A facile approach was developed for the synthesis of ultrathin ZnS-ZnO nanosheets. By simply manipulating the synthetic temperature, ZnS-ZnO composite nanosheets with sulfur vacancy are successfully obtained using ZnS(en)0.5 as precursor. The formation of the ZnS-ZnO composite leads to the creation of a heterojunction at the interface between the two materials, which enhances the separation of piezogenerated electrons and holes. Additionally, sulfur vacancies are concurrently introduced into the ZnS lattice during the heat treatment process. This defective ZnS with sulfur vacancies exhibits a narrowed bandgap and low excitation energy. Consequently, the defective ZnS-ZnO composite nanosheets demonstrate much higher piezocatalytic activity compared to ZnS and ZnO catalysts, surpassing the performance of most reported piezocatalysts. Furthermore, the ZnS-ZnO composite nanosheets maintain stability over five cycles of catalytic reactions. The study offers a promising approach for enhancing piezocatalytic performance for H2 production.
{"title":"Facile synthesis of defective ZnS-ZnO composite nanosheets for efficient piezocatalytic H2 production","authors":"Xiaoxiao Lu, Xiaojing Zhao, Xiangyu Chen, Miaoqiong Xu, Miaoling Huang, Wen-Jie Chen, Yubin Liu, Xiaoyang Pan","doi":"10.1039/d4nr03733b","DOIUrl":"https://doi.org/10.1039/d4nr03733b","url":null,"abstract":"A facile approach was developed for the synthesis of ultrathin ZnS-ZnO nanosheets. By simply manipulating the synthetic temperature, ZnS-ZnO composite nanosheets with sulfur vacancy are successfully obtained using ZnS(en)0.5 as precursor. The formation of the ZnS-ZnO composite leads to the creation of a heterojunction at the interface between the two materials, which enhances the separation of piezogenerated electrons and holes. Additionally, sulfur vacancies are concurrently introduced into the ZnS lattice during the heat treatment process. This defective ZnS with sulfur vacancies exhibits a narrowed bandgap and low excitation energy. Consequently, the defective ZnS-ZnO composite nanosheets demonstrate much higher piezocatalytic activity compared to ZnS and ZnO catalysts, surpassing the performance of most reported piezocatalysts. Furthermore, the ZnS-ZnO composite nanosheets maintain stability over five cycles of catalytic reactions. The study offers a promising approach for enhancing piezocatalytic performance for H2 production.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"3 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594318","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}
Sajid Sajid, Salem Alzahmi, Nouar Tabet, Mohammad Y. Al-Haik, Saleh T. Mahmoud, Yousef Haik, Ahmed Mourtada Elseman, Ihab M Obaidat
Perovskite solar cells (PSCs) with high power conversion efficiencies (PCEs) can be produced using a variety of methods, such as different fabrication methods, device layout modification, and ingredients and interfaces engineering. The efficiency of the perovskite solar cell is largely dependent on the overall quality of the perovskite thin-film in every scenario. The utilization of spin-coating followed by antisolvent pouring (ASP) method is prevalent in nearly all fabrication techniques to attain a superior perovskite thin-films. Nevertheless, there are a few guidelines that must be followed precisely when using ASP approach, including antisolvent amount, duration, and the area for dropping. The aforementioned challenging and necessary strategies frequently result in perovskite thin-films with pinholes, tiny grains, and broad grain boundaries, which impair the performance of PSCs. Therefore, the implementation of a straightforward approach that does not require the use of such complex ASP steps is crucial. Here, we employ a simple process that involves the hot-dipping of lead iodide (PbI2) thin-films in a hot solution of methylammonium iodide (MAI) and formamidinium iodide (FAI) in isopropanol (IPA) to produce high-quality perovskite thin-films. As the time required for the desired perovskite to crystallize is critical, we carefully examined the various hot-dipping process times, such as 10 seconds, 20 seconds, 30 seconds, and 40 seconds. These time intervals yielded thin-films, which were named PSK-10, PSK-20, PSK-30, and PSK-40, respectively. Morphological and optoelectronic characterization demonstrated the high quality of the perovskite thin-films obtained through dipping PbI2 for 30 seconds. Consequently, PSK-30-based PSCs produced higher PCEs up to 21.52% compared to the ASP-based devices (20.79%). Furthermore, the unsealed PSCs prepared with PSK-30 and ASP were assessed for 252 hours at 25℃ and 40-45% relative humidity in order to determine their operational stability. The ASP-based device demonstrated poor stability, maintaining only 10% of the original PCE, whereas the PSK-30-based device retained 70% of its initial PCE. These results offer a new and viable approach to producing highly efficient and stable PSCs.
