In the 21st century’s wave of technological advancement, sensors, as a key component of the Internet of Things (IoT), have significantly propelled the development of smart cities and intelligent transportation systems. However, the high deployment costs of traditional sensors limit their practicality for large-scale applications and maintenance. To address this issue, this study proposes a low-cost, concealed, durable, and highly scalable multifunctional smart cement sensor based on triboelectric nanogenerators (SC-TENG) for constructing an all-weather intelligent monitoring system. By embedding differently shaped surface insulating electrodes into the cement and applying super-hydrophobic treatment to the cement surface, the SC-TENG can effectively monitor vehicle speed, measure vehicle length, and provide fencing warnings in public places at a low cost. Experimental results indicate that the SC-TENG can operate stably under various environmental conditions, maintaining stable output in ambient temperatures from 0 to 40 °C and relative humidity of 30%–70%, with negligible signal degradation even after approximately 2500 cycles. This research is significantly important for enhancing road safety, improving public security, and reducing energy consumption, providing technical support and solutions for the construction of smart cities.
{"title":"Multifunctional Smart Cement Sensor Based on Triboelectric Nanogenerators","authors":"Bochun Lai, Chenhui Xu, Yiran Hu, Yongyang Chen, Zhihui Li, Jiayue Zheng, Hanlin Zhou, Fangzhou Zhang* and Zhiyi Wu*, ","doi":"10.1021/acsaelm.4c0129010.1021/acsaelm.4c01290","DOIUrl":"https://doi.org/10.1021/acsaelm.4c01290https://doi.org/10.1021/acsaelm.4c01290","url":null,"abstract":"<p >In the 21st century’s wave of technological advancement, sensors, as a key component of the Internet of Things (IoT), have significantly propelled the development of smart cities and intelligent transportation systems. However, the high deployment costs of traditional sensors limit their practicality for large-scale applications and maintenance. To address this issue, this study proposes a low-cost, concealed, durable, and highly scalable multifunctional smart cement sensor based on triboelectric nanogenerators (SC-TENG) for constructing an all-weather intelligent monitoring system. By embedding differently shaped surface insulating electrodes into the cement and applying super-hydrophobic treatment to the cement surface, the SC-TENG can effectively monitor vehicle speed, measure vehicle length, and provide fencing warnings in public places at a low cost. Experimental results indicate that the SC-TENG can operate stably under various environmental conditions, maintaining stable output in ambient temperatures from 0 to 40 °C and relative humidity of 30%–70%, with negligible signal degradation even after approximately 2500 cycles. This research is significantly important for enhancing road safety, improving public security, and reducing energy consumption, providing technical support and solutions for the construction of smart cities.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"6 11","pages":"7923–7932 7923–7932"},"PeriodicalIF":4.3,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142713644","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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: 10.1021/acsaelm.4c0181810.1021/acsaelm.4c01818
Alok Ranjan*, Lunjie Zeng and Eva Olsson*,
High-κ gate dielectrics compatible with two-dimensional (2D) materials are crucial for advanced electronics, and Sb2O3 (antimony trioxide) shows significant potential. Here, we show that the soft breakdown induces oxygen vacancies and migration of copper into Sb2O3. Hard breakdown, driven by joule heating, gives rise to a substantial temperature increase, leading to morphological transformations and oxygen redistribution. In situ transmission electron microscopy (in situ TEM) measurements correlated with device performance show the formation of nanoconducting filaments due to the increased concentration of oxygen vacancies and copper migration in connection with the soft breakdown. The hard breakdown is associated with the formation of antimony-enriched nanocrystals. These findings offer critical insights into the suitability of Sb2O3 as a high-κ gate dielectric.
