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Butylammonium-Based Chiral 2D Perovskite Single Crystals for Efficient UV Circularly Polarized Light Differentiation and High-Performance X-ray Detection
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-06 DOI: 10.1021/acsami.5c01035
Qi Gu, Kefan Chen, Xiong Zhang, Shuaihua Wang, Shaofan Wu, Wanxia Huang
Chiral two-dimensional perovskites are a promising candidate for circularly polarized light (CPL) detection, which combine inherent chirality with excellent optoelectronic properties, while exhibiting good structural stability. In this paper, a pair of chiral two-dimensional perovskites, single-crystal R/S-(BrBA)2PbBr4 are synthesized using a cooling crystallization solution method. Due to the introduction of chiral organic molecules, the inorganic layers undergo significant distortion and deformation. The large optical bandgap of the materials and the vertically oriented electrode structure of the detector result in an extremely low dark current, combined with circular dichroism (CD) spectroscopy and a photocurrent anisotropy factor of 0.14 at 405 nm, and demonstrate the good potential of the materials for detecting circularly polarized light in the ultraviolet band. In addition, the unique semiconductor properties enable it to have a detection sensitivity of 531.33 μC Gy–1 cm–2 (at 0.15 V/μm) and a detection limit of less than 100 nGy s–1 in X-ray detection, which is far lower than that of requirements in conventional medical diagnosis (5.5 μGy s–1). The final imaging experiments have also verified its feasibility for application in X-ray imaging.
{"title":"Butylammonium-Based Chiral 2D Perovskite Single Crystals for Efficient UV Circularly Polarized Light Differentiation and High-Performance X-ray Detection","authors":"Qi Gu, Kefan Chen, Xiong Zhang, Shuaihua Wang, Shaofan Wu, Wanxia Huang","doi":"10.1021/acsami.5c01035","DOIUrl":"https://doi.org/10.1021/acsami.5c01035","url":null,"abstract":"Chiral two-dimensional perovskites are a promising candidate for circularly polarized light (CPL) detection, which combine inherent chirality with excellent optoelectronic properties, while exhibiting good structural stability. In this paper, a pair of chiral two-dimensional perovskites, single-crystal R/S-(BrBA)<sub>2</sub>PbBr<sub>4</sub> are synthesized using a cooling crystallization solution method. Due to the introduction of chiral organic molecules, the inorganic layers undergo significant distortion and deformation. The large optical bandgap of the materials and the vertically oriented electrode structure of the detector result in an extremely low dark current, combined with circular dichroism (CD) spectroscopy and a photocurrent anisotropy factor of 0.14 at 405 nm, and demonstrate the good potential of the materials for detecting circularly polarized light in the ultraviolet band. In addition, the unique semiconductor properties enable it to have a detection sensitivity of 531.33 μC Gy<sup>–1</sup> cm<sup>–2</sup> (at 0.15 V/μm) and a detection limit of less than 100 nGy s<sup>–1</sup> in X-ray detection, which is far lower than that of requirements in conventional medical diagnosis (5.5 μGy s<sup>–1</sup>). The final imaging experiments have also verified its feasibility for application in X-ray imaging.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"53 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143561325","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Tailoring Presynthesized Amorphous Sb2S3 Particles Enables High-Efficiency Pure Antimony Sulfide Solar Cells.
IF 8.3 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-06 DOI: 10.1021/acsami.4c17684
Xiaolei Li, Yuanjie Yang, Liangliang Feng, Yuanhui Yang, Kai Hu, Hongling Guo, Gang Wang, Yi Zhang

At present, hydrothermal deposition techniques are unique to attain high-efficiency antimony sulfide (Sb2S3) solar cells. It is very common that during the mixing of antimony and sulfur sources before the hydrothermal reaction, the solution quickly changes from colorless to yellow due to the formation of amorphous Sb2S3 particles. However, the effect of presynthesized Sb2S3 particles on the deposition kinetics of Sb2S3 absorber layers and the device performance is completely unknown. To pave the pathway toward high-efficiency Sb2S3 solar cells, it is urgent to disclose the mechanism behind such a phenomenon. By accurately controlling the number and size of presynthesized Sb2S3 particles in the hydrothermal precursor solution, it was found that the suspended Sb2S3 particles act as growth centers, facilitating the orderly deposition of the Sb2S3 film on the substrate, which in turn affects the film's thickness, grain size, densification, and crystallinity. Based on this finding, the Sb2S3 solar cell with an efficiency of 7.29% is achieved, which is currently one of the highest fundamental efficiency obtained for Sb2S3 prepared by hydrothermal methods without doping. This study lays the groundwork for investigating the growth mechanism of Sb2S3 produced by hydrothermal deposition techniques and provides guidelines for the preparation of high-efficiency Sb2S3 solar cells.