{"title":"Facile Approach for Fabricating Efficient and Stable Perovskite Solar Cells","authors":"Sajid Sajid, Salem Alzahmi, Nouar Tabet, Mohammad Y. Al-Haik, Saleh T. Mahmoud, Yousef Haik, Ahmed Mourtada Elseman, Ihab M Obaidat","doi":"10.1039/d4nr03705g","DOIUrl":"https://doi.org/10.1039/d4nr03705g","url":null,"abstract":"Perovskite solar cells (PSCs) with high power conversion efficiencies (PCEs) can be produced using a variety of methods, such as different fabrication methods, device layout modification, and ingredients and interfaces engineering. The efficiency of the perovskite solar cell is largely dependent on the overall quality of the perovskite thin-film in every scenario. The utilization of spin-coating followed by antisolvent pouring (ASP) method is prevalent in nearly all fabrication techniques to attain a superior perovskite thin-films. Nevertheless, there are a few guidelines that must be followed precisely when using ASP approach, including antisolvent amount, duration, and the area for dropping. The aforementioned challenging and necessary strategies frequently result in perovskite thin-films with pinholes, tiny grains, and broad grain boundaries, which impair the performance of PSCs. Therefore, the implementation of a straightforward approach that does not require the use of such complex ASP steps is crucial. Here, we employ a simple process that involves the hot-dipping of lead iodide (PbI2) thin-films in a hot solution of methylammonium iodide (MAI) and formamidinium iodide (FAI) in isopropanol (IPA) to produce high-quality perovskite thin-films. As the time required for the desired perovskite to crystallize is critical, we carefully examined the various hot-dipping process times, such as 10 seconds, 20 seconds, 30 seconds, and 40 seconds. These time intervals yielded thin-films, which were named PSK-10, PSK-20, PSK-30, and PSK-40, respectively. Morphological and optoelectronic characterization demonstrated the high quality of the perovskite thin-films obtained through dipping PbI2 for 30 seconds. Consequently, PSK-30-based PSCs produced higher PCEs up to 21.52% compared to the ASP-based devices (20.79%). Furthermore, the unsealed PSCs prepared with PSK-30 and ASP were assessed for 252 hours at 25℃ and 40-45% relative humidity in order to determine their operational stability. The ASP-based device demonstrated poor stability, maintaining only 10% of the original PCE, whereas the PSK-30-based device retained 70% of its initial PCE. These results offer a new and viable approach to producing highly efficient and stable PSCs.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"144 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142594269","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}
Ionic thermal sensors (ITSs) represent a promising frontier in sensing technology, offering unique advantages over conventional electronic sensors. Comprising a polymer matrix and electrolyte, these sensors possess inherent flexibility, stretchability, and biocompatibility, allowing them to establish stable and intimate contact with soft surfaces without inducing mechanical or thermal stress. Through an ion migration/dissociation mechanism similar to biosensing, ITS ensures low impedance contact and high sensitivity, especially in physiological monitoring applications. This review provides a comprehensive overview of ionic thermal sensing mechanisms, contrasting them with their electronic counterparts. Additionally, it explores the intricacy of the sensor architecture, detailing the roles of active sensing elements, stretchable electrodes, and flexible substrates. The decoupled sensing mechanisms for skin-inspired multimodal sensors are also introduced based on several representative examples. The latest applications of ITS are categorized into ionic skin (i-skin), healthcare, spatial thermal perception, and environment detection, regarding to their materials, structures, and operation modes. Finally, the perspectives of ITS research are presented, emphasizing the significance of standardized sensing parameters and emerging requirements for practical applications.
