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Proton Conduction in Zirconium-Based Metal–Organic Frameworks for Advanced Applications
IF 4.3 3区 材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC Pub Date : 2025-04-03 DOI: 10.1021/acsaelm.5c0018310.1021/acsaelm.5c00183
Kai-Xin Zhao, Guo-Qin Zhang, Xin-Ru Wu, Hong-Bin Luo*, Zhi-Xing Han, Yangyang Liu* and Xiao-Ming Ren, 

Zirconium-based metal–organic frameworks (Zr-MOFs) have emerged as a promising class of crystalline porous materials, attracting significant interest in the field of proton conduction due to their exceptional chemical stability, structural flexibility, and functional tunability. Notably, proton-conducting Zr-MOFs show immense potential for diverse advanced technological applications. In this Spotlight on Applications paper, we provide an overview of proton-conducting Zr-MOFs and spotlight the recent progress of their utilization as proton exchange membranes in proton exchange membrane fuel cells (PEMFCs), light-responsive systems for proton pumps, and chemical sensors for formic acid detection. Furthermore, we also discussed the challenges, future prospects, and opportunities for promoting the application of proton-conducting Zr-MOFs.

{"title":"Proton Conduction in Zirconium-Based Metal–Organic Frameworks for Advanced Applications","authors":"Kai-Xin Zhao,&nbsp;Guo-Qin Zhang,&nbsp;Xin-Ru Wu,&nbsp;Hong-Bin Luo*,&nbsp;Zhi-Xing Han,&nbsp;Yangyang Liu* and Xiao-Ming Ren,&nbsp;","doi":"10.1021/acsaelm.5c0018310.1021/acsaelm.5c00183","DOIUrl":"https://doi.org/10.1021/acsaelm.5c00183https://doi.org/10.1021/acsaelm.5c00183","url":null,"abstract":"<p >Zirconium-based metal–organic frameworks (Zr-MOFs) have emerged as a promising class of crystalline porous materials, attracting significant interest in the field of proton conduction due to their exceptional chemical stability, structural flexibility, and functional tunability. Notably, proton-conducting Zr-MOFs show immense potential for diverse advanced technological applications. In this Spotlight on Applications paper, we provide an overview of proton-conducting Zr-MOFs and spotlight the recent progress of their utilization as proton exchange membranes in proton exchange membrane fuel cells (PEMFCs), light-responsive systems for proton pumps, and chemical sensors for formic acid detection. Furthermore, we also discussed the challenges, future prospects, and opportunities for promoting the application of proton-conducting Zr-MOFs.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"7 8","pages":"3164–3175 3164–3175"},"PeriodicalIF":4.3,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsaelm.5c00183","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853999","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}
引用次数: 0
Photoresponse Evaluation of a Multiband Self-Driven SnO2/CuO/Si Heterojunction Photodetector Fabricated by Pulsed Laser Deposition
IF 4.3 3区 材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC Pub Date : 2025-04-03 DOI: 10.1021/acsaelm.5c0011810.1021/acsaelm.5c00118
Sabreen A. Khalaf, Ethar Yahya Salih*, Asmiet Ramizy, Raid A. Ismail and Mustafa K. A. Mohammed*, 

In this Article, a systematic multiband (p-n and n-p-n) analysis of a self-powered SnO2/CuO/Si heterojunction photodetector was conducted, considering both incident wavelength and light intensity episodes. Furthermore, the microstructural and optical features of the acquired layers were examined. The topography investigations revealed that the average diameters of the nanoparticles were 43.3 and 57.9 nm for the CuO and SnO2 films, respectively, with corresponding optical bandgaps of 1.98 and 3.75 eV. Additionally, the investigated junctions (n-SnO2/n-Si, p-CuO/n-Si, and n-SnO2/p-CuO) demonstrated distinguished figure-of-merits at zero bias voltage, highlighting the self-driven nature of the proposed geometry over the scanned wavelength range. Two primary driving bands were observed at 340 and 625 nm. Particularly, the n-SnO2/p-CuO structure exhibited a responsivity (Rλ) of 19.37 mA/W and a specific detectivity (D*) of 7.1 × 1011 Jones at 625 nm and 25.3 μW/cm2; these values decreased at 340 nm. The proposed structures also showed reduced figure-of-merits at higher incident light intensities, with an Rλ of 8.9 mA/W and a D* of 3.2 × 1011 Jones observed for the addressed junction at 67.8 μW/cm2. The time-resolved profile indicated fast response and recovery times (τRF) of 190 and 250 ms, respectively. An energy-band diagram of a SnO2/CuO heterojunction photodetector under incident light was also proposed.