{"title":"Tailoring Presynthesized Amorphous Sb<sub>2</sub>S<sub>3</sub> Particles Enables High-Efficiency Pure Antimony Sulfide Solar Cells.","authors":"Xiaolei Li, Yuanjie Yang, Liangliang Feng, Yuanhui Yang, Kai Hu, Hongling Guo, Gang Wang, Yi Zhang","doi":"10.1021/acsami.4c17684","DOIUrl":"https://doi.org/10.1021/acsami.4c17684","url":null,"abstract":"<p><p>At present, hydrothermal deposition techniques are unique to attain high-efficiency antimony sulfide (Sb<sub>2</sub>S<sub>3</sub>) solar cells. It is very common that during the mixing of antimony and sulfur sources before the hydrothermal reaction, the solution quickly changes from colorless to yellow due to the formation of amorphous Sb<sub>2</sub>S<sub>3</sub> particles. However, the effect of presynthesized Sb<sub>2</sub>S<sub>3</sub> particles on the deposition kinetics of Sb<sub>2</sub>S<sub>3</sub> absorber layers and the device performance is completely unknown. To pave the pathway toward high-efficiency Sb<sub>2</sub>S<sub>3</sub> solar cells, it is urgent to disclose the mechanism behind such a phenomenon. By accurately controlling the number and size of presynthesized Sb<sub>2</sub>S<sub>3</sub> particles in the hydrothermal precursor solution, it was found that the suspended Sb<sub>2</sub>S<sub>3</sub> particles act as growth centers, facilitating the orderly deposition of the Sb<sub>2</sub>S<sub>3</sub> film on the substrate, which in turn affects the film's thickness, grain size, densification, and crystallinity. Based on this finding, the Sb<sub>2</sub>S<sub>3</sub> solar cell with an efficiency of 7.29% is achieved, which is currently one of the highest fundamental efficiency obtained for Sb<sub>2</sub>S<sub>3</sub> prepared by hydrothermal methods without doping. This study lays the groundwork for investigating the growth mechanism of Sb<sub>2</sub>S<sub>3</sub> produced by hydrothermal deposition techniques and provides guidelines for the preparation of high-efficiency Sb<sub>2</sub>S<sub>3</sub> solar cells.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.3,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143571538","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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-Terminal Ion-Modulation Multiplier-Based Ion-Doped Stacked Semiconducting Nanosheets for Multifunctional Biomedical Applications.
IF 8.3 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-06 DOI: 10.1021/acsami.4c18930
Jiehua Zhang, Baobao Xu, Yiyi Yang, Zhixin Xie, Haihua Xu

Stacked semiconducting nanosheets (SSNs), which feature strong in-plane covalent bonds but weak van der Waals (vdWs) interactions between adjacent layers, hold substantial promise in next-generation, printable, and flexible devices. Among them, SSN-based transistors with high current multiplication offer significant potential for large-area, high-integration electronics and biomedical applications. However, the three-terminal configuration of the transistor inevitably increases the process step and power unit. Here, we demonstrate a dual-terminal ion modulation multiplier (IMM) based on ion-doped SSNs, which was obtained through a solution-processed and cost-effective method. We observed an ion-induced self-multiplication effect occurring in the IMM, which significantly enhanced the sensing performance, particularly in thermal sensing. The IMM thermal sensor exhibited a high resolution of 0.02 K and ultrahigh sensitivity of ∼27%/K, more than 7 times higher than that of ion-type thermal sensors. By combining the enhanced operational stability of IMMs, we successfully developed a dual-channel stretchable respiratory sensor (dSRS) based on IMMs, capable of real-time monitoring of subnasal respiratory signals. The dSRS effectively distinguished normal, rapid, and deep breathing states while accurately detecting abnormal respiration, including apnea and hypopnea. Utilizing the unique properties of IMMs, we developed a monolithically integrated and high-performance IMM glucose sensor with temperature compensation. This IMM glucose sensor demonstrated a high sensitivity of 0.91%/μM, a low detection limit of 100 nM, and a high detection accuracy under temperature interference. Our results clearly demonstrate that IMM devices endow SSNs with promising electrical and sensing capabilities, paving the way for next-generation electronics in the post-Moore era.