{"title":"Dielectric Breakdown Mechanisms in High-κ Antimony Trioxide (Sb2O3)","authors":"Alok Ranjan*, Lunjie Zeng and Eva Olsson*, ","doi":"10.1021/acsaelm.4c0181810.1021/acsaelm.4c01818","DOIUrl":"https://doi.org/10.1021/acsaelm.4c01818https://doi.org/10.1021/acsaelm.4c01818","url":null,"abstract":"<p >High-κ gate dielectrics compatible with two-dimensional (2D) materials are crucial for advanced electronics, and Sb<sub>2</sub>O<sub>3</sub> (antimony trioxide) shows significant potential. Here, we show that the soft breakdown induces oxygen vacancies and migration of copper into Sb<sub>2</sub>O<sub>3</sub>. Hard breakdown, driven by joule heating, gives rise to a substantial temperature increase, leading to morphological transformations and oxygen redistribution. In situ transmission electron microscopy (in situ TEM) measurements correlated with device performance show the formation of nanoconducting filaments due to the increased concentration of oxygen vacancies and copper migration in connection with the soft breakdown. The hard breakdown is associated with the formation of antimony-enriched nanocrystals. These findings offer critical insights into the suitability of Sb<sub>2</sub>O<sub>3</sub> as a high-κ gate dielectric.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"6 11","pages":"8540–8548 8540–8548"},"PeriodicalIF":4.3,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsaelm.4c01818","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142713594","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Stretchable thin film heaters (TFHs) are essential for localized thermotherapy, conforming to the skin and joints. However, conventional TFHs made from nonbreathable elastomers often cause discomfort and increase infection risks. We propose a sample TFH design that is both breathable and stretchable. By using nickel (Ni) foam as a sacrificial template, we deposit Ag nanowires (Ag NWs) to form the heating element, which is then encapsulated in polydimethylsiloxane (PDMS). Crucially, the PDMS coats only the inner surfaces of the micropipes, leaving the interstitial spaces unfilled, creating a breathable 3D conductive network. This contrasts with traditional TFHs that are typically nonbreathable and limited in flexibility, often leading to heat accumulation and discomfort. Our TFH maintained consistent performance over 1000 cycles of bending, stretching, and water immersion. Even with up to 25% stretching, resistance changes remained under 13%. Breathability tests revealed a 5:1 ratio in deionized water permeability between an uncovered bottle and one covered with our film with a permeation rate of 7 mg/cm2·h. Also, the TFH effectively reached 67 °C within 1 min under a 3.5 V bias. Unlike existing methods that neglect breathability or require complex fabrication, our strategy offers a simple yet robust solution to the limitations of conventional TFHs, combining both breathability and stretchability.
{"title":"Enhancing Comfort and Functionality in Stretchable Thermotherapy Thin Film Heaters through Breathable Design","authors":"Xinkong Wei, Yue Pei, Yunxia Li, Junyi Zhai* and Weihua Han*, ","doi":"10.1021/acsaelm.4c0161010.1021/acsaelm.4c01610","DOIUrl":"https://doi.org/10.1021/acsaelm.4c01610https://doi.org/10.1021/acsaelm.4c01610","url":null,"abstract":"<p >Stretchable thin film heaters (TFHs) are essential for localized thermotherapy, conforming to the skin and joints. However, conventional TFHs made from nonbreathable elastomers often cause discomfort and increase infection risks. We propose a sample TFH design that is both breathable and stretchable. By using nickel (Ni) foam as a sacrificial template, we deposit Ag nanowires (Ag NWs) to form the heating element, which is then encapsulated in polydimethylsiloxane (PDMS). Crucially, the PDMS coats only the inner surfaces of the micropipes, leaving the interstitial spaces unfilled, creating a breathable 3D conductive network. This contrasts with traditional TFHs that are typically nonbreathable and limited in flexibility, often leading to heat accumulation and discomfort. Our TFH maintained consistent performance over 1000 cycles of bending, stretching, and water immersion. Even with up to 25% stretching, resistance changes remained under 13%. Breathability tests revealed a 5:1 ratio in deionized water permeability between an uncovered bottle and one covered with our film with a permeation rate of 7 mg/cm<sup>2</sup>·h. Also, the TFH effectively reached 67 °C within 1 min under a 3.5 V bias. Unlike existing methods that neglect breathability or require complex fabrication, our strategy offers a simple yet robust solution to the limitations of conventional TFHs, combining both breathability and stretchability.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"6 11","pages":"8394–8403 8394–8403"},"PeriodicalIF":4.3,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142713596","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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 : 2024-11-05DOI: 10.1021/acs.iecr.4c0288610.1021/acs.iecr.4c02886
Yuxi Wu, Yuhong Tian*, Xinping He, Jiaxin Guo, Kaiya Yi and Chunhai Yi*,
