Sang-Mun Jung, Yoona Kim, Byung-Jo Lee, Hyeonjung Jung, Jaesub Kwon, Jinhyeon Lee, Kyu-Su Kim, Young-Woo Kim, Ki-Jeong Kim, Hyun-Seok Cho, Jong Hyeok Park, Jeong Woo Han, Yong-Tae Kim
Alkaline Water Electrolysis
碱性水电解
{"title":"Reverse-Current Tolerance for Hydrogen Evolution Reaction Activity of Lead-Decorated Nickel Catalysts in Zero-Gap Alkaline Water Electrolysis Systems (Adv. Funct. Mater. 27/2024)","authors":"Sang-Mun Jung, Yoona Kim, Byung-Jo Lee, Hyeonjung Jung, Jaesub Kwon, Jinhyeon Lee, Kyu-Su Kim, Young-Woo Kim, Ki-Jeong Kim, Hyun-Seok Cho, Jong Hyeok Park, Jeong Woo Han, Yong-Tae Kim","doi":"10.1002/adfm.202470152","DOIUrl":"https://doi.org/10.1002/adfm.202470152","url":null,"abstract":"<b>Alkaline Water Electrolysis</b>","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":null,"pages":null},"PeriodicalIF":19.0,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141496067","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ehsan Alibagheri, Ahmad Ranjbar, Mohammad Khazaei, Thomas D. Kühne, S. Mehdi Vaez Allaei
Haeckelite Structures
海克尔石结构
{"title":"Remarkable Optoelectronic Characteristics of Synthesizable Square-Octagon Haeckelite Structures: Machine Learning Materials Discovery (Adv. Funct. Mater. 27/2024)","authors":"Ehsan Alibagheri, Ahmad Ranjbar, Mohammad Khazaei, Thomas D. Kühne, S. Mehdi Vaez Allaei","doi":"10.1002/adfm.202470150","DOIUrl":"https://doi.org/10.1002/adfm.202470150","url":null,"abstract":"<b>Haeckelite Structures</b>","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":null,"pages":null},"PeriodicalIF":19.0,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141496066","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The bulk photovoltaic effect (BPVE) in ferroelectrics, wherein spontaneous polarization can be reversed within crystals lacking centrosymmetry, encompasses the significant contribution of ferroelectric domain walls (DWs), known as DW‐PVE. Nevertheless, the separation between intrinsic BPVE within the domain and DW‐PVE remains unexplored in 2D ferroelectrics, notwithstanding its significant importance. In this study, sizable crystals of 2D ferroelectric SnS are successfully grown, facilitating a comprehensive yet intricate examination of domain configurations utilizing polarized optical microscopy and piezoresponse force microscopy. By properly selecting the large ferroelectric single domain within SnS crystals, uniform intrinsic BPVE across the domain is unequivocally demonstrated. Furthermore, to further enhance intrinsic BPVE, manipulation of strain poling increased photocurrent, suggesting that locally distributed polarizations due to imperfection introduced in SnS crystals are aligned by strain. These results will offer a new avenue for rigorous comprehension of DW‐PVE in 2D ferroelectrics.