{"title":"Photoresponse Evaluation of a Multiband Self-Driven SnO2/CuO/Si Heterojunction Photodetector Fabricated by Pulsed Laser Deposition","authors":"Sabreen A. Khalaf,&nbsp;Ethar Yahya Salih*,&nbsp;Asmiet Ramizy,&nbsp;Raid A. Ismail and Mustafa K. A. Mohammed*,&nbsp;","doi":"10.1021/acsaelm.5c0011810.1021/acsaelm.5c00118","DOIUrl":"https://doi.org/10.1021/acsaelm.5c00118https://doi.org/10.1021/acsaelm.5c00118","url":null,"abstract":"<p >In this Article, a systematic multiband (p-n and n-p-n) analysis of a self-powered SnO<sub>2</sub>/CuO/Si heterojunction photodetector was conducted, considering both incident wavelength and light intensity episodes. Furthermore, the microstructural and optical features of the acquired layers were examined. The topography investigations revealed that the average diameters of the nanoparticles were 43.3 and 57.9 nm for the CuO and SnO<sub>2</sub> films, respectively, with corresponding optical bandgaps of 1.98 and 3.75 eV. Additionally, the investigated junctions (n-SnO<sub>2</sub>/n-Si, p-CuO/n-Si, and n-SnO<sub>2</sub>/p-CuO) demonstrated distinguished figure-of-merits at zero bias voltage, highlighting the self-driven nature of the proposed geometry over the scanned wavelength range. Two primary driving bands were observed at 340 and 625 nm. Particularly, the n-SnO<sub>2</sub>/p-CuO structure exhibited a responsivity (<i>R</i><sub>λ</sub>) of 19.37 mA/W and a specific detectivity (<i>D</i>*) of 7.1 × 10<sup>11</sup> Jones at 625 nm and 25.3 μW/cm<sup>2</sup>; these values decreased at 340 nm. The proposed structures also showed reduced figure-of-merits at higher incident light intensities, with an <i>R</i><sub>λ</sub> of 8.9 mA/W and a <i>D</i>* of 3.2 × 10<sup>11</sup> Jones observed for the addressed junction at 67.8 μW/cm<sup>2</sup>. The time-resolved profile indicated fast response and recovery times (τ<sub>R</sub>/τ<sub>F</sub>) of 190 and 250 ms, respectively. An energy-band diagram of a SnO<sub>2</sub>/CuO heterojunction photodetector under incident light was also proposed.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"7 8","pages":"3409–3415 3409–3415"},"PeriodicalIF":4.3,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143854014","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}
引用次数: 0
Probing n-Type Conduction in Eumelanin Using Organic Electrochemical Transistors 利用有机电化学晶体管探测乌梅素中的 n 型传导
IF 4.3 3区 材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC Pub Date : 2025-04-03 DOI: 10.1021/acsaelm.5c0029310.1021/acsaelm.5c00293
Natan L. Nozella, João V. Paulin, Gabriel L. Nogueira, Nayrim B. Guerra, Rafael F. de Oliveira* and Carlos F. O. Graeff*, 

Sustainability demands innovative materials and technologies to address environmental and societal needs. In this context, natural biomaterials are gaining significant attention, with eumelanin (EuM) standing out due to its biocompatibility, abundance, and distinct electronic properties. However, the conducting nature of EuM and the main carrier involved in the charge transport have been the subject of a long-standing and inconclusive debate. This work contributes to this discussion by presenting the observation of n-type conduction in EuM films employed as channel material in organic electrochemical transistors (OECTs). The device current is modulated based on strong ionic electronic coupling between electrolyte cations and the π electron system of EuM’s indole units, resulting in charge mobility of μOECT = 0.019 ± 0.016 cm2 V–1 s–1. Our findings provide an innovative contribution to the ongoing debate on the semiconducting properties of EuM and demonstrate a novel electronic device, highlighting the remarkable potential of EuM for sustainable electronics.

{"title":"Probing n-Type Conduction in Eumelanin Using Organic Electrochemical Transistors","authors":"Natan L. Nozella,&nbsp;João V. Paulin,&nbsp;Gabriel L. Nogueira,&nbsp;Nayrim B. Guerra,&nbsp;Rafael F. de Oliveira* and Carlos F. O. Graeff*,&nbsp;","doi":"10.1021/acsaelm.5c0029310.1021/acsaelm.5c00293","DOIUrl":"https://doi.org/10.1021/acsaelm.5c00293https://doi.org/10.1021/acsaelm.5c00293","url":null,"abstract":"<p >Sustainability demands innovative materials and technologies to address environmental and societal needs. In this context, natural biomaterials are gaining significant attention, with eumelanin (EuM) standing out due to its biocompatibility, abundance, and distinct electronic properties. However, the conducting nature of EuM and the main carrier involved in the charge transport have been the subject of a long-standing and inconclusive debate. This work contributes to this discussion by presenting the observation of n-type conduction in EuM films employed as channel material in organic electrochemical transistors (OECTs). The device current is modulated based on strong ionic electronic coupling between electrolyte cations and the π electron system of EuM’s indole units, resulting in charge mobility of μ<sub>OECT</sub> = 0.019 ± 0.016 cm<sup>2</sup> V<sup>–1</sup> s<sup>–1</sup>. Our findings provide an innovative contribution to the ongoing debate on the semiconducting properties of EuM and demonstrate a novel electronic device, highlighting the remarkable potential of EuM for sustainable electronics.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"7 8","pages":"3176–3181 3176–3181"},"PeriodicalIF":4.3,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsaelm.5c00293","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853989","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}
引用次数: 0
Tailoring Contact Properties in Janus TMD Spin-FETs for Enhanced Spin Transport: A Bilayer Interface Approach
IF 4.3 3区 材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC Pub Date : 2025-04-02 DOI: 10.1021/acsaelm.5c0001910.1021/acsaelm.5c00019
Saheb Bera,  and , Hemant Kumar*, 