Bioethanol, as a renewable energy source, is receiving continuous attention for efficient recovery in aqueous solution. In this work, high-permeable ethanol mix matrix membranes (MMMs) were prepared by incorporating covalent organic framework-300 (COF-300) into polydimethylsiloxane (PDMS) by solution blending. The morphology, functional groups, surface roughness, contact angle, and swelling degree of MMMs before and after COF-300 loading were characterized and analyzed. The encouraging finding is that the incorporation of porous COF-300 particles results in a significant enhancement of the hydrophobicity and ethanol affinity, which in turn increases the total flux and separation factor. The pervaporation results showed that the total flux reached 1515.28 g·m–2·h–1 and the separation factor reached 8.7 at a 3 wt % COF loading. Compared with pure PDMS, the total flux and separation factor of MMMs increased by 71.4 and 7.8%, respectively. Primarily based on the unique pore structure characteristics of COF-300, it can provide ultrafast channels for ethanol molecules. At the same time, COF-300 itself is a porous hydrophobicity particle with good ethanol affinity, which will promote the diffusion of ethanol molecules, further promote membrane swelling, and thus increase the separation factor and flux. Moreover, the MMMs in this work exhibited satisfactory stability during 6 months of continuous operation. Therefore, COF-300 is expected to be an ideal filler material to improve the separation performance of permeable ethanol membranes.
{"title":"Preparation of Covalent Organic Framework/PDMS Mixed Matrix Membranes for Efficient Ethanol Recovery via Pervaporation","authors":"Yuxi Wu, Yuhong Tian*, Xinping He, Jiaxin Guo, Kaiya Yi and Chunhai Yi*, ","doi":"10.1021/acs.iecr.4c0288610.1021/acs.iecr.4c02886","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c02886https://doi.org/10.1021/acs.iecr.4c02886","url":null,"abstract":"<p >Bioethanol, as a renewable energy source, is receiving continuous attention for efficient recovery in aqueous solution. In this work, high-permeable ethanol mix matrix membranes (MMMs) were prepared by incorporating covalent organic framework-300 (COF-300) into polydimethylsiloxane (PDMS) by solution blending. The morphology, functional groups, surface roughness, contact angle, and swelling degree of MMMs before and after COF-300 loading were characterized and analyzed. The encouraging finding is that the incorporation of porous COF-300 particles results in a significant enhancement of the hydrophobicity and ethanol affinity, which in turn increases the total flux and separation factor. The pervaporation results showed that the total flux reached 1515.28 g·m<sup>–2</sup>·h<sup>–1</sup> and the separation factor reached 8.7 at a 3 wt % COF loading. Compared with pure PDMS, the total flux and separation factor of MMMs increased by 71.4 and 7.8%, respectively. Primarily based on the unique pore structure characteristics of COF-300, it can provide ultrafast channels for ethanol molecules. At the same time, COF-300 itself is a porous hydrophobicity particle with good ethanol affinity, which will promote the diffusion of ethanol molecules, further promote membrane swelling, and thus increase the separation factor and flux. Moreover, the MMMs in this work exhibited satisfactory stability during 6 months of continuous operation. Therefore, COF-300 is expected to be an ideal filler material to improve the separation performance of permeable ethanol membranes.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"63 45","pages":"19756–19766 19756–19766"},"PeriodicalIF":3.8,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608371","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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 : 2024-11-05DOI: 10.1021/acsaelm.4c0146010.1021/acsaelm.4c01460
Yan-Ting Chen, Yu-Chih Hsu, Yan-Cheng Lin* and Yang-Yen Yu*,
This study synthesized copolymers using two biomass materials, starch and ι-carrageenan, with poly(acrylic acid) and utilized ethylene glycol as a solvent-based cross-linking agent to produce hydrogels. The hydrogels developed from starch or ι-carrageenan exhibited high extensibility and mechanical strength after absorbing water molecules from the environment and maturing. The Young’s modulus was approximately 0.03 and 0.04 GPa, with elongation exceeding 600%, and the water content remained stable at around 15% over time. Additionally, these hydrogels can be hydrolyzed and recycled to recreate elastomers with similar mechanical properties. By the incorporation of chlorophyll into the hydrogels made from the two biomass hydrogels, they were successfully used as memory layers in phototransistor memory. The hydrogel cross-linking involved the formation of covalent bonds between the hydroxy groups of the biomass materials and carboxylic acid groups of poly(acrylic acid), while the non-cross-linked parts interacted with chlorophyll through hydrogen bonding. The devices perform electrical writing by applying gate bias and optical erasure by exposing them to 455 nm blue light. Notably, the device made from starch-based hydrogel exhibits a high memory window (∼21.8 V) and long-term stability exceeding 104 s. In conclusion, this study successfully derived high-biomass-content hydrogels from biomass materials and applied them to optoelectronic devices, demonstrating the successful application of biomass materials in high-quality optoelectronic devices.