{"title":"Dual-Terminal Ion-Modulation Multiplier-Based Ion-Doped Stacked Semiconducting Nanosheets for Multifunctional Biomedical Applications.","authors":"Jiehua Zhang, Baobao Xu, Yiyi Yang, Zhixin Xie, Haihua Xu","doi":"10.1021/acsami.4c18930","DOIUrl":"https://doi.org/10.1021/acsami.4c18930","url":null,"abstract":"<p><p>Stacked semiconducting nanosheets (SSNs), which feature strong in-plane covalent bonds but weak van der Waals (vdWs) interactions between adjacent layers, hold substantial promise in next-generation, printable, and flexible devices. Among them, SSN-based transistors with high current multiplication offer significant potential for large-area, high-integration electronics and biomedical applications. However, the three-terminal configuration of the transistor inevitably increases the process step and power unit. Here, we demonstrate a dual-terminal ion modulation multiplier (IMM) based on ion-doped SSNs, which was obtained through a solution-processed and cost-effective method. We observed an ion-induced self-multiplication effect occurring in the IMM, which significantly enhanced the sensing performance, particularly in thermal sensing. The IMM thermal sensor exhibited a high resolution of 0.02 K and ultrahigh sensitivity of ∼27%/K, more than 7 times higher than that of ion-type thermal sensors. By combining the enhanced operational stability of IMMs, we successfully developed a dual-channel stretchable respiratory sensor (dSRS) based on IMMs, capable of real-time monitoring of subnasal respiratory signals. The dSRS effectively distinguished normal, rapid, and deep breathing states while accurately detecting abnormal respiration, including apnea and hypopnea. Utilizing the unique properties of IMMs, we developed a monolithically integrated and high-performance IMM glucose sensor with temperature compensation. This IMM glucose sensor demonstrated a high sensitivity of 0.91%/μM, a low detection limit of 100 nM, and a high detection accuracy under temperature interference. Our results clearly demonstrate that IMM devices endow SSNs with promising electrical and sensing capabilities, paving the way for next-generation electronics in the post-Moore era.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.3,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143565527","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Schizophrenia Treatment Based on Sustained Release of Risperidone from Poly(lactic-co-glycolic) Acid Implantable Microarray Patch.
IF 8.3 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-06 DOI: 10.1021/acsami.4c20010
Linlin Li, Li Zhao, Mingshan Li, Yushi Tao, Akmal Hidayat Bin Sabri, Natalia Moreno-Castellanos, Rand Ghanma, Brett Greer, Qonita Kurnia Anjani, Helen O McCarthy, Ryan F Donnelly, Eneko Larrañeta

Schizophrenia is one of the most severe mental disorders, affecting approximately 24 million people worldwide. Conventional treatments, such as drug-loaded implants and intramuscular injections, have several limitations, including pain during administration and the need for medical professionals to perform the procedure. In this study, a poly(lactic-co-glycolic) acid (PLGA)-based implantable microneedle patch (IMN) was developed for the transdermal delivery of risperidone (RIS) as a treatment for schizophrenia. RIS IMNs were prepared by sequentially casting gel-based formulations into microneedle (MN) molds. The patches were then characterized using microscopy, differential scanning calorimetry, and infrared spectroscopy, as well as through evaluations of MN insertion and RIS release. A selected formulation was further tested by evaluating its cytocompatibility and its ability to deliver RIS in a rat animal model. The RIS IMN demonstrated excellent mechanical properties, successfully inserting up to 378 nm into model skin, which is crucial for effective transdermal drug delivery. A biocompatibility study using human dermal fibroblasts showed no cytotoxicity, with cell viability and proliferation being close to 100%. The optimized formulation achieved a sustained in vitro release over 7 days, while ex vivo skin deposition and permeation studies showed over 65% RIS delivery efficiency. In vivo animal studies confirmed that RIS IMNs maintained therapeutic plasma concentrations throughout the nine-day experiment, with Cmax values of RIS and 9-OH RIS reaching 387.96 ± 194.02 and 139.89 ± 47.68 ng/mL at 6 and 96 h, respectively. In contrast, intramuscular injection showed a Cmax of 1756.70 ± 246.06 and 1377.38 ± 160.78 ng/mL at 2 and 6 h but lost therapeutic effect after just 24 h. These findings suggest that RIS IMNs offer significant clinical benefits for patients with schizophrenia, providing prolonged therapeutic effects with a simple, self-administering drug delivery system, reducing the need for frequent medical interventions.