{"title":"Bulk Photovoltaic Effect in Single Ferroelectric Domain of SnS Crystal and Control of Local Polarization by Strain","authors":"Ryo Nanae, Satsuki Kitamura, Yih‐Ren Chang, Kaito Kanahashi, Tomonori Nishimura, Redhwan Moqbel, Kung‐Hsuan Lin, Mina Maruyama, Yanlin Gao, Susumu Okada, Kai Qi, Jui‐Han Fu, Vincent Tung, Takashi Taniguchi, Kenji Watanabe, Kosuke Nagashio","doi":"10.1002/adfm.202406140","DOIUrl":"https://doi.org/10.1002/adfm.202406140","url":null,"abstract":"The bulk photovoltaic effect (BPVE) in ferroelectrics, wherein spontaneous polarization can be reversed within crystals lacking centrosymmetry, encompasses the significant contribution of ferroelectric domain walls (DWs), known as DW‐PVE. Nevertheless, the separation between intrinsic BPVE within the domain and DW‐PVE remains unexplored in 2D ferroelectrics, notwithstanding its significant importance. In this study, sizable crystals of 2D ferroelectric SnS are successfully grown, facilitating a comprehensive yet intricate examination of domain configurations utilizing polarized optical microscopy and piezoresponse force microscopy. By properly selecting the large ferroelectric single domain within SnS crystals, uniform intrinsic BPVE across the domain is unequivocally demonstrated. Furthermore, to further enhance intrinsic BPVE, manipulation of strain poling increased photocurrent, suggesting that locally distributed polarizations due to imperfection introduced in SnS crystals are aligned by strain. These results will offer a new avenue for rigorous comprehension of DW‐PVE in 2D ferroelectrics.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":null,"pages":null},"PeriodicalIF":19.0,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141495766","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ya Ma, Yingui Cao, Menghang Zu, Qiang Gao, Ga Liu, Jianying Ji, Haiting Xu, Qiang Yang, Xiaoxiao Shi, Rui L. Reis, Subhas C. Kundu, Ji Zheng, Zhou Li, Bo Xiao
The treatment outcomes of nanomedicines against colorectal cancer are severely restricted by their insufficient accumulation in the tumor tissues, unsatisfactory antitumor effect, and weak immunometabolic modulation. To address these issues, flying‐saucer‐shaped nanoheterojunctions by coating copper oxide (CuxO) onto the surface of PEGylated zinc oxide (ZnO) nanoparticles are constructed. When exposed to ultrasound, the resultant CuxO@ZnO nanoheterojunctions exhibit increased locomotor activities, facilitating colorectal mucus infiltration, deep tumor penetration, and tumor cell internalization. The decoration of CuxO suppresses the rapid recombination of electrons and holes in CuxO@ZnO exposed to ultrasound, promoting the production of singlet oxygen and hydroxyl radical, which are generated by CuxO through a Fenton‐like chemodynamic reaction and CuxO@ZnO through sonodynamic reaction. After rectal administration, the sono‐chemodynamic CuxO@ZnO plus PD‐L1 antibodies effectively inhibit the growth of orthotopic and distant tumors. It elicits immunometabolic responses by inducing immunogenic cell death, activating the interferon genes signaling pathway stimulator, and inhibiting glucose transport and the glycolytic signaling pathways. This combined modality also increases the proportion of beneficial microbes (e.g., Bifidobacterium) and decreases the abundance of harmful microorganisms (e.g., Romboutsia) in the intestine. This treatment modality (CuxO@ZnO plus ultrasound and PD‐L1 antibodies) is a promising strategy for the synergistic treatment of colorectal cancer.