{"title":"Development and Application of Biomass Hydrogel in Photonic Transistor Memory","authors":"Yan-Ting Chen, Yu-Chih Hsu, Yan-Cheng Lin* and Yang-Yen Yu*, ","doi":"10.1021/acsaelm.4c0146010.1021/acsaelm.4c01460","DOIUrl":"https://doi.org/10.1021/acsaelm.4c01460https://doi.org/10.1021/acsaelm.4c01460","url":null,"abstract":"<p >This study synthesized copolymers using two biomass materials, starch and ι-carrageenan, with poly(acrylic acid) and utilized ethylene glycol as a solvent-based cross-linking agent to produce hydrogels. The hydrogels developed from starch or ι-carrageenan exhibited high extensibility and mechanical strength after absorbing water molecules from the environment and maturing. The Young’s modulus was approximately 0.03 and 0.04 GPa, with elongation exceeding 600%, and the water content remained stable at around 15% over time. Additionally, these hydrogels can be hydrolyzed and recycled to recreate elastomers with similar mechanical properties. By the incorporation of chlorophyll into the hydrogels made from the two biomass hydrogels, they were successfully used as memory layers in phototransistor memory. The hydrogel cross-linking involved the formation of covalent bonds between the hydroxy groups of the biomass materials and carboxylic acid groups of poly(acrylic acid), while the non-cross-linked parts interacted with chlorophyll through hydrogen bonding. The devices perform electrical writing by applying gate bias and optical erasure by exposing them to 455 nm blue light. Notably, the device made from starch-based hydrogel exhibits a high memory window (∼21.8 V) and long-term stability exceeding 10<sup>4</sup> s. In conclusion, this study successfully derived high-biomass-content hydrogels from biomass materials and applied them to optoelectronic devices, demonstrating the successful application of biomass materials in high-quality optoelectronic devices.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"6 11","pages":"8180–8189 8180–8189"},"PeriodicalIF":4.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142713577","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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 : 2024-11-05DOI: 10.1021/acsaelm.4c0130510.1021/acsaelm.4c01305
Steven J. DiGregorio, Mary Pat Nicodemus and Owen J. Hildreth*,
Self-reducing reactive silver inks are promising for printed electronics due to their low processing temperatures, high performance, and prolonged shelf life. Previous research showed that dense, high-quality silver can be printed without needing any postprint sintering steps by preferentially growing silver at the ink–substrate interface while also minimizing silver growth at the ink–vapor interface. This work builds on this concept and highlights importances of suppressing complexing agent evaporation rate to improve ink performance. By suppressing complexing agent evaporation increases silver formation at the ink–substrate interface, electrical conductivity improvement by over 2.5× for some ink formulations. Two independent studies demonstrate the benefits of this approach: one compares inks synthesized with varying vapor pressure complexing agents and the other prints inks in a complexing agent-rich environment to slow evaporation rates. Both approaches consistently yielded denser silver with lower resistances. For instance, using a propylamine complexing agent instead of ammonia at 40 °C resulted in a 96% decrease in resistance. Additionally, the ink printed at 100 °C with propylamine achieved state-of-the-art conductivity equivalent to 80% of bulk silver’s conductivity. The results confirm that slower complexing agent evaporation rates lead to denser silver with significantly lower resistances. This work introduces a unique strategy for enhancing ink performance that differs from conventional methods such as elevated temperatures, ink chemistry alterations, or postprocessing. The significantly improved low-temperature performance may broaden the applications of reactive silver inks and inspire future strategies that leverage suppressed complexing agent evaporation.