{"title":"Schizophrenia Treatment Based on Sustained Release of Risperidone from Poly(lactic-<i>co</i>-glycolic) Acid Implantable Microarray Patch.","authors":"Linlin Li, Li Zhao, Mingshan Li, Yushi Tao, Akmal Hidayat Bin Sabri, Natalia Moreno-Castellanos, Rand Ghanma, Brett Greer, Qonita Kurnia Anjani, Helen O McCarthy, Ryan F Donnelly, Eneko Larrañeta","doi":"10.1021/acsami.4c20010","DOIUrl":"https://doi.org/10.1021/acsami.4c20010","url":null,"abstract":"<p><p>Schizophrenia is one of the most severe mental disorders, affecting approximately 24 million people worldwide. Conventional treatments, such as drug-loaded implants and intramuscular injections, have several limitations, including pain during administration and the need for medical professionals to perform the procedure. In this study, a poly(lactic-<i>co</i>-glycolic) acid (PLGA)-based implantable microneedle patch (IMN) was developed for the transdermal delivery of risperidone (RIS) as a treatment for schizophrenia. RIS IMNs were prepared by sequentially casting gel-based formulations into microneedle (MN) molds. The patches were then characterized using microscopy, differential scanning calorimetry, and infrared spectroscopy, as well as through evaluations of MN insertion and RIS release. A selected formulation was further tested by evaluating its cytocompatibility and its ability to deliver RIS in a rat animal model. The RIS IMN demonstrated excellent mechanical properties, successfully inserting up to 378 nm into model skin, which is crucial for effective transdermal drug delivery. A biocompatibility study using human dermal fibroblasts showed no cytotoxicity, with cell viability and proliferation being close to 100%. The optimized formulation achieved a sustained <i>in vitro</i> release over 7 days, while <i>ex vivo</i> skin deposition and permeation studies showed over 65% RIS delivery efficiency. <i>In vivo</i> animal studies confirmed that RIS IMNs maintained therapeutic plasma concentrations throughout the nine-day experiment, with <i>C</i><sub>max</sub> values of RIS and 9-OH RIS reaching 387.96 ± 194.02 and 139.89 ± 47.68 ng/mL at 6 and 96 h, respectively. In contrast, intramuscular injection showed a <i>C</i><sub>max</sub> of 1756.70 ± 246.06 and 1377.38 ± 160.78 ng/mL at 2 and 6 h but lost therapeutic effect after just 24 h. These findings suggest that RIS IMNs offer significant clinical benefits for patients with schizophrenia, providing prolonged therapeutic effects with a simple, self-administering drug delivery system, reducing the need for frequent medical interventions.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.3,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143571535","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Hot Electron Photoemission from Tunable Electron Affinity Semiconductor Cathodes
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-06 DOI: 10.1021/acsami.4c18187
Ragib Ahsan, Anika Tabassum Priyoti, Jun Meng, Ryan Jacobs, John Booske, Rehan Kapadia
A voltage-tunable negative electron affinity (NEA) semiconductor photocathode offers one key advantage over current materials such as cesiated NEA photocathodes: stability under ambient conditions. A semiconductor/insulator/graphene heterostructure can inject electrons into the conduction band of the insulator, where an electric field “heats” them up so that the effective emission barrier seen by the “hot” electrons is negative, enabling a voltage-tunable NEA surface. Here, we have experimentally demonstrated a peak emission current density of 2.253 × 10–3 A/cm2 and a peak external quantum efficiency (EQE) of ∼1.53% from a p-Si/amorphous-Al2O3/graphene-based hot electron laser-assisted cathode (HELAC). We have developed a full-band Monte Carlo Boltzmann Transport Equation (MCBTE) solver to study the hot electron transport behavior in three different crystalline insulators: SiO2, Al2O3, and MgO. Through MCBTE and semiconductor device simulations, we have predicted a peak emission current density of ∼103 A/cm2, far above our experimental value, indicating that the optimal performance of state-of-the-art HELACs has not yet been realized. This theoretical framework provides an understanding of the key performance limitations of the device and can be used to guide the optimal design (e.g., through the selection of new materials) of voltage-tunable NEA semiconductor photocathodes.
{"title":"Hot Electron Photoemission from Tunable Electron Affinity Semiconductor Cathodes","authors":"Ragib Ahsan, Anika Tabassum Priyoti, Jun Meng, Ryan Jacobs, John Booske, Rehan Kapadia","doi":"10.1021/acsami.4c18187","DOIUrl":"https://doi.org/10.1021/acsami.4c18187","url":null,"abstract":"A voltage-tunable negative electron affinity (NEA) semiconductor photocathode offers one key advantage over current materials such as cesiated NEA photocathodes: stability under ambient conditions. A semiconductor/insulator/graphene heterostructure can inject electrons into the conduction band of the insulator, where an electric field “heats” them up so that the effective emission barrier seen by the “hot” electrons is negative, enabling a voltage-tunable NEA surface. Here, we have experimentally demonstrated a peak emission current density of 2.253 × 10<sup>–3</sup> A/cm<sup>2</sup> and a peak external quantum efficiency (EQE) of ∼1.53% from a p-Si/amorphous-Al<sub>2</sub>O<sub>3</sub>/graphene-based hot electron laser-assisted cathode (HELAC). We have developed a full-band Monte Carlo Boltzmann Transport Equation (MCBTE) solver to study the hot electron transport behavior in three different crystalline insulators: SiO<sub>2</sub>, Al<sub>2</sub>O<sub>3</sub>, and MgO. Through MCBTE and semiconductor device simulations, we have predicted a peak emission current density of ∼10<sup>3</sup> A/cm<sup>2</sup>, far above our experimental value, indicating that the optimal performance of state-of-the-art HELACs has not yet been realized. This theoretical framework provides an understanding of the key performance limitations of the device and can be used to guide the optimal design (e.g., through the selection of new materials) of voltage-tunable NEA semiconductor photocathodes.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"16 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143561319","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Metal-Like Conductivity in Acid-Treated PEDOT:PSS Films: Surpassing 15,000 S/Cm.