{"title":"Flying‐Saucer‐Shaped Nanoheterojunctions with Enhanced Colorectal Tumor Accumulation for Increased Oxidative Stress and Immunometabolic Regulation","authors":"Ya Ma, Yingui Cao, Menghang Zu, Qiang Gao, Ga Liu, Jianying Ji, Haiting Xu, Qiang Yang, Xiaoxiao Shi, Rui L. Reis, Subhas C. Kundu, Ji Zheng, Zhou Li, Bo Xiao","doi":"10.1002/adfm.202402164","DOIUrl":"https://doi.org/10.1002/adfm.202402164","url":null,"abstract":"The treatment outcomes of nanomedicines against colorectal cancer are severely restricted by their insufficient accumulation in the tumor tissues, unsatisfactory antitumor effect, and weak immunometabolic modulation. To address these issues, flying‐saucer‐shaped nanoheterojunctions by coating copper oxide (Cu<jats:sub>x</jats:sub>O) onto the surface of PEGylated zinc oxide (ZnO) nanoparticles are constructed. When exposed to ultrasound, the resultant Cu<jats:sub>x</jats:sub>O@ZnO nanoheterojunctions exhibit increased locomotor activities, facilitating colorectal mucus infiltration, deep tumor penetration, and tumor cell internalization. The decoration of Cu<jats:sub>x</jats:sub>O suppresses the rapid recombination of electrons and holes in Cu<jats:sub>x</jats:sub>O@ZnO exposed to ultrasound, promoting the production of singlet oxygen and hydroxyl radical, which are generated by Cu<jats:sub>x</jats:sub>O through a Fenton‐like chemodynamic reaction and Cu<jats:sub>x</jats:sub>O@ZnO through sonodynamic reaction. After rectal administration, the sono‐chemodynamic Cu<jats:sub>x</jats:sub>O@ZnO plus PD‐L1 antibodies effectively inhibit the growth of orthotopic and distant tumors. It elicits immunometabolic responses by inducing immunogenic cell death, activating the interferon genes signaling pathway stimulator, and inhibiting glucose transport and the glycolytic signaling pathways. This combined modality also increases the proportion of beneficial microbes (<jats:italic>e.g</jats:italic>., <jats:italic>Bifidobacterium</jats:italic>) and decreases the abundance of harmful microorganisms (<jats:italic>e.g</jats:italic>., <jats:italic>Romboutsia</jats:italic>) in the intestine. This treatment modality (Cu<jats:sub>x</jats:sub>O@ZnO plus ultrasound and PD‐L1 antibodies) is a promising strategy for the synergistic treatment of colorectal cancer.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":null,"pages":null},"PeriodicalIF":19.0,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141495747","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The significance of exploring optimal electrode materials cannot be overstated, particularly in mitigating the critical issues posed by sluggish redox kinetics, significant volume variations, and severe structural collapse resulting from the insertion and extraction of sodium ions. These efforts are crucial for enhancing the longevity and rapid charging capabilities of sodium‐ion batteries (SIBs). Herein, a defect engineering strategy for the in situ encapsulation of single‐phase ternary iron phosphoselenide into porous carbon by robust chemical bonds with the formation of rod‐like multicavity nanohybrids (FePSe3@C) is presented. The incorporation of Se atom not only modulates the electronic structure of the central metal Fe atom and enhances the intrinsic electrical conductivity, but also generates numerous additional reaction sites and accelerates the reaction kinetics of FePSe3@C, as corroborated by theoretical calculations and kinetic analysis. Notably, the FePSe3@C demonstrates an outstanding rate capability of 321.7 mAh g−1 even at 20 A g−1 and long cycling stability over 1000 cycles. The sodium‐ion full cell, pairing the FePSe3@C anode with the Na3V2(PO4)3@C cathode, exhibits a remarkable energy density of 202 Wh kg−1, demonstrating its practical applicability. This work provides a controllable defect and morphology engineering strategy to construct advanced materials with fast charge transfer for high‐power/energy SIBs.
探索最佳电极材料的意义无论怎样强调都不为过，尤其是在缓解缓慢的氧化还原动力学、显著的体积变化以及钠离子的插入和萃取造成的严重结构塌陷等关键问题方面。这些工作对于提高钠离子电池（SIB）的使用寿命和快速充电能力至关重要。本文提出了一种缺陷工程策略，通过强化学键将单相三元磷硒化铁原位封装到多孔碳中，形成棒状多腔纳米杂化物（FePSe3@C）。理论计算和动力学分析证实，硒原子的加入不仅改变了中心金属 Fe 原子的电子结构，增强了其内在导电性，还产生了大量额外的反应位点，加速了 FePSe3@C 的反应动力学。值得注意的是，即使在 20 A g-1 的条件下，FePSe3@C 也能显示出 321.7 mAh g-1 的出色速率能力和超过 1000 个循环的长期循环稳定性。将 FePSe3@C 阳极与 Na3V2(PO4)3@C 阴极配对的钠离子全电池显示出 202 Wh kg-1 的显著能量密度，证明了其实用性。这项研究提供了一种可控的缺陷和形态工程策略，可为高功率/高能量 SIB 构建具有快速电荷转移的先进材料。