自还原反应银油墨具有加工温度低、性能高、保存期长等优点,因此在印刷电子产品中大有可为。先前的研究表明,通过在油墨-基底界面优先生长银,同时尽量减少油墨-蒸气界面的银生长,无需任何印后烧结步骤即可印制出致密的高质量银。这项工作以这一概念为基础,强调了抑制络合剂蒸发率对改善油墨性能的重要性。通过抑制络合剂的蒸发,增加了油墨-基底界面的银形成,某些油墨配方的导电率提高了 2.5 倍以上。两项独立的研究证明了这种方法的优势:一项研究比较了使用不同蒸汽压络合剂合成的油墨,另一项研究在富含络合剂的环境中印刷油墨,以减缓蒸发速度。这两种方法都能获得更致密、电阻更低的银。例如,在 40 °C 下使用丙胺络合剂而不是氨,电阻降低了 96%。此外,在 100 °C 下使用丙胺印刷的油墨达到了最先进的导电性,相当于块银导电性的 80%。结果证实,较慢的络合剂蒸发速度可使银更致密,电阻显著降低。这项研究提出了一种独特的提高油墨性能的策略,它不同于传统的方法,如升高温度、改变油墨化学成分或进行后处理。明显改善的低温性能可能会拓宽活性银油墨的应用范围,并启发未来利用抑制络合剂蒸发的策略。
{"title":"Improving the Density and Electrical Properties of Self-Reducing Reactive Silver Inks by Suppressing Complexing Agent Evaporation","authors":"Steven J. DiGregorio, Mary Pat Nicodemus and Owen J. Hildreth*, ","doi":"10.1021/acsaelm.4c0130510.1021/acsaelm.4c01305","DOIUrl":"https://doi.org/10.1021/acsaelm.4c01305https://doi.org/10.1021/acsaelm.4c01305","url":null,"abstract":"<p >Self-reducing reactive silver inks are promising for printed electronics due to their low processing temperatures, high performance, and prolonged shelf life. Previous research showed that dense, high-quality silver can be printed without needing any postprint sintering steps by preferentially growing silver at the ink–substrate interface while also minimizing silver growth at the ink–vapor interface. This work builds on this concept and highlights importances of suppressing complexing agent evaporation rate to improve ink performance. By suppressing complexing agent evaporation increases silver formation at the ink–substrate interface, electrical conductivity improvement by over 2.5× for some ink formulations. Two independent studies demonstrate the benefits of this approach: one compares inks synthesized with varying vapor pressure complexing agents and the other prints inks in a complexing agent-rich environment to slow evaporation rates. Both approaches consistently yielded denser silver with lower resistances. For instance, using a propylamine complexing agent instead of ammonia at 40 °C resulted in a 96% decrease in resistance. Additionally, the ink printed at 100 °C with propylamine achieved state-of-the-art conductivity equivalent to 80% of bulk silver’s conductivity. The results confirm that slower complexing agent evaporation rates lead to denser silver with significantly lower resistances. This work introduces a unique strategy for enhancing ink performance that differs from conventional methods such as elevated temperatures, ink chemistry alterations, or postprocessing. The significantly improved low-temperature performance may broaden the applications of reactive silver inks and inspire future strategies that leverage suppressed complexing agent evaporation.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"6 11","pages":"7950–7959 7950–7959"},"PeriodicalIF":4.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142719571","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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 : 2024-11-05DOI: 10.1021/acsaelm.4c0157110.1021/acsaelm.4c01571
Muhammad Sheeraz, Viet-Dung Tran, Yong Jin Jo, Gyehyeon Kim, Shinuk Cho, Changhee Sohn, Ill Won Kim, Young-Han Shin*, Chang Won Ahn* and Tae Heon Kim*,
Exotic physical phenomena in solids emerge with changes of nonlinear responses (e.g., polarization hysteresis under an electric field) of order parameters to external stimuli. In epitaxial ferroelectric films, polar ordering states of electric dipole moments cooperate with local disorder originating from thickness-dependent mitigation of misfit strain inherently and/or chemical off-stoichiometry extrinsically. The mutual interaction of electric polarization with both intrinsic and extrinsic factors in ferroelectric thin films produces sizable modification of ferroelectric hysteretic characteristics. Herein, we demonstrate defect-induced manipulation of ferroelectric hysteresis in epitaxial Bi1/2(Na,K)1/2TiO3 films. Notably, pinched hysteresis loops and linked double switching current behaviors are observed with the formation of screw dislocations on the surfaces of lead-free ferroelectric films grown at high temperatures. Plausibly, structural transitions of tetragonal phases to rhombohedral-like monoclinic symmetry driven by Na enrichment enable the appearance of ferroelastic domain variants, of which screw dislocations can be created to accommodate local stress at the boundaries. Polarization switching at the dislocation-mediated ferroelastic domain walls has been also limited and thereby, single ferroelectric hysteresis loops evolve to double-like hysteresis loops. Our result of defect-engineered ferroelectric hysteresis is of potential interest for designing advanced electronic devices such as functional energy storage and harvesters with high performance.