{"title":"Advances in Flexible Ionic Thermal Sensors: Present and Perspectives","authors":"Zehao Zhao, Yun Shen, Run Hu, Dongyan Xu","doi":"10.1039/d4nr03423f","DOIUrl":"https://doi.org/10.1039/d4nr03423f","url":null,"abstract":"Ionic thermal sensors (ITSs) represent a promising frontier in sensing technology, offering unique advantages over conventional electronic sensors. Comprising a polymer matrix and electrolyte, these sensors possess inherent flexibility, stretchability, and biocompatibility, allowing them to establish stable and intimate contact with soft surfaces without inducing mechanical or thermal stress. Through an ion migration/dissociation mechanism similar to biosensing, ITS ensures low impedance contact and high sensitivity, especially in physiological monitoring applications. This review provides a comprehensive overview of ionic thermal sensing mechanisms, contrasting them with their electronic counterparts. Additionally, it explores the intricacy of the sensor architecture, detailing the roles of active sensing elements, stretchable electrodes, and flexible substrates. The decoupled sensing mechanisms for skin-inspired multimodal sensors are also introduced based on several representative examples. The latest applications of ITS are categorized into ionic skin (i-skin), healthcare, spatial thermal perception, and environment detection, regarding to their materials, structures, and operation modes. Finally, the perspectives of ITS research are presented, emphasizing the significance of standardized sensing parameters and emerging requirements for practical applications.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"17 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588978","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}
Photodynamic therapy (PDT) and chemodynamic therapy (CDT) are both promising cancer treatments to inhibit tumor cells by generating highly cytotoxic reactive oxygen species (ROS). Herein, we report a novel tumor microenvironment (TME) stimulus-responsive water-soluble glycosylated photosensitizer (BT-TPE@Fe-Lac), which can serve as a high-efficiency antitumor agent by combining PDT and CDT, based on the coordination of Fe³⁺ with lactosyl bis(2-pyridylmethyl)amine and AIE luminogen (benzothiazole-hydroxytetraphenylethene, BT-TPE). BT-TPE@Fe-Lac is stable under physiological conditions and selectively targets HepG2 cells via asialoglycoprotein receptor (ASGPR)-mediated endocytosis. It rapidly dissociated into AIE-active BT-TPE molecules and lactosyl ferric (III) complex in the acidic lysosomes of cancer cells. Upon exposure to light, the BT-TPE produced O₂•⁻ radicals for type I PDT. Ferric (III) complex were reduced to Fe(II) complex upon depletion of glutathione, which primes the breakdown of endogenous H2O2 within the tumor microenvironment, thus generating highly toxic •OH for enhanced CDT. Compared with monotherapy of PDT or CDT, BT-TPE@Fe-Lac can significantly increase the intracellular ROS levels to induce more tumor cell death under low drug doses and hypoxia-dependent conditions. This strategy leverages the unique properties of the TME to optimize therapeutic outcomes, offering a promising approach for the TME-responsive nanoplatform in advanced cancer therapy.