{"title":"Vacancy‐Rich Ternary Iron Phosphoselenide Multicavity Nanorods: A Highly Reversible and Fast Anode for Sodium‐Ion Batteries","authors":"Zhidong Tian, Wei Sun, Jiaqi Yu, Jun Yuan, Junxiang Chen, Yangjie Liu, Yichun Ding, Xiang Hu, Zhenhai Wen","doi":"10.1002/adfm.202404320","DOIUrl":"https://doi.org/10.1002/adfm.202404320","url":null,"abstract":"The significance of exploring optimal electrode materials cannot be overstated, particularly in mitigating the critical issues posed by sluggish redox kinetics, significant volume variations, and severe structural collapse resulting from the insertion and extraction of sodium ions. These efforts are crucial for enhancing the longevity and rapid charging capabilities of sodium‐ion batteries (SIBs). Herein, a defect engineering strategy for the in situ encapsulation of single‐phase ternary iron phosphoselenide into porous carbon by robust chemical bonds with the formation of rod‐like multicavity nanohybrids (FePSe<jats:sub>3</jats:sub>@C) is presented. The incorporation of Se atom not only modulates the electronic structure of the central metal Fe atom and enhances the intrinsic electrical conductivity, but also generates numerous additional reaction sites and accelerates the reaction kinetics of FePSe<jats:sub>3</jats:sub>@C, as corroborated by theoretical calculations and kinetic analysis. Notably, the FePSe<jats:sub>3</jats:sub>@C demonstrates an outstanding rate capability of 321.7 mAh g<jats:sup>−1</jats:sup> even at 20 A g<jats:sup>−1</jats:sup> and long cycling stability over 1000 cycles. The sodium‐ion full cell, pairing the FePSe<jats:sub>3</jats:sub>@C anode with the Na<jats:sub>3</jats:sub>V<jats:sub>2</jats:sub>(PO<jats:sub>4</jats:sub>)<jats:sub>3</jats:sub>@C cathode, exhibits a remarkable energy density of 202 Wh kg<jats:sup>−1</jats:sup>, demonstrating its practical applicability. This work provides a controllable defect and morphology engineering strategy to construct advanced materials with fast charge transfer for high‐power/energy SIBs.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":null,"pages":null},"PeriodicalIF":19.0,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141495773","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yi Zhang, Cheng Liao, Maolan Abudusaimaiti, Haibo Zhou, Jinliang Liu, Wei Li, Yong Zhang, Qingsong Mei
Spatial and temporal precisely control of direction and speed is crucial for nanomotors to enable complex operations and applications in microsurgery, drug delivery, isolation of biological targets, and so on. Judicious material design involving Janus nanoparticles has been popular over the past decades, however, precise and customizable modulation of Janus structure with a specific asymmetric ratio for motion control is still challenging. In this study, a universal “interface allocation” strategy is developed for efficient and controllable preparation of Janus mesoporous silica‐coated upconversion nanoparticles (Janus UCNP@mSiO2) with precisely tuned asymmetric ratio to achieve near‐infrared (NIR)‐controlled active mobility for relieving vessel plaque. Mesoporous silica with a thickness of 50 nm is precisely coated onto the nanoparticles’ surface with an optimal coverage ratio of 50% to encapsulate gas propellant. Upon exposure to upconverted blue light, the nanomotors release nitric oxide, facilitating their motion and pathologically improving atherosclerosis through endothelium‐dependent vasodilation. Experimental and theoretical simulation results demonstrate the advantages of NIR‐controlled Janus upconversion nanomotors in atherosclerosis treatment, including enhanced nanoparticle‐transmittance rate (34.83% to 85.57%) and excellent in vivo therapeutic efficacy.