随着阶次参数的非线性响应(如电场下的极化滞后)对外部刺激的变化,固体中出现了奇异的物理现象。在外延铁电薄膜中,电偶极矩的极性有序状态与局部无序状态相互配合,而局部无序状态的产生是由于随厚度变化的内在错配应变和/或外在化学偏离化学计量的缓解。在铁电薄膜中,电极化与内在和外在因素的相互作用会对铁电滞回特性产生巨大的改变。在此,我们展示了外延 Bi1/2(Na,K)1/2TiO3 薄膜中缺陷诱导的铁电滞回操纵。值得注意的是,随着高温下生长的无铅铁电薄膜表面螺旋位错的形成,我们观察到了捏合磁滞环和相连的双开关电流行为。有理由相信,在 Na 富集的驱动下,四方相的结构转变为类似斜方晶系的单斜对称结构,这使得铁电畴变体得以出现,其中的螺旋位错可以在边界处形成以适应局部应力。位错介导的铁电弹性域壁的极化转换也受到了限制,因此,单铁电磁滞环演变成了双类磁滞环。我们的缺陷工程铁电磁滞结果对于设计先进的电子器件,如高性能的功能性能量存储和收集器具有潜在的意义。
{"title":"Defect Engineering of Ferroelectric Hysteresis in Lead-Free Bi1/2(Na,K)1/2TiO3 Thin Films","authors":"Muhammad Sheeraz, Viet-Dung Tran, Yong Jin Jo, Gyehyeon Kim, Shinuk Cho, Changhee Sohn, Ill Won Kim, Young-Han Shin*, Chang Won Ahn* and Tae Heon Kim*, ","doi":"10.1021/acsaelm.4c0157110.1021/acsaelm.4c01571","DOIUrl":"https://doi.org/10.1021/acsaelm.4c01571https://doi.org/10.1021/acsaelm.4c01571","url":null,"abstract":"<p >Exotic physical phenomena in solids emerge with changes of nonlinear responses (e.g., polarization hysteresis under an electric field) of order parameters to external stimuli. In epitaxial ferroelectric films, polar ordering states of electric dipole moments cooperate with local disorder originating from thickness-dependent mitigation of misfit strain inherently and/or chemical off-stoichiometry extrinsically. The mutual interaction of electric polarization with both intrinsic and extrinsic factors in ferroelectric thin films produces sizable modification of ferroelectric hysteretic characteristics. Herein, we demonstrate defect-induced manipulation of ferroelectric hysteresis in epitaxial Bi<sub>1/2</sub>(Na,K)<sub>1/2</sub>TiO<sub>3</sub> films. Notably, pinched hysteresis loops and linked double switching current behaviors are observed with the formation of screw dislocations on the surfaces of lead-free ferroelectric films grown at high temperatures. Plausibly, structural transitions of tetragonal phases to rhombohedral-like monoclinic symmetry driven by Na enrichment enable the appearance of ferroelastic domain variants, of which screw dislocations can be created to accommodate local stress at the boundaries. Polarization switching at the dislocation-mediated ferroelastic domain walls has been also limited and thereby, single ferroelectric hysteresis loops evolve to double-like hysteresis loops. Our result of defect-engineered ferroelectric hysteresis is of potential interest for designing advanced electronic devices such as functional energy storage and harvesters with high performance.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"6 11","pages":"8328–8338 8328–8338"},"PeriodicalIF":4.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142713575","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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 : 2024-11-04DOI: 10.1021/acs.iecr.4c0170610.1021/acs.iecr.4c01706
Satya Priyadarshi, Subhan Pal and Ravikrishnan Vinu*,