Janus transition metal dichalcogenides (TMDs) are promising two-dimensional (2D) semiconducting materials for spin field-effect transistor (spinFET) applications due to their strong spin–orbit coupling and broken out-of-plane inversion symmetry. However, maintaining a smooth interface between Janus TMDs and bulk ferromagnetic metals in spinFET is challenging due to the metal-induced gap states (MIGS) created by interface dangling bonds. In this study, we have shown that the insertion of an additional layer of Janus TMD as a buffer electrode between the ferromagnetic electrode and the Janus TMD channel effectively eliminates MIGS. Also, this buffer layer reduces the Schottky barrier height by creating a dipole moment at the interface between the top and bottom Janus TMD layers. Furthermore, the transition from n-type to p-type contact is achievable by altering the polarity of the interface dipole, which is associated with the direction of charge transfer at the metal–semiconductor interface. We also show that the tunneling probability of charge carriers can be enhanced by applying interlayer strain. Additionally, we find that the spin-polarization factor exceeds 60% at the ferromagnetic metal-bilayer Janus TMD interface, which is favorable for spin-polarized carrier transmission in spinFETs. Our results provide a roadmap for designing Janus TMD-based spinFETs for low-power, ultrafast neuromorphic device applications.

{"title":"Tailoring Contact Properties in Janus TMD Spin-FETs for Enhanced Spin Transport: A Bilayer Interface Approach","authors":"Saheb Bera,&nbsp; and ,&nbsp;Hemant Kumar*,&nbsp;","doi":"10.1021/acsaelm.5c0001910.1021/acsaelm.5c00019","DOIUrl":"https://doi.org/10.1021/acsaelm.5c00019https://doi.org/10.1021/acsaelm.5c00019","url":null,"abstract":"<p >Janus transition metal dichalcogenides (TMDs) are promising two-dimensional (2D) semiconducting materials for spin field-effect transistor (spinFET) applications due to their strong spin–orbit coupling and broken out-of-plane inversion symmetry. However, maintaining a smooth interface between Janus TMDs and bulk ferromagnetic metals in spinFET is challenging due to the metal-induced gap states (MIGS) created by interface dangling bonds. In this study, we have shown that the insertion of an additional layer of Janus TMD as a buffer electrode between the ferromagnetic electrode and the Janus TMD channel effectively eliminates MIGS. Also, this buffer layer reduces the Schottky barrier height by creating a dipole moment at the interface between the top and bottom Janus TMD layers. Furthermore, the transition from n-type to p-type contact is achievable by altering the polarity of the interface dipole, which is associated with the direction of charge transfer at the metal–semiconductor interface. We also show that the tunneling probability of charge carriers can be enhanced by applying interlayer strain. Additionally, we find that the spin-polarization factor exceeds 60% at the ferromagnetic metal-bilayer Janus TMD interface, which is favorable for spin-polarized carrier transmission in spinFETs. Our results provide a roadmap for designing Janus TMD-based spinFETs for low-power, ultrafast neuromorphic device applications.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"7 8","pages":"3324–3332 3324–3332"},"PeriodicalIF":4.3,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143854343","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}
引用次数: 0
Dual-Sided Microstructured rGO–CNT Flexible Sensors for High-Sensitivity and Wide-Range Pressure Detection
IF 4.3 3区 材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC Pub Date : 2025-04-02 DOI: 10.1021/acsaelm.4c0219410.1021/acsaelm.4c02194
Xiaomeng Yang, Hui Sun, Yu Feng, Xiaodong Yu, Hongyu Zhang, Meng Chen, Guanglie Zhang* and Wen Jung Li*, 

Recent advancements in flexible electronics have highlighted the importance of microstructured sensor designs for enhancing device performance. However, developing thin-film sensors that maintain both high sensitivity and wide measurement range remains a significant challenge. We present a pressure sensor that combines reduced graphene oxide (rGO), carbon nanotubes (CNT), and polydimethylsiloxane (PDMS) in a microstructured architecture. The sensor incorporates a pressure-sensitive film featuring double-sided embossed microstructured surfaces. This unique design enables a remarkable measurement range of 0–180 kPa while preserving exceptional sensitivity of 0.2 kPa–1 in the 0–13 kPa range. The exceptional performance attributes of this sensor make it highly suitable for applications demanding both precision at low pressures and broad operational capabilities. We have demonstrated the versatility of this sensor by successfully employing it for handwriting recognition and plantar pressure monitoring applications. This work represents a significant advancement in the field of flexible film sensors, paving the way for their widespread adoption in real-world applications, from wearable electronics to human–machine interfaces.