{"title":"Interface Allocation Precisely Customized Janus Upconversion Nanomotor for Atherosclerosis Amelioration","authors":"Yi Zhang, Cheng Liao, Maolan Abudusaimaiti, Haibo Zhou, Jinliang Liu, Wei Li, Yong Zhang, Qingsong Mei","doi":"10.1002/adfm.202405916","DOIUrl":"https://doi.org/10.1002/adfm.202405916","url":null,"abstract":"Spatial and temporal precisely control of direction and speed is crucial for nanomotors to enable complex operations and applications in microsurgery, drug delivery, isolation of biological targets, and so on. Judicious material design involving Janus nanoparticles has been popular over the past decades, however, precise and customizable modulation of Janus structure with a specific asymmetric ratio for motion control is still challenging. In this study, a universal “interface allocation” strategy is developed for efficient and controllable preparation of Janus mesoporous silica‐coated upconversion nanoparticles (Janus UCNP@mSiO<jats:sub>2</jats:sub>) with precisely tuned asymmetric ratio to achieve near‐infrared (NIR)‐controlled active mobility for relieving vessel plaque. Mesoporous silica with a thickness of 50 nm is precisely coated onto the nanoparticles’ surface with an optimal coverage ratio of 50% to encapsulate gas propellant. Upon exposure to upconverted blue light, the nanomotors release nitric oxide, facilitating their motion and pathologically improving atherosclerosis through endothelium‐dependent vasodilation. Experimental and theoretical simulation results demonstrate the advantages of NIR‐controlled Janus upconversion nanomotors in atherosclerosis treatment, including enhanced nanoparticle‐transmittance rate (34.83% to 85.57%) and excellent in vivo therapeutic efficacy.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":null,"pages":null},"PeriodicalIF":19.0,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141495779","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yingyu Guo, Zhongqiang Chen, Zuanming Jin, Xuefeng Wang, Chao Zhang, Alexey V. Balakin, Alexander P. Shkurinov, Yan Peng, Yiming Zhu, Songlin Zhuang
Terahertz (THz) electromagnetic interference (EMI) shielding materials is crucial for ensuring THz electromagnetic protection and information confidentiality technology. Here, it is demonstrated that high electrical conductivity and strong absorption of THz electromagnetic radiation by type‐II Dirac semimetal PdTe2 film make it a promising material for EMI shielding. Compared to MXene film, a commonly used metallic 2D material, the PdTe2 film demonstrates a remarkable 40.36% increase in average EMI shielding efficiency per unit thickness within a broadband THz frequency range. Furthermore, it is demonstrated that a photoinduced long life‐time THz transparency in Dirac semimetal PdTe2 films is attributed to the formation of small polarons due to the strong electron‐phonon coupling. A 15 nm‐thick PdTe2 film exhibits a photoinduced change of EMI SE of 1.1 dB, a value exceeding three times that measured on MXene film with a similar pump fluence. This work provides insights into the fundamental photocarrier properties in type‐II Dirac semimetals that are essential for designing advanced THz optoelectronic devices.
太赫兹（THz）电磁干扰（EMI）屏蔽材料对于确保太赫兹电磁防护和信息保密技术至关重要。本文研究表明，II型狄拉克半金属PdTe2薄膜具有高导电性和对太赫兹电磁辐射的强吸收性，是一种很有前途的电磁干扰屏蔽材料。与常用的金属二维材料 MXene 薄膜相比，PdTe2 薄膜在宽带太赫兹频率范围内的单位厚度平均 EMI 屏蔽效率显著提高了 40.36%。此外，研究还证明，在狄拉克半金属 PdTe2 薄膜中，光诱导的长寿命太赫兹透明度归因于强电子-声子耦合形成的小极子。15 nm 厚的 PdTe2 薄膜在光诱导下显示出 1.1 dB 的 EMI SE 变化，这个值是在 MXene 薄膜上类似泵浦通量测量值的三倍多。这项研究深入揭示了 II 型狄拉克半金属的基本光电载体特性，这对于设计先进的太赫兹光电器件至关重要。
{"title":"Dynamically Controllable Terahertz Electromagnetic Interference Shielding by Small Polaron Responses in Dirac Semimetal PdTe2 Thin Films","authors":"Yingyu Guo, Zhongqiang Chen, Zuanming Jin, Xuefeng Wang, Chao Zhang, Alexey V. Balakin, Alexander P. Shkurinov, Yan Peng, Yiming Zhu, Songlin Zhuang","doi":"10.1002/adfm.202407749","DOIUrl":"https://doi.org/10.1002/adfm.202407749","url":null,"abstract":"Terahertz (THz) electromagnetic interference (EMI) shielding materials is crucial for ensuring THz electromagnetic protection and information confidentiality technology. Here, it is demonstrated that high electrical conductivity and strong absorption of THz electromagnetic radiation