{"title":"Glycosylated AIE-active Fe (III) photosensitizer activated by tumor microenvironment for synergistic type I photodynamic and chemodynamic therapy","authors":"Gai-li Feng, Wei Zhou, Jinping Qiao, Guang-Jian Liu, Guo-Wen Xing","doi":"10.1039/d4nr03871a","DOIUrl":"https://doi.org/10.1039/d4nr03871a","url":null,"abstract":"Photodynamic therapy (PDT) and chemodynamic therapy (CDT) are both promising cancer treatments to inhibit tumor cells by generating highly cytotoxic reactive oxygen species (ROS). Herein, we report a novel tumor microenvironment (TME) stimulus-responsive water-soluble glycosylated photosensitizer (<strong>BT-TPE@Fe-Lac</strong>), which can serve as a high-efficiency antitumor agent by combining PDT and CDT, based on the coordination of Fe³⁺ with lactosyl bis(2-pyridylmethyl)amine and AIE luminogen (benzothiazole-hydroxytetraphenylethene,<strong> BT-TPE</strong>). <strong>BT-TPE@Fe-Lac</strong> is stable under physiological conditions and selectively targets HepG2 cells via asialoglycoprotein receptor (ASGPR)-mediated endocytosis. It rapidly dissociated into AIE-active <strong>BT-TPE</strong> molecules and lactosyl ferric (III) complex in the acidic lysosomes of cancer cells. Upon exposure to light, the <strong>BT-TPE</strong> produced O₂<small><sup>•</sup></small>⁻ radicals for type I PDT. Ferric (III) complex were reduced to Fe(II) complex upon depletion of glutathione, which primes the breakdown of endogenous H<small><sub>2</sub></small>O<small><sub>2</sub></small> within the tumor microenvironment, thus generating highly toxic •OH for enhanced CDT. Compared with monotherapy of PDT or CDT, <strong>BT-TPE@Fe-Lac</strong> can significantly increase the intracellular ROS levels to induce more tumor cell death under low drug doses and hypoxia-dependent conditions. This strategy leverages the unique properties of the TME to optimize therapeutic outcomes, offering a promising approach for the TME-responsive nanoplatform in advanced cancer therapy.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"17 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142589052","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}
Saman Bagheri, Rashmeet Kaur Khurana, Md. Ibrahim Kholil, Michael J. Loes, Shengyuan Luo, Alexander Sinitskii
MXenes are a large family of two-dimensional transition metal carbides, nitrides, and carbonitrides. While MXenes have great potential for applications in analytical chemistry, most of the studies in this field focused on Ti3C2Tx, the most popular MXene material. For example, several studies employed Ti3C2Tx as an adsorbent for the trace detection of toxic analytes, but there is limited knowledge on the utility of other MXene materials for this application. In this work, we investigated the potential of Cr2TiC2Tx, one of the least studied MXenes, for application as an adsorbent material in the ultrasonic-assisted dispersive micro solid-phase extraction (d-μ-SPE) method for the detection of heavy metals at trace levels in food and soil samples. We synthesized a Cr2TiC2Tx material comprising μm-scale monolayer flakes and characterized it by a variety of microscopic and spectroscopic techniques. Cr2TiC2Tx MXene showed remarkable performance in the d-μ-SPE method with the detection limits of 0.09 and 1.9 ng mL−1, and dynamic ranges of 0.3−90 μg L−1 and 6−120 μg L−1 for cadmium (Cd2+) and lead (Pb2+) ions, respectively. The great performance of Cr2TiC2Tx MXene as an adsorbent for the trace detection of heavy metals highlights the importance of investigating other MXenes beyond Ti3C2Tx for analytical applications.