{"title":"Dual-Sided Microstructured rGO–CNT Flexible Sensors for High-Sensitivity and Wide-Range Pressure Detection","authors":"Xiaomeng Yang,&nbsp;Hui Sun,&nbsp;Yu Feng,&nbsp;Xiaodong Yu,&nbsp;Hongyu Zhang,&nbsp;Meng Chen,&nbsp;Guanglie Zhang* and Wen Jung Li*,&nbsp;","doi":"10.1021/acsaelm.4c0219410.1021/acsaelm.4c02194","DOIUrl":"https://doi.org/10.1021/acsaelm.4c02194https://doi.org/10.1021/acsaelm.4c02194","url":null,"abstract":"<p >Recent advancements in flexible electronics have highlighted the importance of microstructured sensor designs for enhancing device performance. However, developing thin-film sensors that maintain both high sensitivity and wide measurement range remains a significant challenge. We present a pressure sensor that combines reduced graphene oxide (rGO), carbon nanotubes (CNT), and polydimethylsiloxane (PDMS) in a microstructured architecture. The sensor incorporates a pressure-sensitive film featuring double-sided embossed microstructured surfaces. This unique design enables a remarkable measurement range of 0–180 kPa while preserving exceptional sensitivity of 0.2 kPa<sup>–1</sup> in the 0–13 kPa range. The exceptional performance attributes of this sensor make it highly suitable for applications demanding both precision at low pressures and broad operational capabilities. We have demonstrated the versatility of this sensor by successfully employing it for handwriting recognition and plantar pressure monitoring applications. This work represents a significant advancement in the field of flexible film sensors, paving the way for their widespread adoption in real-world applications, from wearable electronics to human–machine interfaces.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"7 8","pages":"3244–3254 3244–3254"},"PeriodicalIF":4.3,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsaelm.4c02194","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143854345","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}
引用次数: 0
Impedimetric Immunosensor for 5-Methylcytosine Detection Based on a Poly(o-phenylenediamine)-Encapsulated Gold Nanoparticle Platform
IF 4.3 3区 材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC Pub Date : 2025-04-02 DOI: 10.1021/acsaelm.5c0021610.1021/acsaelm.5c00216
Pedro C. M. Pizzol, Miquéias L. Portugal, Heitor F. Trevizan, Patrícia Monteiro Seraphim and Marcos F. S. Teixeira*, 

A label-free impedimetric immunosensor for the detection of 5-methylcytosine (5-mC), a key epigenetic marker, was developed based on a one-step electropolymerized nanocomposite of poly(o-phenylenediamine) (poly(o-PD)) and gold nanoparticles (AuNPs). The nanocomposite film was electropolymerized onto a screen-printed electrode (SPE) with a gold working electrode area of 0.0078 cm2. The system was characterized by cyclic voltammetry and electrochemical impedance spectroscopy (EIS). The EIS measurements, including Nyquist, Bode, and complex capacitance plots, confirmed the successful formation of the nanocomposite and its stepwise modification with glutaraldehyde, anti-5-methylcytosine antibody (Ab-5mC), and bovine serum albumin (BSA). The immunosensor utilized the inherent redox activity of the poly(o-PD) toward dissolved oxygen as a transduction mechanism, eliminating the need for external redox mediators. The binding of 5-mC to the immobilized Ab-5mC hindered the access of dissolved oxygen to the redox-active phenazine-like units within the poly(o-PD) matrix, resulting in a measurable increase in the charge transfer resistance. The immunosensor exhibited a linear response to the logarithm of 5-mC concentration in the range of 2.5 to 160 pg mL–1, with a low limit of detection (LOD) of 1.73 and 1.18 pg mL–1 when using the imaginary and absolute impedance, respectively. The incorporation of AuNPs significantly enhanced the electrochemically active surface area and improved the electron transfer kinetics, contributing to the high sensitivity of the immunosensor. This work demonstrates the potential of a one-step electropolymerized poly(o-PD)-AuNP nanocomposite for the development of simple, label-free, and sensitive impedimetric immunosensors for epigenetic biomarker detection.

