronounced interest due to their exceptional photo‐induced intracellular bio‐catalytic (enzyme‐mimicking) responses. However, designing defective nanozymes with pH‐responsive multi‐bio‐catalytic functions without any dopants is challenging. Herein, oxygen‐deficient “trojan horse‐like” folate‐functionalized, L‐arginine‐coated ceria (FA‐L‐arg‐CeO<jats:sub>2</jats:sub>) nanozymes with synergistic multi‐enzyme‐mimicking and anti‐cancer potential are introduced. Intrinsic surface oxygen vacancies (V<jats:sub>O</jats:sub><jats:sup>●</jats:sup>) are strategically created in the nanozymes under kinetically favorable synthesis conditions. Increased surface V<jats:sub>O</jats:sub><jats:sup>●</jats:sup> promotes band structure reconstruction and amplified photochemical‐response efficacy under single laser irradiation (808 nm), outperforming the defect‐free commercial nano‐CeO<jats:sub>2</jats:sub> in rapid anti‐tumorigenic activities. Through folate receptor‐mediated endocytosis, these biostable nanozymes localized in MDA‐MB‐231 cells (84% in 48 h) and demonstrated NIR‐accelerated enzymatic functions depending on the pH of the biological milieu. The reduced band gap energy facilitated effective electron‐hole separation, up‐regulating in vitro photo‐redox reactions that impart exceptional therapeutic potential and inhibit 62% cell metastasis within only 12 h. By perturbing intratumoural redox homeostasis, V<jats:sub>O</jats:sub><jats:sup>●</jats:sup>‐rich FA‐L‐arg‐CeO<jats:sub>2</jats:sub> nanozymes unanimously killed 86% of MDA‐MB‐231 cancer cells while preferentially shielding benign L929 cells. Transcending beyond conventional drug‐loaded or dopant‐incorporated‐CeO<jats:sub>2</jats:sub> nanoplatforms, these defective multi‐modal nanozymes unravel a new avenue for developing smart, low‐cost, bio‐active agents with enhanced efficacy and bio‐safety.","PeriodicalId":7200,"journal":{"name":"Advanced Materials & Technologies","volume":"12 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142194082","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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