{"title":"Cr2TiC2Tx MXene as an Adsorbent Material in Ultrasonic-Assisted d-µ-Solid Phase Extraction for Trace Detection of Heavy Metals","authors":"Saman Bagheri, Rashmeet Kaur Khurana, Md. Ibrahim Kholil, Michael J. Loes, Shengyuan Luo, Alexander Sinitskii","doi":"10.1039/d4nr02556c","DOIUrl":"https://doi.org/10.1039/d4nr02556c","url":null,"abstract":"MXenes are a large family of two-dimensional transition metal carbides, nitrides, and carbonitrides. While MXenes have great potential for applications in analytical chemistry, most of the studies in this field focused on Ti3C2Tx, the most popular MXene material. For example, several studies employed Ti3C2Tx as an adsorbent for the trace detection of toxic analytes, but there is limited knowledge on the utility of other MXene materials for this application. In this work, we investigated the potential of Cr2TiC2Tx, one of the least studied MXenes, for application as an adsorbent material in the ultrasonic-assisted dispersive micro solid-phase extraction (d-μ-SPE) method for the detection of heavy metals at trace levels in food and soil samples. We synthesized a Cr2TiC2Tx material comprising μm-scale monolayer flakes and characterized it by a variety of microscopic and spectroscopic techniques. Cr2TiC2Tx MXene showed remarkable performance in the d-μ-SPE method with the detection limits of 0.09 and 1.9 ng mL−1, and dynamic ranges of 0.3−90 μg L−1 and 6−120 μg L−1 for cadmium (Cd2+) and lead (Pb2+) ions, respectively. The great performance of Cr2TiC2Tx MXene as an adsorbent for the trace detection of heavy metals highlights the importance of investigating other MXenes beyond Ti3C2Tx for analytical applications.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"243 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142589224","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}
Yuanpeng Zhang, Bei Yan, Xingge Li, Huan Liu, Xiao Liu, Xianjin Xiao, Zenghui Mao, Zhihao Ming
DNA computing circuits are favored by researchers due to their high density, high parallelism, and biocompatibility. However, compared with electronic circuits, current DNA circuits have significant errors in understanding the OFF state and logic “0”. Nowadays, DNA circuits only have two input states: logic “0” and logic “1”, where logic “0” also means the OFF state. Corresponding to an electronic circuit, it is more like an on-off switch than a logic circuit. To correct this conceptual confusion, we propose a three-level circuit. The circuit divides the input signal into three cases: “none”, logic “0” and logic “1”. In subsequent experiments, 34 input combinations of primary AND gate, OR gate and secondary AND-OR, OR-AND cascade circuits were successfully implemented to perform the operation, which distinguished the OFF state and logic “0” correctly. Based on this, we implemented a more complex voting operation with only 12 strands successfully. We believe that our redefinition of OFF state and logic “0” will promote tremendous developments in DNA computing circuits.
DNA 计算电路因其高密度、高并行性和生物兼容性而受到研究人员的青睐。然而，与电子电路相比，目前的 DNA 电路在理解关断状态和逻辑 "0 "时存在很大误差。目前，DNA 电路只有两种输入状态：逻辑 "0 "和逻辑 "1"，其中逻辑 "0 "也意味着关断状态。与电子电路相对应，它更像是一个开关，而不是逻辑电路。为了纠正这种概念上的混淆，我们提出了一种三电平电路。该电路将输入信号分为三种情况：无"、逻辑 "0 "和逻辑 "1"。在随后的实验中，我们成功实现了 34 种输入组合的一级 AND 门、OR 门和二级 AND-OR、OR-AND 级联电路来执行操作，正确区分了关断状态和逻辑 "0"。在此基础上，我们成功地实现了仅有 12 条链的更复杂的表决操作。我们相信，我们对OFF状态和逻辑 "0 "的重新定义将推动DNA计算电路的巨大发展。
{"title":"Refined Design of DNA Logic Gate for Implementing DNA-based Three-level Circuit","authors":"Yuanpeng Zhang, Bei Yan, Xingge Li, Huan Liu, Xiao Liu, Xianjin Xiao, Zenghui Mao, Zhihao Ming","doi":"10.1039/d4nr03606a","DOIUrl":"https://doi.org/10.1039/d4nr03606a","url":null,"abstract":"DNA computing circuits are favored by researchers due to their high density, high parallelism, and biocompatibility. However, compared with electronic circuits, current DNA circuits have significant errors in understanding the OFF state and logic “0”. Nowadays, DNA circuits only have two input states: logic “0” and logic “1”, where logic “0” also means the OFF state. Corresponding to an electronic circuit, it is more like an on-off switch than a logic circuit. To correct this conceptual confusion, we propose a three-level circuit. The circuit divides the input signal into three cases: “none”, logic “0” and logic “1”. In subsequent experiments, 34 input combinations of primary AND gate, OR gate and secondary AND-OR, OR-AND cascade circuits were successfully implemented to perform the operation, which distinguished the OFF state and logic “0” correctly. Based on this, we implemented a more complex voting operation with only 12 strands successfully. We believe that our redefinition of OFF state and logic “0” will promote tremendous developments in DNA computing circuits.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"1 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142589022","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}