IF 8.3 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-06 DOI: 10.1021/acsami.4c19958
Xinyuan Qian, Jiahuan Qiu, Bin Hu, Junxian Yao, Min Zuo, Ziliang Wu, Guorong Shan, Yihu Song, Qiang Zheng, Boyu Peng, Hanying Li, Miao Du

Although poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) films with high conductivity have been obtained through conventional organic solvent and acid treatment, their conductivity has not yet exceeded 10000 S/cm. In this paper, by combining blade-coating and treating with high concentration and volatilizable trifluoromethanesulfonic acid (CF3SO3H), PEDOT:PSS films with ultrahigh conductivity of 15143 S/cm, comparable to some metals, were prepared. Characterizations of morphology and structure indicate the formation of a perfectly continuous fibrous network structure, highly oriented crystallization, and tightly packed π-π stacking of PEDOT chains after removing a vast amount of PSS, which contributes to boosting the electrical conductivity of the treated PEDOT:PSS film. The distinguished electrical properties and ultrahigh conductivity enable it to replace metal materials as electrodes for "all-polymer" capacitive piezoelectric sensors with outstanding pressure sensitivity. Moreover, by regulating the blade-coating condition, the CF3SO3H-treated PEDOT:PSS films exhibit excellent electrochemical performance, which is an ideal channel material in organic electrochemical transistors (OECTs). The CF3SO3H-treated PEDOT:PSS film-based OECT devices display a high transconductance of 50.6 ± 5.5 mS and carrier mobility of 9.3 ± 1.5 cm2V-1s-1. This study not only provides new insights into the development of a simple and efficient PEDOT:PSS film treatment method but also expands its application in flexible electronics. Especially, the present research offers a useful reference in preparing "all-polymer"-based flexible electronic devices.

{"title":"Metal-Like Conductivity in Acid-Treated PEDOT:PSS Films: Surpassing 15,000 S/Cm.","authors":"Xinyuan Qian, Jiahuan Qiu, Bin Hu, Junxian Yao, Min Zuo, Ziliang Wu, Guorong Shan, Yihu Song, Qiang Zheng, Boyu Peng, Hanying Li, Miao Du","doi":"10.1021/acsami.4c19958","DOIUrl":"https://doi.org/10.1021/acsami.4c19958","url":null,"abstract":"<p><p>Although poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) films with high conductivity have been obtained through conventional organic solvent and acid treatment, their conductivity has not yet exceeded 10000 S/cm. In this paper, by combining blade-coating and treating with high concentration and volatilizable trifluoromethanesulfonic acid (CF<sub>3</sub>SO<sub>3</sub>H), PEDOT:PSS films with ultrahigh conductivity of 15143 S/cm, comparable to some metals, were prepared. Characterizations of morphology and structure indicate the formation of a perfectly continuous fibrous network structure, highly oriented crystallization, and tightly packed π-π stacking of PEDOT chains after removing a vast amount of PSS, which contributes to boosting the electrical conductivity of the treated PEDOT:PSS film. The distinguished electrical properties and ultrahigh conductivity enable it to replace metal materials as electrodes for \"all-polymer\" capacitive piezoelectric sensors with outstanding pressure sensitivity. Moreover, by regulating the blade-coating condition, the CF<sub>3</sub>SO<sub>3</sub>H-treated PEDOT:PSS films exhibit excellent electrochemical performance, which is an ideal channel material in organic electrochemical transistors (OECTs). The CF<sub>3</sub>SO<sub>3</sub>H-treated PEDOT:PSS film-based OECT devices display a high transconductance of 50.6 ± 5.5 mS and carrier mobility of 9.3 ± 1.5 cm<sup>2</sup>V<sup>-1</sup>s<sup>-1</sup>. This study not only provides new insights into the development of a simple and efficient PEDOT:PSS film treatment method but also expands its application in flexible electronics. Especially, the present research offers a useful reference in preparing \"all-polymer\"-based flexible electronic devices.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.3,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143571529","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Fluoride Ion Passivation of CsPbBr3 Nanocrystals at Room Temperature for Highly Efficient and Stable White Light-Emitting Diodes
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-06 DOI: 10.1021/acsami.5c01999
Wenqiang Liu, Zitong Qi, Tuanning Liu, Yang Zhang
Inorganic halide perovskite nanocrystals (NCs) are regarded as promising emitters for light-emitting diodes due to their bright and narrow emission. However, surface defects often result in trap states and ion migration, which remains a huge challenge for high-quality perovskite NCs. Herein, fluoride ions are introduced into CsPbBr3 perovskite NCs at room temperature through the chelation of ligands. Experimental results demonstrate that these fluoride ions from inorganic salts can improve the average lifetime and crystallinity of CsPbBr3 NCs. Meanwhile, the resulting photoluminescence quantum yield is optimized up to 99.02%, and it has high stability to water, heat, and ultraviolet light. Density functional theory calculations show that fluoride ions have a higher binding energy compared to other ligands, which not only removes the electron trapping center but also increases the halogen ion migration energy. By mixing green-emission CsPbBr3 NCs and red-emission K2SiF6:Mn4+ phosphors on a blue chip, the fabricated white light emitting diode shows a high luminous efficiency of 147.8 lm/W, a wide color gamut (129% for NTSC), and CIE coordinates of (0.3160, 0.3051). Furthermore, the photoluminescence intensity decreased by only 2.9% after 48 h of continuous operation.