基于聚(邻苯二胺)(poly(o-PD))和金纳米粒子(AuNPs)的一步电聚合纳米复合材料,开发了一种用于检测关键表观遗传标记--5-甲基胞嘧啶(5-mC)的无标记阻抗免疫传感器。纳米复合薄膜被电聚合到金工作电极面积为 0.0078 cm2 的丝网印刷电极(SPE)上。该系统通过循环伏安法和电化学阻抗谱(EIS)进行表征。包括奈奎斯特图、波特图和复合电容图在内的电化学阻抗谱测量结果证实了纳米复合材料的成功形成及其与戊二醛、抗 5-甲基胞嘧啶抗体(Ab-5mC)和牛血清白蛋白(BSA)的逐步修饰。该免疫传感器利用聚(邻-PD)对溶解氧的固有氧化还原活性作为传导机制,无需外部氧化还原介质。5-mC 与固定化 Ab-5mC 的结合阻碍了溶解氧进入聚(邻-PD)基质中具有氧化还原活性的酚嗪类单元,从而导致电荷转移电阻明显增加。在 2.5 至 160 pg mL-1 的范围内,免疫传感器对 5-mC 浓度的对数呈线性响应,使用虚阻抗和绝对阻抗时,检测限(LOD)分别为 1.73 和 1.18 pg mL-1。AuNPs 的加入显著提高了电化学活性表面积,改善了电子传递动力学,从而提高了免疫传感器的灵敏度。这项工作证明了一步法电聚合聚(邻-PD)-AuNP 纳米复合材料在开发用于表观遗传生物标记检测的简单、无标记、灵敏的阻抗免疫传感器方面的潜力。
{"title":"Impedimetric Immunosensor for 5-Methylcytosine Detection Based on a Poly(o-phenylenediamine)-Encapsulated Gold Nanoparticle Platform","authors":"Pedro C. M. Pizzol,&nbsp;Miquéias L. Portugal,&nbsp;Heitor F. Trevizan,&nbsp;Patrícia Monteiro Seraphim and Marcos F. S. Teixeira*,&nbsp;","doi":"10.1021/acsaelm.5c0021610.1021/acsaelm.5c00216","DOIUrl":"https://doi.org/10.1021/acsaelm.5c00216https://doi.org/10.1021/acsaelm.5c00216","url":null,"abstract":"<p >A label-free impedimetric immunosensor for the detection of 5-methylcytosine (5-mC), a key epigenetic marker, was developed based on a one-step electropolymerized nanocomposite of poly(<i>o</i>-phenylenediamine) (poly(o-PD)) and gold nanoparticles (AuNPs). The nanocomposite film was electropolymerized onto a screen-printed electrode (SPE) with a gold working electrode area of 0.0078 cm<sup>2</sup>. The system was characterized by cyclic voltammetry and electrochemical impedance spectroscopy (EIS). The EIS measurements, including Nyquist, Bode, and complex capacitance plots, confirmed the successful formation of the nanocomposite and its stepwise modification with glutaraldehyde, anti-5-methylcytosine antibody (Ab-5mC), and bovine serum albumin (BSA). The immunosensor utilized the inherent redox activity of the poly(o-PD) toward dissolved oxygen as a transduction mechanism, eliminating the need for external redox mediators. The binding of 5-mC to the immobilized Ab-5mC hindered the access of dissolved oxygen to the redox-active phenazine-like units within the poly(o-PD) matrix, resulting in a measurable increase in the charge transfer resistance. The immunosensor exhibited a linear response to the logarithm of 5-mC concentration in the range of 2.5 to 160 pg mL<sup>–1</sup>, with a low limit of detection (LOD) of 1.73 and 1.18 pg mL<sup>–1</sup> when using the imaginary and absolute impedance, respectively. The incorporation of AuNPs significantly enhanced the electrochemically active surface area and improved the electron transfer kinetics, contributing to the high sensitivity of the immunosensor. This work demonstrates the potential of a one-step electropolymerized poly(o-PD)-AuNP nanocomposite for the development of simple, label-free, and sensitive impedimetric immunosensors for epigenetic biomarker detection.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"7 8","pages":"3486–3500 3486–3500"},"PeriodicalIF":4.3,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsaelm.5c00216","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143854348","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}
引用次数: 0
Miniaturized Micrometer-Level Copper Wiring and Electrodes Based on Reverse-Offset Printing for Flexible Circuits
IF 4.3 3区 材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC Pub Date : 2025-04-02 DOI: 10.1021/acsaelm.5c0023010.1021/acsaelm.5c00230
Kim Eiroma*, Asko Sneck, Olli Halonen, Tuomas Happonen, Henrik Sandberg and Jaakko Leppäniemi*, 

High-resolution reverse-offset printing (ROP) is developed for miniaturization of printed electronics, resulting in a notable decrease in material usage compared to conventional printing processes. Two alternative ROP processes for patterning of metal conductors are available that are comparable in their cost per sample: direct nanoparticle (NP) printing (e.g., Ag and Cu) and patterning of vacuum-deposited metal (Ag, Al, Au, Cu, Ti, etc.) films using ROP printed polymer resist ink and the lift-off (LO) process. In this work, we focus on ROP of Cu NP ink followed by intense pulsed light (IPL) sintering and vacuum-deposited Cu patterned by ROP lift-off (LO). The good large-scale uniformity of the two processes is demonstrated by a grid of 300 individual thickness, sheet resistance, and resistivity measurement points with low variation over the 10 cm × 10 cm printed sample area. Sheet resistances of 0.56 ± 0.03 and 1.23 ± 0.05 Ω/□ are obtained at 113 and 40 nm thickness for Cu NP and Cu LO, respectively. Both processes show <5% thickness variation over a large area. A line-space (L/S) resolution of 2 μm is obtained for ROP patterned vacuum-deposited Cu having very low line edge roughness (LER) (∼60 nm), whereas for direct ROP printed Cu NP ink, the L/S resolution (2–4 μm) is limited by LER (∼900 nm) and influenced by the printed layer thickness. Based on the two fabrication routes, a flexible chip component assembly process is presented. Preliminary bending resistance results indicate that both ROP-based patterning processes yield a robust electrical interconnection between the ultrathin polyimide (PI) 5 mm × 5 mm chip and thermoplastic polyurethane (TPU). ROP shows promise as a scalable and sustainable patterning method for flexible ICs/chips that are assembled on flexible, stretchable, or biodegradable substrates and used, e.g., in wearable, large-scale sensing, and in environmental monitoring.