by type‐II Dirac semimetal PdTe<jats:sub>2</jats:sub> film make it a promising material for EMI shielding. Compared to MXene film, a commonly used metallic 2D material, the PdTe<jats:sub>2</jats:sub> film demonstrates a remarkable 40.36% increase in average EMI shielding efficiency per unit thickness within a broadband THz frequency range. Furthermore, it is demonstrated that a photoinduced long life‐time THz transparency in Dirac semimetal PdTe<jats:sub>2</jats:sub> films is attributed to the formation of small polarons due to the strong electron‐phonon coupling. A 15 nm‐thick PdTe<jats:sub>2</jats:sub> film exhibits a photoinduced change of EMI SE of 1.1 dB, a value exceeding three times that measured on MXene film with a similar pump fluence. This work provides insights into the fundamental photocarrier properties in type‐II Dirac semimetals that are essential for designing advanced THz optoelectronic devices.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":null,"pages":null},"PeriodicalIF":19.0,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141495510","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Detection and discrimination of volatile organic compounds (VOCs) is important to provide a more realistic assessment of their potential implication in complex environments and medical diagnostics based on volatile biomarkers. Herein, chemiresistive sensors are fabricated using stacked MoS2 nanoflakes with defects and exposed‐edge sites. The sensor is found to be extremely selective to triethylamine (TEA) over polar, non‐polar VOCs and atmospheric gases. The sensor exhibits a sensitivity of 1.72% ppm−1, fast response/recovery (19 s/39 s) to 100 ppm TEA at room temperature, low limit of detection (64 ppb), device reproducibility, humidity tolerance (RH 90%) and stability tested up to 60 days. The kinetic analysis of sensing curves reveals two discrete adsorption sites corresponding to edge and basal sites of interaction, with a higher rate constant of association and dissociation for TEA. The Density Functional Theory (DFT) studies support higher adsorption energy of TEA on MoS2 surface with respect to other volatile amines. The sensor demonstrates TEA recognition and composition estimation capability in a binary mixture of a similar class of VOCs using Machine Learning driven analysis with 95% accuracy. The ability to discriminate amines in binary mixture of other volatile amines paves the way for the advancement of next‐generation devices in the field of disease diagnosis.
{"title":"Site‐Selective MoS2‐Based Sensor for Detection and Discrimination of Triethylamine from Volatile Amines Using Kinetic Analysis and Machine Learning","authors":"Snehraj Gaur, Sukhwinder Singh, Jyotirmoy Deb, Vansh Bhutani, Rajkumar Mondal, Vishakha Pareek, Ritu Gupta","doi":"10.1002/adfm.202405232","DOIUrl":"https://doi.org/10.1002/adfm.202405232","url":null,"abstract":"Detection and discrimination of volatile organic compounds (VOCs) is important to provide a more realistic assessment of their potential implication in complex environments and medical diagnostics based on volatile biomarkers. Herein, chemiresistive sensors are fabricated using stacked MoS<jats:sub>2</jats:sub> nanoflakes with defects and exposed‐edge sites. The sensor is found to be extremely selective to triethylamine (TEA) over polar, non‐polar VOCs and atmospheric gases. The sensor exhibits a sensitivity of 1.72% ppm<jats:sup>−1</jats:sup>, fast response/recovery (19 s/39 s) to 100 ppm TEA at room temperature, low limit of detection (64 ppb), device reproducibility, humidity tolerance (RH 90%) and stability tested up to 60 days. The kinetic analysis of sensing curves reveals two discrete adsorption sites corresponding to edge and basal sites of interaction, with a higher rate constant of association and dissociation for TEA. The Density Functional Theory (DFT) studies support higher adsorption energy of TEA on MoS<jats:sub>2</jats:sub> surface with respect to other volatile amines. The sensor demonstrates TEA recognition and composition estimation capability in a binary mixture of a similar class of VOCs using Machine Learning driven analysis with 95% accuracy. The ability to discriminate amines in binary mixture of other volatile amines paves the way for the advancement of next‐generation devices in the field of disease diagnosis.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":null,"pages":null},"PeriodicalIF":19.0,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141495618","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Preetam Dacha, Katherina Haase, Angelika Wrzesińska‐Lashkova, Darius Pohl, Roman Maletz, Vojtech Millek, Alexander Tahn, Bernd Rellinghaus, Christina Dornack, Yana Vaynzof, Mike Hambsch, Stefan C. B. Mannsfeld