{"title":"Fluoride Ion Passivation of CsPbBr3 Nanocrystals at Room Temperature for Highly Efficient and Stable White Light-Emitting Diodes","authors":"Wenqiang Liu, Zitong Qi, Tuanning Liu, Yang Zhang","doi":"10.1021/acsami.5c01999","DOIUrl":"https://doi.org/10.1021/acsami.5c01999","url":null,"abstract":"Inorganic halide perovskite nanocrystals (NCs) are regarded as promising emitters for light-emitting diodes due to their bright and narrow emission. However, surface defects often result in trap states and ion migration, which remains a huge challenge for high-quality perovskite NCs. Herein, fluoride ions are introduced into CsPbBr<sub>3</sub> perovskite NCs at room temperature through the chelation of ligands. Experimental results demonstrate that these fluoride ions from inorganic salts can improve the average lifetime and crystallinity of CsPbBr<sub>3</sub> NCs. Meanwhile, the resulting photoluminescence quantum yield is optimized up to 99.02%, and it has high stability to water, heat, and ultraviolet light. Density functional theory calculations show that fluoride ions have a higher binding energy compared to other ligands, which not only removes the electron trapping center but also increases the halogen ion migration energy. By mixing green-emission CsPbBr<sub>3</sub> NCs and red-emission K<sub>2</sub>SiF<sub>6</sub>:Mn<sup>4+</sup> phosphors on a blue chip, the fabricated white light emitting diode shows a high luminous efficiency of 147.8 lm/W, a wide color gamut (129% for NTSC), and CIE coordinates of (0.3160, 0.3051). Furthermore, the photoluminescence intensity decreased by only 2.9% after 48 h of continuous operation.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"36 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143561322","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
High-Performance Energy Storage in Ba(Al0.5Nb0.5)O3-Modified (Bi0.5Na0.5)TiO3-Based Lead-Free Ceramics via High-Entropy Strategy.
IF 8.3 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-06 DOI: 10.1021/acsami.4c22588
Zhiqiang Zhang, Fan Zhang, Yiwen Niu, Meiyue Li, Jihang Liu, Zhan Jie Wang

Lead-free dielectric capacitors are widely utilized in high-power pulse devices due to their outstanding power density, rapid charging-discharging speed, and environmental friendliness. However, there are still challenges in further improving their energy storage performance. Recently, a high-entropy strategy has received widespread attention to obtain high-performance dielectric capacitors. In this work, Ba(Al0.5Nb0.5)O3 (BAN) was introduced into lead-free (Bi0.5Na0.5)TiO3-based ceramics to increase configuration entropy and chemical disorder, exploiting a synergistic high-entropy strategy to optimize the energy storage characteristics. Remarkably, superior energy storage density (Wrec ∼7.40 J/cm3) and efficiency (η ∼85.5%) at a great electric breakdown strength (Eb ∼547 kV/cm) are achieved in 0.85(0.6(Bi0.5Na0.5)TiO3-0.4(Sr0.7Bi0.2)TiO3)-0.15BAN high-entropy ceramic. The integration of BAN boosts the increase of entropy and induces grain refinement, strengthened relaxation behavior, formation of polar nanoregions, and a widened band gap, leading to reduced Pr and improved Eb as well as excellent energy storage performance. Moreover, good thermal stability, frequency stability, and charge-discharge performance are also realized. This study confirms that high-entropy engineering is a feasible route to realize high-performance energy storage, providing prospective lead-free dielectric materials for practical applications.