Reducing MOF particles to the nanoscale size range is beneficial due to their increased surface-to-volume ratio, higher defects exposing metals and ligands, and short diffusion path. While great efforts have been made to reduce the particle sizes by controlling the reaction kinetics or terminating the particle growth, large-scale, rapid synthesis of MOF nanoparticles (NPs) remains a challenge. Here, we report supercritical (sc) CO2-assisted synthesis of HKUST-1 NPs in a continuous flow reactor, which yielded pure and thermally stable MOFs with median sizes of 110 250 nm and BET surface area of 1610 – 1890 m2/g with under 10 seconds synthesis time. ScCO2 and ethanol with a mole ratio of 9:1 are used as co-solvents for the fast nucleation of HKUST-1 and crystal formation. A typical dry yield of 53.7 wt % is achieved with 0.1 M Cu precursor under mild conditions at 75°C and 13 MPa. The space-time yields and surface area production rates are 5668 kg∙m-3∙d-1 and 1.0*1010 m2∙m-3∙d-1. Particle size and morphology analysis indicate aggregation of nascent structures occurs in the aerosolized state, leading to a non-classical crystal growth mechanism and enabling multiple pathways for tuning the synthesis process. With the ability to recycle CO2, solvents, and unreacted precursors, the method can be used for the scalable production of MOFs.
{"title":"HKUST-1 MOF Nanoparticles: Non-classical Crystallization Route in Supercritical CO2","authors":"Ji Feng, Almond Lau, Igor V. Novosselov","doi":"10.1039/d4nr03070b","DOIUrl":"https://doi.org/10.1039/d4nr03070b","url":null,"abstract":"Reducing MOF particles to the nanoscale size range is beneficial due to their increased surface-to-volume ratio, higher defects exposing metals and ligands, and short diffusion path. While great efforts have been made to reduce the particle sizes by controlling the reaction kinetics or terminating the particle growth, large-scale, rapid synthesis of MOF nanoparticles (NPs) remains a challenge. Here, we report supercritical (sc) CO2-assisted synthesis of HKUST-1 NPs in a continuous flow reactor, which yielded pure and thermally stable MOFs with median sizes of 110 250 nm and BET surface area of 1610 – 1890 m2/g with under 10 seconds synthesis time. ScCO2 and ethanol with a mole ratio of 9:1 are used as co-solvents for the fast nucleation of HKUST-1 and crystal formation. A typical dry yield of 53.7 wt % is achieved with 0.1 M Cu precursor under mild conditions at 75°C and 13 MPa. The space-time yields and surface area production rates are 5668 kg∙m-3∙d-1 and 1.0*1010 m2∙m-3∙d-1. Particle size and morphology analysis indicate aggregation of nascent structures occurs in the aerosolized state, leading to a non-classical crystal growth mechanism and enabling multiple pathways for tuning the synthesis process. With the ability to recycle CO2, solvents, and unreacted precursors, the method can be used for the scalable production of MOFs.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"129 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142589206","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}
Jinxiu Liu, Chunchi Zhang, Yan Huang, Haijuan Wu, Chao Tan, Zegao Wang
Two-dimensional MoS2 semiconductor has been considered as the promising ingenious solution to extension Moore's law. However, its wafer-scale growth from lab to fab is still in the fancy stages in the field of chip industry. The distribution, concentration and activity of the sulfur-precursor and molybdenum-precursor significantly affect the MoS2 wafter uniform including its grain size, thickness and vacancy. Although the sulfur-precursor has gained much attention, for example, the sulfur source generated from ZnS facilitates the MoS2 growth, the effect of molybdenum-precursor and its growth mechanism is still unclear. In this study, we studied the influence of covalent/ionic molybdenum precursors starting from the principle of chemical vapor deposition and looking for a universal wafer synthesis path. It is found that the reaction speed of Na2MoO4 as a typical ion precursor is very favourable for wafer growth defect control and surface homogeneity compared with MoO3 as a typical covalent precursor. The evaporated [MoO4]2- ion with the smallest cluster has high activity which can easily realize the uniform control of the MoS2 wafer. In addition, the 2-inch monolayer MoS2 film can be grown in the growth time range of 3-5 minutes using ion precursors, which can achieve a mobility of 12 cm2V-1 s -1and maximum IOn/IOff ratio of 9.87×109. This study insights the MoS2 wafer growth mechanism and facilitates the development of a MoS2-based electronics system.