{"title":"Miniaturized Micrometer-Level Copper Wiring and Electrodes Based on Reverse-Offset Printing for Flexible Circuits","authors":"Kim Eiroma*,&nbsp;Asko Sneck,&nbsp;Olli Halonen,&nbsp;Tuomas Happonen,&nbsp;Henrik Sandberg and Jaakko Leppäniemi*,&nbsp;","doi":"10.1021/acsaelm.5c0023010.1021/acsaelm.5c00230","DOIUrl":"https://doi.org/10.1021/acsaelm.5c00230https://doi.org/10.1021/acsaelm.5c00230","url":null,"abstract":"<p >High-resolution reverse-offset printing (ROP) is developed for miniaturization of printed electronics, resulting in a notable decrease in material usage compared to conventional printing processes. Two alternative ROP processes for patterning of metal conductors are available that are comparable in their cost per sample: direct nanoparticle (NP) printing (e.g., Ag and Cu) and patterning of vacuum-deposited metal (Ag, Al, Au, Cu, Ti, etc.) films using ROP printed polymer resist ink and the lift-off (LO) process. In this work, we focus on ROP of Cu NP ink followed by intense pulsed light (IPL) sintering and vacuum-deposited Cu patterned by ROP lift-off (LO). The good large-scale uniformity of the two processes is demonstrated by a grid of 300 individual thickness, sheet resistance, and resistivity measurement points with low variation over the 10 cm × 10 cm printed sample area. Sheet resistances of 0.56 ± 0.03 and 1.23 ± 0.05 Ω/□ are obtained at 113 and 40 nm thickness for Cu NP and Cu LO, respectively. Both processes show &lt;5% thickness variation over a large area. A line-space (L/S) resolution of 2 μm is obtained for ROP patterned vacuum-deposited Cu having very low line edge roughness (LER) (∼60 nm), whereas for direct ROP printed Cu NP ink, the L/S resolution (2–4 μm) is limited by LER (∼900 nm) and influenced by the printed layer thickness. Based on the two fabrication routes, a flexible chip component assembly process is presented. Preliminary bending resistance results indicate that both ROP-based patterning processes yield a robust electrical interconnection between the ultrathin polyimide (PI) 5 mm × 5 mm chip and thermoplastic polyurethane (TPU). ROP shows promise as a scalable and sustainable patterning method for flexible ICs/chips that are assembled on flexible, stretchable, or biodegradable substrates and used, e.g., in wearable, large-scale sensing, and in environmental monitoring.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"7 8","pages":"3511–3520 3511–3520"},"PeriodicalIF":4.3,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsaelm.5c00230","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143854344","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}
引用次数: 0
Millimeter-Sized Single-Crystalline Anatase Nb-Doped TiO2 Membranes Exhibiting High Electrical Conduction and Transparency 毫米级单晶掺杂铌的氧化钛膜具有高导电性和透明度
IF 4.3 3区 材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC Pub Date : 2025-04-02 DOI: 10.1021/acsaelm.4c0234210.1021/acsaelm.4c02342
Yuzuki Uchida, Jiyang Huang, Masamichi Negishi, Seung Sae Hong and Tomoteru Fukumura*, 

Nb-doped TiO2 (TNO) is a transparent conducting electrode, contributing to transparent electronics and bioelectronics. Using a TNO membrane, we can fabricate transparent, flexible, and removable electrode patches and wires. However, highly conducting TNO membranes cannot be easily fabricated because of crack formation originating due to the large lattice mismatch between the sacrificial layer and TNO. Herein, La0.7Sr0.3MnO3 was used as a sacrificial layer to reduce the lattice mismatch with TNO, and TNO epitaxial thin films were grown on a SrTiO3 single-crystal substrate using the sacrificial layer. Although La0.7Sr0.3MnO3 was insoluble in water but soluble in acid, fewer cracks were formed in the millimeter-sized TNO membrane because of the chemical resistance of TNO to most acids and bases. Consequently, the TNO membrane exhibited high crystallinity and electrical conductivity, similar to those of TNO epitaxial thin films.

{"title":"Millimeter-Sized Single-Crystalline Anatase Nb-Doped TiO2 Membranes Exhibiting High Electrical Conduction and Transparency","authors":"Yuzuki Uchida,&nbsp;Jiyang Huang,&nbsp;Masamichi Negishi,&nbsp;Seung Sae Hong and Tomoteru Fukumura*,&nbsp;","doi":"10.1021/acsaelm.4c0234210.1021/acsaelm.4c02342","DOIUrl":"https://doi.org/10.1021/acsaelm.4c02342https://doi.org/10.1021/acsaelm.4c02342","url":null,"abstract":"<p >Nb-doped TiO<sub>2</sub> (TNO) is a transparent conducting electrode, contributing to transparent electronics and bioelectronics. Using a TNO membrane, we can fabricate transparent, flexible, and removable electrode patches and wires. However, highly conducting TNO membranes cannot be easily fabricated because of crack formation originating due to the large lattice mismatch between the sacrificial layer and TNO. Herein, La<sub>0.7</sub>Sr<sub>0.3</sub>MnO<sub>3</sub> was used as a sacrificial layer to reduce the lattice mismatch with TNO, and TNO epitaxial thin films were grown on a SrTiO<sub>3</sub> single-crystal substrate using the sacrificial layer. Although La<sub>0.7</sub>Sr<sub>0.3</sub>MnO<sub>3</sub> was insoluble in water but soluble in acid, fewer cracks were formed in the millimeter-sized TNO membrane because of the chemical resistance of TNO to most acids and bases. Consequently, the TNO membrane exhibited high crystallinity and electrical conductivity, similar to those of TNO epitaxial thin films.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"7 8","pages":"3308–3313 3308–3313"},"PeriodicalIF":4.3,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsaelm.4c02342","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853925","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}
引用次数: 0
A Haptic Glove with Flexible Piezoresistive Sensors Made by Graphene and Polyurethane Sponge for Object Recognition Based on Machine Learning Methods
IF 4.3 3区 材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC Pub Date : 2025-04-02 DOI: 10.1021/acsaelm.5c0016510.1021/acsaelm.5c00165
Yang Song, Tongjie Liu, Anyang Hu, Feilu Wang*, Hao Wang, Lang Wu and Renting Hu, 