{"title":"High-Performance Energy Storage in Ba(Al<sub>0.5</sub>Nb<sub>0.5</sub>)O<sub>3</sub>-Modified (Bi<sub>0.5</sub>Na<sub>0.5</sub>)TiO<sub>3</sub>-Based Lead-Free Ceramics via High-Entropy Strategy.","authors":"Zhiqiang Zhang, Fan Zhang, Yiwen Niu, Meiyue Li, Jihang Liu, Zhan Jie Wang","doi":"10.1021/acsami.4c22588","DOIUrl":"https://doi.org/10.1021/acsami.4c22588","url":null,"abstract":"<p><p>Lead-free dielectric capacitors are widely utilized in high-power pulse devices due to their outstanding power density, rapid charging-discharging speed, and environmental friendliness. However, there are still challenges in further improving their energy storage performance. Recently, a high-entropy strategy has received widespread attention to obtain high-performance dielectric capacitors. In this work, Ba(Al<sub>0.5</sub>Nb<sub>0.5</sub>)O<sub>3</sub> (BAN) was introduced into lead-free (Bi<sub>0.5</sub>Na<sub>0.5</sub>)TiO<sub>3</sub>-based ceramics to increase configuration entropy and chemical disorder, exploiting a synergistic high-entropy strategy to optimize the energy storage characteristics. Remarkably, superior energy storage density (<i>W</i><sub>rec</sub> ∼7.40 J/cm<sup>3</sup>) and efficiency (η ∼85.5%) at a great electric breakdown strength (<i>E</i><sub>b</sub> ∼547 kV/cm) are achieved in 0.85(0.6(Bi<sub>0.5</sub>Na<sub>0.5</sub>)TiO<sub>3</sub>-0.4(Sr<sub>0.7</sub>Bi<sub>0.2</sub>)TiO<sub>3</sub>)-0.15BAN high-entropy ceramic. The integration of BAN boosts the increase of entropy and induces grain refinement, strengthened relaxation behavior, formation of polar nanoregions, and a widened band gap, leading to reduced <i>P</i><sub>r</sub> and improved <i>E</i><sub>b</sub> as well as excellent energy storage performance. Moreover, good thermal stability, frequency stability, and charge-discharge performance are also realized. This study confirms that high-entropy engineering is a feasible route to realize high-performance energy storage, providing prospective lead-free dielectric materials for practical applications.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.3,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143571526","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Suppressing Hydrogen Evolution and Dendrite Formation on a Zn Anode by Coating In2O3 with Tailored Affinity to H* and Zn.
IF 8.3 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-06 DOI: 10.1021/acsami.5c00853
Zeshen Deng, Wenbiao Zhang, Qingsheng Gao, Lichun Yang, Yuping Wu, Min Zhu

To suppress the hydrogen evolution reaction (HER) and dendrite formation on the Zn anode in aqueous Zn-ion batteries, a submicrometer In2O3 coating on the Zn anode (referred to as Zn@In2O3) was constructed via magnetron sputtering. Density functional theory (DFT) and experimental data show that the In2O3 coating suppresses the HER because of its weaker interactions with H* compared with Zn, inhibiting the Volmer step. At the same time, the In2O3 coating exhibits a moderate affinity for Zn*, higher than that on Zn but lower than that at the In2O3-Zn interface, thus facilitating the desolvation of the hydrated Zn2+ ions while promoting its deposition on the Zn substrate beneath the In2O3 coating. The resultant suppression of side reactions and dendrite growth significantly enhance the reversible plating/stripping of Zn. The optimized Zn@In2O3 stably cycles over 6400 h with a low voltage hysteresis of 9.5 mV at 1 mA cm-2 and 1 mAh cm-2 in symmetric cells. The average Coulombic efficiency of Zn plating/stripping is increased from 95.8 to 99.6% owing to the In2O3 coating. Moreover, when coupled with the Mn0.15V2O5·nH2O cathode, the Zn@In2O3 battery maintains a capacity retention of 78.6% after 2000 cycles at 5 A g-1. This facile and economical modification of Zn anodes provides an idea for realizing the practical application of AZIBs.