This study investigates the effect of combining a free-radical initiator, TEMPO (2,2,6,6-tetramethyl-1-piperidinyloxy), and a zeolite catalyst (HY) on the pyrolysis of JP-10 (exotetrahydrodicyclopentadiene) and 3-carene (3,7,7-trimethylbicyclo [4.1.0] hept-3-ene) for their use as endothermic hydrocarbon fuels. Analytical fast pyrolysis experiments were conducted at 445, 590, and 764 °C in a curie point pyrolyzer hyphenated with a gas chromatograph/mass spectrometer. The experiments explored different cracking methods: noncatalytic pyrolysis, free-radical initiator-assisted pyrolysis, zeolite (HY)-assisted pyrolysis, and a combined approach using both HY zeolite and TEMPO, for the pyrolysis of JP-10 and 3-carene. The results demonstrate that the combination of TEMPO and HY enhances the yield of low-molecular-weight (LMW) hydrocarbons compared to thermal cracking or cracking with either initiator or zeolite alone, especially at a low temperature. For JP-10, the TEMPO + HY-assisted cracking at 445 °C resulted in a combined LMW alkane and alkene yield of 19%, which is considerably higher than that achieved with HY-assisted cracking (14%) and TEMPO-assisted cracking (2%). Similarly, the TEMPO + HY-assisted pyrolysis of 3-carene at 445 °C produced ∼17% yield of LMW hydrocarbons, which was higher than the yields achieved using either TEMPO alone (1%) or HY alone (12%). Plausible free-radical reactions were proposed based on the detected products. The findings suggest that TEMPO can be an effective additive for enhancing the yield of LMW hydrocarbons from jet fuels for endothermic fuel applications.
本研究探讨了将自由基引发剂 TEMPO(2,2,6,6-四甲基-1-哌啶基氧基)和沸石催化剂(HY)结合使用对 JP-10(外四氢双环戊二烯)和 3-蒈烯(3,7,7-三甲基双环 [4.1.0] 庚-3-烯)热解的影响,以便将它们用作内热烃燃料。在与气相色谱仪/质谱仪相连接的居里点热解器中,在 445、590 和 764 °C 温度下进行了快速热解分析实验。实验探索了不同的裂解方法:非催化热解、自由基引发剂辅助热解、沸石(HY)辅助热解以及使用 HY 沸石和 TEMPO 的组合方法来热解 JP-10 和 3-蒈烯。结果表明,与热裂解或单独使用引发剂或沸石进行裂解相比,TEMPO 和 HY 的组合提高了低分子量 (LMW) 碳氢化合物的产量,尤其是在低温条件下。对于 JP-10,在 445 °C 下进行 TEMPO + HY 辅助裂解后,低分子量烷烃和烯烃的综合产率为 19%,大大高于 HY 辅助裂解(14%)和 TEMPO 辅助裂解(2%)的产率。同样,TEMPO + HY 辅助在 445 °C 高温分解 3-蒈烯时,低分子量碳氢化合物的产量为 17%,高于单独使用 TEMPO(1%)或单独使用 HY(12%)时的产量。根据检测到的产物,提出了一些似是而非的自由基反应。研究结果表明,TEMPO 可以作为一种有效的添加剂,提高喷气燃料中低分子量碳氢化合物的产率,用于内热燃料应用。
{"title":"TEMPO-Assisted Thermal and Catalytic Cracking of 3-Carene and JP-10 to Produce Low-Molecular-Weight Hydrocarbons","authors":"Satya Priyadarshi, Subhan Pal and Ravikrishnan Vinu*, ","doi":"10.1021/acs.iecr.4c0170610.1021/acs.iecr.4c01706","DOIUrl":"https://doi.org/10.1021/acs.iecr.4c01706https://doi.org/10.1021/acs.iecr.4c01706","url":null,"abstract":"<p >This study investigates the effect of combining a free-radical initiator, TEMPO (2,2,6,6-tetramethyl-1-piperidinyloxy), and a zeolite catalyst (HY) on the pyrolysis of JP-10 (exotetrahydrodicyclopentadiene) and 3-carene (3,7,7-trimethylbicyclo [4.1.0] hept-3-ene) for their use as endothermic hydrocarbon fuels. Analytical fast pyrolysis experiments were conducted at 445, 590, and 764 °C in a curie point pyrolyzer hyphenated with a gas chromatograph/mass spectrometer. The experiments explored different cracking methods: noncatalytic pyrolysis, free-radical initiator-assisted pyrolysis, zeolite (HY)-assisted pyrolysis, and a combined approach using both HY zeolite and TEMPO, for the pyrolysis of JP-10 and 3-carene. The results demonstrate that the combination of TEMPO and HY enhances the yield of low-molecular-weight (LMW) hydrocarbons compared to thermal cracking or cracking with either initiator or zeolite alone, especially at a low temperature. For JP-10, the TEMPO + HY-assisted cracking at 445 °C resulted in a combined LMW alkane and alkene yield of 19%, which is considerably higher than that achieved with HY-assisted cracking (14%) and TEMPO-assisted cracking (2%). Similarly, the TEMPO + HY-assisted pyrolysis of 3-carene at 445 °C produced ∼17% yield of LMW hydrocarbons, which was higher than the yields achieved using either TEMPO alone (1%) or HY alone (12%). Plausible free-radical reactions were proposed based on the detected products. The findings suggest that TEMPO can be an effective additive for enhancing the yield of LMW hydrocarbons from jet fuels for endothermic fuel applications.