The rapid advancement of artificial intelligence technology has propelled flexible tactile sensors into a wide range of application prospects across multiple domains. Flexible tactile sensors can convert the active dynamic tactile sensing signals into digital signals, which provide real-time insight and prediction capabilities by using machine learning methods to analyze the digital signals. This paper reports a low-cost and efficient strategy to fabricate flexible piezoresistive sensors with porous sponge structures. The prepared flexible piezoresistive sensors based on polyurethane (PU) sponge and graphene exhibit excellent properties such as excellent sensitivity (1.7356 kPa–1 at 0–55 kPa pressure), fast response/recovery time (147 ms/59 ms), small hysteresis error (6.51%), and stable repeatability (under 2000 cyclic pressure tests). The sensor is well suited for wearable devices due to its sensitivity over a wide range and its fast, cost-effective design process. Therefore, a haptic glove is designed with the flexible piezoresistive sensors for object recognition. By wearing the haptic glove, 1500 sets of time series signals during the grasp process for 15 different objects are detected and collected precisely. Then, the Residual Network (ResNet) with great feature extraction and generalization ability is constructed to recognize the 15 objects by the tactile time serial signals detected from the haptic glove, and the corresponding recognition accuracy is 95.67%. This work combines flexible tactile sensors with machine learning methods, providing an effective approach for flexible tactile sensors in more innovative applications.

人工智能技术的飞速发展推动柔性触觉传感器在多个领域获得了广泛的应用前景。柔性触觉传感器可将有源动态触觉传感信号转换为数字信号,通过使用机器学习方法分析数字信号,提供实时洞察和预测能力。本文介绍了一种利用多孔海绵结构制造柔性压阻传感器的低成本高效策略。所制备的基于聚氨酯(PU)海绵和石墨烯的柔性压阻传感器具有优异的性能,例如灵敏度高(0-55 kPa 压力下为 1.7356 kPa-1)、响应/恢复时间快(147 ms/59 ms)、滞后误差小(6.51%)以及重复性稳定(可进行 2000 次循环压力测试)。由于该传感器的灵敏度范围广,设计过程快速、成本效益高,因此非常适合用于可穿戴设备。因此,利用柔性压阻传感器设计了一种用于物体识别的触觉手套。通过佩戴触觉手套,1500 组时间序列信号在 15 个不同物体的抓取过程中被精确检测和收集。然后,通过触觉手套检测到的触觉时间序列信号,构建了具有强大特征提取和泛化能力的残差网络(ResNet)来识别这 15 个物体,相应的识别准确率达到 95.67%。这项工作将柔性触觉传感器与机器学习方法相结合,为柔性触觉传感器在更多创新应用中提供了一种有效方法。
{"title":"A Haptic Glove with Flexible Piezoresistive Sensors Made by Graphene and Polyurethane Sponge for Object Recognition Based on Machine Learning Methods","authors":"Yang Song,&nbsp;Tongjie Liu,&nbsp;Anyang Hu,&nbsp;Feilu Wang*,&nbsp;Hao Wang,&nbsp;Lang Wu and Renting Hu,&nbsp;","doi":"10.1021/acsaelm.5c0016510.1021/acsaelm.5c00165","DOIUrl":"https://doi.org/10.1021/acsaelm.5c00165https://doi.org/10.1021/acsaelm.5c00165","url":null,"abstract":"<p >The rapid advancement of artificial intelligence technology has propelled flexible tactile sensors into a wide range of application prospects across multiple domains. Flexible tactile sensors can convert the active dynamic tactile sensing signals into digital signals, which provide real-time insight and prediction capabilities by using machine learning methods to analyze the digital signals. This paper reports a low-cost and efficient strategy to fabricate flexible piezoresistive sensors with porous sponge structures. The prepared flexible piezoresistive sensors based on polyurethane (PU) sponge and graphene exhibit excellent properties such as excellent sensitivity (1.7356 kPa<sup>–1</sup> at 0–55 kPa pressure), fast response/recovery time (147 ms/59 ms), small hysteresis error (6.51%), and stable repeatability (under 2000 cyclic pressure tests). The sensor is well suited for wearable devices due to its sensitivity over a wide range and its fast, cost-effective design process. Therefore, a haptic glove is designed with the flexible piezoresistive sensors for object recognition. By wearing the haptic glove, 1500 sets of time series signals during the grasp process for 15 different objects are detected and collected precisely. Then, the Residual Network (ResNet) with great feature extraction and generalization ability is constructed to recognize the 15 objects by the tactile time serial signals detected from the haptic glove, and the corresponding recognition accuracy is 95.67%. This work combines flexible tactile sensors with machine learning methods, providing an effective approach for flexible tactile sensors in more innovative applications.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"7 8","pages":"3448–3460 3448–3460"},"PeriodicalIF":4.3,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853917","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}
引用次数: 0
Spirulina-Based Self-Powered Biological UV Photodetectors 基于螺旋藻的自供电生物紫外线光电探测器
IF 4.3 3区 材料科学 Q1 ENGINEERING, ELECTRICAL & ELECTRONIC Pub Date : 2025-04-01 DOI: 10.1021/acsaelm.4c0229510.1021/acsaelm.4c02295
Anamika Chatterjee, Akshai Shyam, Thirugnasambandam G Manivasagam* and Sudip K. Batabyal*, 