{"title":"Suppressing Hydrogen Evolution and Dendrite Formation on a Zn Anode by Coating In<sub>2</sub>O<sub>3</sub> with Tailored Affinity to H* and Zn.","authors":"Zeshen Deng, Wenbiao Zhang, Qingsheng Gao, Lichun Yang, Yuping Wu, Min Zhu","doi":"10.1021/acsami.5c00853","DOIUrl":"https://doi.org/10.1021/acsami.5c00853","url":null,"abstract":"<p><p>To suppress the hydrogen evolution reaction (HER) and dendrite formation on the Zn anode in aqueous Zn-ion batteries, a submicrometer In<sub>2</sub>O<sub>3</sub> coating on the Zn anode (referred to as Zn@In<sub>2</sub>O<sub>3</sub>) was constructed via magnetron sputtering. Density functional theory (DFT) and experimental data show that the In<sub>2</sub>O<sub>3</sub> coating suppresses the HER because of its weaker interactions with H* compared with Zn, inhibiting the Volmer step. At the same time, the In<sub>2</sub>O<sub>3</sub> coating exhibits a moderate affinity for Zn*, higher than that on Zn but lower than that at the In<sub>2</sub>O<sub>3</sub>-Zn interface, thus facilitating the desolvation of the hydrated Zn<sup>2+</sup> ions while promoting its deposition on the Zn substrate beneath the In<sub>2</sub>O<sub>3</sub> coating. The resultant suppression of side reactions and dendrite growth significantly enhance the reversible plating/stripping of Zn. The optimized Zn@In<sub>2</sub>O<sub>3</sub> stably cycles over 6400 h with a low voltage hysteresis of 9.5 mV at 1 mA cm<sup>-2</sup> and 1 mAh cm<sup>-2</sup> in symmetric cells. The average Coulombic efficiency of Zn plating/stripping is increased from 95.8 to 99.6% owing to the In<sub>2</sub>O<sub>3</sub> coating. Moreover, when coupled with the Mn<sub>0.15</sub>V<sub>2</sub>O<sub>5</sub>·nH<sub>2</sub>O cathode, the Zn@In<sub>2</sub>O<sub>3</sub> battery maintains a capacity retention of 78.6% after 2000 cycles at 5 A g<sup>-1</sup>. This facile and economical modification of Zn anodes provides an idea for realizing the practical application of AZIBs.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.3,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143571536","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Ta4C3 MXene Slows Progression of Fatty Liver Disease through Its Anti-Inflammatory and ROS-Scavenging Effects.
IF 8.3 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2025-03-06 DOI: 10.1021/acsami.4c20945
Shuying He, Yuerong Lv, Jingnan Qiu, Shudan Cui, Zixian Gao, Liang Peng

Treating metabolic dysfunction-associated fatty liver disease (MAFLD) and reducing the occurrence of MAFLD-associated liver cancer remain challenging. Two-dimensional (2D) tantalum carbide (Ta4C3) MXene nanozymes (MXenzymes) exhibit antioxidant and anti-inflammatory activities and have thus attracted considerable attention in the fields of oncology and engineering. However, the potential mechanism of action and bioactive properties of Ta4C3 in MAFLD remain uncertain. In our study, Ta4C3 not only inhibited lipid accumulation and disrupted lipid metabolism in hepatocytes but also reduced cell death caused by fatty acids by decreasing intracellular reactive oxygen species (ROS) levels, which significantly promoted the polarization of M1 macrophages to M2 macrophages by alleviating oxidative stress and further suppressing inflammatory factor expression. In mice fed a methionine-choline-deficient (MCD) diet, Ta4C3 reduced lipid accumulation, the infiltration of inflammatory cells, and liver cell apoptosis by modulating the cellular microenvironment through its anti-inflammatory and antioxidant properties. Therefore, Ta4C3 can be used as a multifunctional bioactive material to alleviate hepatic steatosis and inflammation in individuals with MAFLD/metabolic dysfunction-associated steatohepatitis (MASH) because of its robust antioxidant and anti-inflammatory effects.

{"title":"Ta<sub>4</sub>C<sub>3</sub> MXene Slows Progression of Fatty Liver Disease through Its Anti-Inflammatory and ROS-Scavenging Effects.","authors":"Shuying He, Yuerong Lv, Jingnan Qiu, Shudan Cui, Zixian Gao, Liang Peng","doi":"10.1021/acsami.4c20945","DOIUrl":"https://doi.org/10.1021/acsami.4c20945","url":null,"abstract":"<p><p>Treating metabolic dysfunction-associated fatty liver disease (MAFLD) and reducing the occurrence of MAFLD-associated liver cancer remain challenging. Two-dimensional (2D) tantalum carbide (Ta<sub>4</sub>C<sub>3</sub>) MXene nanozymes (MXenzymes) exhibit antioxidant and anti-inflammatory activities and have thus attracted considerable attention in the fields of oncology and engineering. However, the potential mechanism of action and bioactive properties of Ta<sub>4</sub>C<sub>3</sub> in MAFLD remain uncertain. In our study, Ta<sub>4</sub>C<sub>3</sub> not only inhibited lipid accumulation and disrupted lipid metabolism in hepatocytes but also reduced cell death caused by fatty acids by decreasing intracellular reactive oxygen species (ROS) levels, which significantly promoted the polarization of M1 macrophages to M2 macrophages by alleviating oxidative stress and further suppressing inflammatory factor expression. In mice fed a methionine-choline-deficient (MCD) diet, Ta<sub>4</sub>C<sub>3</sub> reduced lipid accumulation, the infiltration of inflammatory cells, and liver cell apoptosis by modulating the cellular microenvironment through its anti-inflammatory and antioxidant properties. Therefore, Ta<sub>4</sub>C<sub>3</sub> can be used as a multifunctional bioactive material to alleviate hepatic steatosis and inflammation in individuals with MAFLD/metabolic dysfunction-associated steatohepatitis (MASH) because of its robust antioxidant and anti-inflammatory effects.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.3,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143571537","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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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