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"63 45","pages":"19435–19448 19435–19448"},"PeriodicalIF":3.8,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608007","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In this study, a MoO3@TiO2 composite core–shell material was developed to remove Rhodamine B (RhB) dye through synergistic adsorption and photocatalytic degradation. n–n heterostructures were formed by coupling n-type semiconductors to enhance the efficiency of photocarrier separation and photocatalytic performance. MoO3, which possesses strong adsorption capacity, was primarily used as a dye adsorbent. Additionally, the formation of an n–n heterojunction with TiO2 enabled MoO3 to expand the photocorresponding range of TiO2, leading to the generation of superoxide (O2•) and hydroxyl (•OH) free radicals for dye degradation. The experimental results demonstrate that the MoO3@TiO2 core–shell composite exhibits excellent performance for RhB dye removal, with adsorption and degradation rates reaching 35.7 and 70.3%, respectively, even at low catalyst concentrations. This approach offers new insights into the development of MoO3 core–shell photocatalysts.
{"title":"Degradation of Rhodamine B by Visible Light Driven MoO3@TiO2 Core–Shell Photocatalyst","authors":"Hejin Liu, Peng Qiao, Ying Liu, Xin Guo, Yanxiu Liu, Hua Song, Xueqin Wang* and Wenyi Wang*, ","doi":"10.1021/acs.langmuir.4c0333310.1021/acs.langmuir.4c03333","DOIUrl":"https://doi.org/10.1021/acs.langmuir.4c03333https://doi.org/10.1021/acs.langmuir.4c03333","url":null,"abstract":"<p >In this study, a MoO<sub>3</sub>@TiO<sub>2</sub> composite core–shell material was developed to remove Rhodamine B (RhB) dye through synergistic adsorption and photocatalytic degradation. n–n heterostructures were formed by coupling n-type semiconductors to enhance the efficiency of photocarrier separation and photocatalytic performance. MoO<sub>3</sub>, which possesses strong adsorption capacity, was primarily used as a dye adsorbent. Additionally, the formation of an n–n heterojunction with TiO<sub>2</sub> enabled MoO<sub>3</sub> to expand the photocorresponding range of TiO<sub>2</sub>, leading to the generation of superoxide (O<sub>2</sub><sup>•</sup>) and hydroxyl (<sup>•</sup>OH) free radicals for dye degradation. The experimental results demonstrate that the MoO<sub>3</sub>@TiO<sub>2</sub> core–shell composite exhibits excellent performance for RhB dye removal, with adsorption and degradation rates reaching 35.7 and 70.3%, respectively, even at low catalyst concentrations. This approach offers new insights into the development of MoO<sub>3</sub> core–shell photocatalysts.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"40 45","pages":"24029–24036 24029–24036"},"PeriodicalIF":3.7,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608009","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}