Overexposure to ultraviolet (UV) radiation can be monitored by a portable UV photodetector that provides reminders to humans. However, the traditional UV photodetector falls short of practical demands due to the power supply problem, impeding further development. This study describes an exceptionally sensitive self-powered biological ultraviolet photodetector leveraging a photosynthetic organism sandwiched between two electrodes. By the introduction of a cyanobacteria Spirulina sp. as a photoactive material, the device achieves exceptional sensitivity and stability in UV light detection under self-powered operation. Notably, upon illumination with 372 nm at zero bias, the device demonstrates impressive responsivity and detectivity values of 65 mA/W and 9 × 1010 Jones for the intensity of 0.4 mW/cm2, respectively. Additionally, the optimized device showed rapid rise and decay times, clocking in approximately 0.078 and 0.20 s, respectively, even at low intensity. There are many inorganic self-powered UV photodetectors widely used, but biological materials are underexplored. Now, here, we fabricated the device with nontoxic, renewable live cyanobacterial cells to mitigate environmental harm. In summary, the self-powered Spirulina-based UV photodetector demonstrates exceptional sensitivity, stability, and quick response and recovery times, making it a promising and environmentally friendly solution to the current challenges in UV detection applications.

过度暴露于紫外线(UV)辐射可通过便携式紫外线光电探测器进行监测,并向人类发出提醒。然而,传统的紫外线光电探测器由于供电问题无法满足实际需求,阻碍了进一步的发展。本研究介绍了一种异常灵敏的自供电生物紫外线光电探测器,它利用了夹在两个电极之间的光合生物。通过引入蓝藻螺旋藻作为光活性材料,该装置在自供电运行条件下实现了优异的紫外光检测灵敏度和稳定性。值得注意的是,在零偏压条件下,当紫外线波长为 372 纳米时,该器件的响应度和检测度分别达到了 65 mA/W 和 9 × 1010 Jones(强度为 0.4 mW/cm2)。此外,即使在低强度下,优化后的器件也能显示出快速的上升和衰减时间,分别约为 0.078 秒和 0.20 秒。目前有许多无机自供电紫外光检测器被广泛使用,但生物材料的应用还很欠缺。现在,我们利用无毒、可再生的蓝藻活细胞制造了这种装置,以减轻对环境的危害。总之,基于螺旋藻的自供电紫外光检测器表现出卓越的灵敏度、稳定性、快速响应和恢复时间,使其成为应对当前紫外检测应用挑战的一种前景广阔的环保型解决方案。
{"title":"Spirulina-Based Self-Powered Biological UV Photodetectors","authors":"Anamika Chatterjee,&nbsp;Akshai Shyam,&nbsp;Thirugnasambandam G Manivasagam* and Sudip K. Batabyal*,&nbsp;","doi":"10.1021/acsaelm.4c0229510.1021/acsaelm.4c02295","DOIUrl":"https://doi.org/10.1021/acsaelm.4c02295https://doi.org/10.1021/acsaelm.4c02295","url":null,"abstract":"<p >Overexposure to ultraviolet (UV) radiation can be monitored by a portable UV photodetector that provides reminders to humans. However, the traditional UV photodetector falls short of practical demands due to the power supply problem, impeding further development. This study describes an exceptionally sensitive self-powered biological ultraviolet photodetector leveraging a photosynthetic organism sandwiched between two electrodes. By the introduction of a cyanobacteria Spirulina sp. as a photoactive material, the device achieves exceptional sensitivity and stability in UV light detection under self-powered operation. Notably, upon illumination with 372 nm at zero bias, the device demonstrates impressive responsivity and detectivity values of 65 mA/W and 9 × 10<sup>10</sup> Jones for the intensity of 0.4 mW/cm<sup>2</sup>, respectively. Additionally, the optimized device showed rapid rise and decay times, clocking in approximately 0.078 and 0.20 s, respectively, even at low intensity. There are many inorganic self-powered UV photodetectors widely used, but biological materials are underexplored. Now, here, we fabricated the device with nontoxic, renewable live cyanobacterial cells to mitigate environmental harm. In summary, the self-powered <i>Spirulina</i>-based UV photodetector demonstrates exceptional sensitivity, stability, and quick response and recovery times, making it a promising and environmentally friendly solution to the current challenges in UV detection applications.</p>","PeriodicalId":3,"journal":{"name":"ACS Applied Electronic Materials","volume":"7 8","pages":"3274–3284 3274–3284"},"PeriodicalIF":4.3,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853900","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}
引用次数: 0
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