Sol–gel‐based solution‐processed metal oxides have emerged as a key fabrication method for applications in thin film transistors both as a semiconducting and a dielectric layer. Here, a low‐temperature, green solvent‐based, non‐toxic, and cost‐effective solution shearing approach for the fabrication of thin aluminum oxide (AlOx) dielectrics is reported. Optimization of sustainability aspects like energy demand, and selection of chemicals used allows to reduce the environmental impact of the life cycle of the resulting product already in the design phase. Using this approach, ultra‐thin, device‐grade AlOx films of 7 nm are coated—the thinnest films to be reported for any solution‐fabrication method. The metal oxide formation is achieved by both thermal annealing and deep ultra‐violet (UV) light exposure techniques, resulting in capacitances of 750 and 600 nF cm−2, respectively. The structural analysis using microscopy and x‐ray spectroscopy techniques confirmed the formation of smooth, ultra‐thin AlOx films. These thin films are employed in organic field‐effect transistors (OFETs) resulting in stable, low hysteresis devices leading to high mobilities (6.1 ± 0.9 cm2 V−1 s−1), near zero threshold voltage (−0.14 ± 0.07 V) and a low subthreshold swing (96 ± 16 mV dec−1), enabling device operation at only ±0.5 V with a good Ion/Ioff ratio (3.7 × 105).
{"title":"Eco‐Friendly Approach to Ultra‐Thin Metal Oxides‐ Solution Sheared Aluminum Oxide for Half‐Volt Operation of Organic Field‐Effect Transistors","authors":"Preetam Dacha, Katherina Haase, Angelika Wrzesińska‐Lashkova, Darius Pohl, Roman Maletz, Vojtech Millek, Alexander Tahn, Bernd Rellinghaus, Christina Dornack, Yana Vaynzof, Mike Hambsch, Stefan C. B. Mannsfeld","doi":"10.1002/adfm.202315850","DOIUrl":"https://doi.org/10.1002/adfm.202315850","url":null,"abstract":"Sol–gel‐based solution‐processed metal oxides have emerged as a key fabrication method for applications in thin film transistors both as a semiconducting and a dielectric layer. Here, a low‐temperature, green solvent‐based, non‐toxic, and cost‐effective solution shearing approach for the fabrication of thin aluminum oxide (AlO<jats:sub>x</jats:sub>) dielectrics is reported. Optimization of sustainability aspects like energy demand, and selection of chemicals used allows to reduce the environmental impact of the life cycle of the resulting product already in the design phase. Using this approach, ultra‐thin, device‐grade AlO<jats:sub>x</jats:sub> films of 7 nm are coated—the thinnest films to be reported for any solution‐fabrication method. The metal oxide formation is achieved by both thermal annealing and deep ultra‐violet (UV) light exposure techniques, resulting in capacitances of 750 and 600 nF cm<jats:sup>−2</jats:sup>, respectively. The structural analysis using microscopy and x‐ray spectroscopy techniques confirmed the formation of smooth, ultra‐thin AlO<jats:sub>x</jats:sub> films. These thin films are employed in organic field‐effect transistors (OFETs) resulting in stable, low hysteresis devices leading to high mobilities (6.1 ± 0.9 cm<jats:sup>2</jats:sup> V<jats:sup>−1</jats:sup> s<jats:sup>−1</jats:sup>), near zero threshold voltage (−0.14 ± 0.07 V) and a low subthreshold swing (96 ± 16 mV dec<jats:sup>−1</jats:sup>), enabling device operation at only ±0.5 V with a good <jats:italic>I</jats:italic><jats:sub>on</jats:sub>/<jats:italic>I</jats:italic><jats:sub>off</jats:sub> ratio (3.7 × 10<jats:sup>5</jats:sup>).","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":null,"pages":null},"PeriodicalIF":19.0,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141495706","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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