{"title":"Promotion of Mo-based Ionic Crystal Precursor for MoS2 Wafer Growth","authors":"Jinxiu Liu, Chunchi Zhang, Yan Huang, Haijuan Wu, Chao Tan, Zegao Wang","doi":"10.1039/d4nr02955k","DOIUrl":"https://doi.org/10.1039/d4nr02955k","url":null,"abstract":"Two-dimensional MoS2 semiconductor has been considered as the promising ingenious solution to extension Moore's law. However, its wafer-scale growth from lab to fab is still in the fancy stages in the field of chip industry. The distribution, concentration and activity of the sulfur-precursor and molybdenum-precursor significantly affect the MoS2 wafter uniform including its grain size, thickness and vacancy. Although the sulfur-precursor has gained much attention, for example, the sulfur source generated from ZnS facilitates the MoS2 growth, the effect of molybdenum-precursor and its growth mechanism is still unclear. In this study, we studied the influence of covalent/ionic molybdenum precursors starting from the principle of chemical vapor deposition and looking for a universal wafer synthesis path. It is found that the reaction speed of Na2MoO4 as a typical ion precursor is very favourable for wafer growth defect control and surface homogeneity compared with MoO3 as a typical covalent precursor. The evaporated [MoO4]2- ion with the smallest cluster has high activity which can easily realize the uniform control of the MoS2 wafer. In addition, the 2-inch monolayer MoS2 film can be grown in the growth time range of 3-5 minutes using ion precursors, which can achieve a mobility of 12 cm2V-1 s -1and maximum IOn/IOff ratio of 9.87×109. This study insights the MoS2 wafer growth mechanism and facilitates the development of a MoS2-based electronics system.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"61 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580746","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}
Tuning the size of intermetallic nanocrystals is challenging due to the conflicting effects of surface free energy and surface diffusion on the disorder-to-order phase transition during wet-chemistry growth. Herein, we synthesized intermetallic PdCd nanocubes with tunable sizes ranging from 8 to 15 nm by adjusting the Cd precursor concentrations using a wet-chemistry approach. This process shares a mechanism of size tuning similar to quantum dot synthesis, involving the regulation of monomer concentration determined by the precursor concentrations. The intermetallic PdCd nanocubes exhibit distinct size-dependent optical properties compared to platinum group metal nanocrystals of similar size ranges, with increased light-induced catalytic enhancement as size increases. The 15 nm-sized nanocubes exhibited the most significant light-induced catalytic enhancement, reaching 3.3 times, while the 8 nm-sized nanocubes showed only a 1.6-fold enhancement in 4-nitrophenol reduction. This study emphasizes the importance of tuning the size of intermetallic nanocrystals, providing valuable insights for future exploration of their size-dependent properties.
{"title":"Exploring size-dependent optical property alterations in fine-tuning intermetallic PdCd nanocube sizes.","authors":"Jia-Lin Li, Ting-Yu Tien, Hung-Chun Liao, Hsin-Lun Wu","doi":"10.1039/d4nr03640a","DOIUrl":"https://doi.org/10.1039/d4nr03640a","url":null,"abstract":"<p><p>Tuning the size of intermetallic nanocrystals is challenging due to the conflicting effects of surface free energy and surface diffusion on the disorder-to-order phase transition during wet-chemistry growth. Herein, we synthesized intermetallic PdCd nanocubes with tunable sizes ranging from 8 to 15 nm by adjusting the Cd precursor concentrations using a wet-chemistry approach. This process shares a mechanism of size tuning similar to quantum dot synthesis, involving the regulation of monomer concentration determined by the precursor concentrations. The intermetallic PdCd nanocubes exhibit distinct size-dependent optical properties compared to platinum group metal nanocrystals of similar size ranges, with increased light-induced catalytic enhancement as size increases. The 15 nm-sized nanocubes exhibited the most significant light-induced catalytic enhancement, reaching 3.3 times, while the 8 nm-sized nanocubes showed only a 1.6-fold enhancement in 4-nitrophenol reduction. This study emphasizes the importance of tuning the size of intermetallic nanocrystals, providing valuable insights for future exploration of their size-dependent properties.</p>","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":" ","pages":""},"PeriodicalIF":5.8,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142581253","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}
Fátima Santillán, Carlie Charron, Betty Galarreta, Leonard G Luyt
We report the development of a peptide-based optical nanoprobe specifically tailored for prostate cancer imaging. The imaging probe is comprised of cyclic peptide nanotubes, formed via the aqueous co-assembly of four cyclic D,L-alternating octapeptides. The inherent properties of these cyclic building blocks have been carefully selected to enhance their efficacy in imaging applications, through the addition of a cancer targeting peptide and a fluorescent dye. Comprehensive characterization using scanning electron microscopy (FESEM) and low-voltage transmission electron microscopy (LV-TEM) confirms the formation of nanotubes through co-assembly of the cyclic peptides. The resulting nanotubes show an average diameter of 28 nm. Circular dichroism (CD) spectroscopy validates the formation of stable beta-sheet hydrogen bonding structures at both 20 and 37 ºC, ensuring their suitability for biomedical applications. Evaluation of PSMA-binding specificity of the resulting peptide nanotubes is assessed using confocal fluorescence microscopy demonstrating receptor-mediated uptake in prostate cancer cells. We anticipate this strategy will provide the basis for the utilization of co-assembled systems for advancing molecular imaging techniques in prostate cancer and other cancers.
{"title":"Tailored Peptide Nanomaterials for Receptor Targeted Prostate Cancer Imaging","authors":"Fátima Santillán, Carlie Charron, Betty Galarreta, Leonard G Luyt","doi":"10.1039/d4nr03273j","DOIUrl":"https://doi.org/10.1039/d4nr03273j","url":null,"abstract":"We report the development of a peptide-based optical nanoprobe specifically tailored for prostate cancer imaging. The imaging probe is comprised of cyclic peptide nanotubes, formed via the aqueous co-assembly of four cyclic D,L-alternating octapeptides. The inherent properties of these cyclic building blocks have been carefully selected to enhance their efficacy in imaging applications, through the addition of a cancer targeting peptide and a fluorescent dye. Comprehensive characterization using scanning electron microscopy (FESEM) and low-voltage transmission electron microscopy (LV-TEM) confirms the formation of nanotubes through co-assembly of the cyclic peptides. The resulting nanotubes show an average diameter of 28 nm. Circular dichroism (CD) spectroscopy validates the formation of stable beta-sheet hydrogen bonding structures at both 20 and 37 ºC, ensuring their suitability for biomedical applications. Evaluation of PSMA-binding specificity of the resulting peptide nanotubes is assessed using confocal fluorescence microscopy demonstrating receptor-mediated uptake in prostate cancer cells. We anticipate this strategy will provide the basis for the utilization of co-assembled systems for advancing molecular imaging techniques in prostate cancer and other cancers.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"28 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580542","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}
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