Marcin Giza, Aleksey Kozikov, Paula L. Lalaguna, Jake D. Hutchinson, Vaibhav Verma, Benjamin Vella, Rahul Kumar, Nathan Hill, Dumitru Sirbu, Elisabetta Arca, Noel Healy, Rebecca L. Milot, Malcolm Kadodwala, Pablo Docampo
Surface treatment of perovskite materials with their layered counterparts has become an ubiquitous strategy for maximizing device performance. While layered materials confer great benefits to the longevity and long-term efficiency of the resulting device stack via passivation of defects and surface traps, numerous reports have previously demonstrated that these materials evolve under exposure to light and humidity, suggesting that they are not fully stable. Therefore, it is crucial to study the behavior of these materials in isolation and in conditions mimicking a device stack. Here, it is shown that perovskite capping layers templated by a range of cations on top of methylammonium lead iodide devolve in conditions commonly found during perovskite fabrication, such as exposure to light, solvent, and moisture. Photophysical, structural, and morphological studies are used to show that the degradation of these layered perovskites occurs via a self-limiting, pinhole-mediated mechanism. This results in the loss of whole perovskite sheets, from a few monolayers to tens of nanometers of material, until the system stabilizes again as demonstrated for exfoliated flakes of PEA2PbI4. This means that initially targeted structures may have devolved, with clear optimization implications for device fabrication.
{"title":"Illuminating the Devolution of Perovskite Passivation Layers","authors":"Marcin Giza, Aleksey Kozikov, Paula L. Lalaguna, Jake D. Hutchinson, Vaibhav Verma, Benjamin Vella, Rahul Kumar, Nathan Hill, Dumitru Sirbu, Elisabetta Arca, Noel Healy, Rebecca L. Milot, Malcolm Kadodwala, Pablo Docampo","doi":"10.1002/sstr.202400234","DOIUrl":"https://doi.org/10.1002/sstr.202400234","url":null,"abstract":"Surface treatment of perovskite materials with their layered counterparts has become an ubiquitous strategy for maximizing device performance. While layered materials confer great benefits to the longevity and long-term efficiency of the resulting device stack via passivation of defects and surface traps, numerous reports have previously demonstrated that these materials evolve under exposure to light and humidity, suggesting that they are not fully stable. Therefore, it is crucial to study the behavior of these materials in isolation and in conditions mimicking a device stack. Here, it is shown that perovskite capping layers templated by a range of cations on top of methylammonium lead iodide devolve in conditions commonly found during perovskite fabrication, such as exposure to light, solvent, and moisture. Photophysical, structural, and morphological studies are used to show that the degradation of these layered perovskites occurs via a self-limiting, pinhole-mediated mechanism. This results in the loss of whole perovskite sheets, from a few monolayers to tens of nanometers of material, until the system stabilizes again as demonstrated for exfoliated flakes of PEA<sub>2</sub>PbI<sub>4</sub>. This means that initially targeted structures may have devolved, with clear optimization implications for device fabrication.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142218403","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hao Ding, Jingyu Hou, Kun Zhai, Xin Gao, Junquan Huang, Feng Ke, Bingchao Yang, Congpu Mu, Fusheng Wen, Jianyong Xiang, Bochong Wang, Tianyu Xue, Anmin Nie, Xiaobing Liu, Lin Wang, Xiang-Feng Zhou, Zhongyuan Liu
High pressure provides a unique tuning method depending on structure modulation to explore the structure–property relationship. Herein, the pressure-induced structural phase transformation and enhanced superconductivity in a layered binary phosphide Sn4P3 are reported. Comprehensive measurements using in situ synchrotron X-Ray diffraction and Raman spectroscopy reveal a structural phase transition with mild distortion of SnP3 building blocks and interlayer shrinkage under high pressure. This differs from a conventional trigonal SnAs(P)3 to square SnAs(P)4 topotactic transition in SnAs(P)-based compound. Through this structure reconstruction under high pressure, electron distribution has been reorganized and phonons have softened, facilitating a high superconducting temperature (Tc) value of 7.8 K at 34.9 GPa, which is almost six times higher than its ambient value. The study introduces a new transition route in layered SnAs/SnP-based intermetallic materials and provides insight into the structural and electronic changes under high pressure for Sn4P3.
{"title":"Pressure-Enhanced Superconductivity and Structural Phase Transition in Layered Sn4P3","authors":"Hao Ding, Jingyu Hou, Kun Zhai, Xin Gao, Junquan Huang, Feng Ke, Bingchao Yang, Congpu Mu, Fusheng Wen, Jianyong Xiang, Bochong Wang, Tianyu Xue, Anmin Nie, Xiaobing Liu, Lin Wang, Xiang-Feng Zhou, Zhongyuan Liu","doi":"10.1002/sstr.202400381","DOIUrl":"https://doi.org/10.1002/sstr.202400381","url":null,"abstract":"High pressure provides a unique tuning method depending on structure modulation to explore the structure–property relationship. Herein, the pressure-induced structural phase transformation and enhanced superconductivity in a layered binary phosphide Sn<sub>4</sub>P<sub>3</sub> are reported. Comprehensive measurements using in situ synchrotron X-Ray diffraction and Raman spectroscopy reveal a structural phase transition with mild distortion of SnP<sub>3</sub> building blocks and interlayer shrinkage under high pressure. This differs from a conventional trigonal SnAs(P)<sub>3</sub> to square SnAs(P)<sub>4</sub> topotactic transition in SnAs(P)-based compound. Through this structure reconstruction under high pressure, electron distribution has been reorganized and phonons have softened, facilitating a high superconducting temperature (<i>T</i><sub>c</sub>) value of 7.8 K at 34.9 GPa, which is almost six times higher than its ambient value. The study introduces a new transition route in layered SnAs/SnP-based intermetallic materials and provides insight into the structural and electronic changes under high pressure for Sn<sub>4</sub>P<sub>3</sub>.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142218398","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ziying Ji, Yiran Wu, Lu Liu, Wei Zheng, Meng Wu, Yuexia Li, Zhengming Sun, Guobing Ying
The 2D Ti3C2Tx MXene has a large specific surface area, abundant functional groups, and low work function, which has potential in the field of photocatalytic materials. However, the manufacturing of controllable films with high photocatalytic properties and desirable transmittance is a challenging task. Herein, low-cost, large-scale, and rapid preparation of Ti3C2Tx/TiO2 flexible composite films have been successfully prepared by inkjet printing technology, which can be applied in complex and special environments, as well as in photoelectrically controllable places for photocatalytic performance. With the increase of the anatase TiO2, the transmittance of Ti3C2Tx/TiO2 films increases from 55.37% to 73.27% at 780 nm, corresponding to the square resistance of 1.112–206.496 kΩ sq−1 and the figure of merit of 0.48–0.005. When the amount of anatase TiO2 is 15%, the film has the best photocatalytic effect on methylene blue (MB) dye, reaching 68.94%. After five cycles of testing, the degradation efficiency of MB dye decreases by only 5.68%, showing that the film has good cycling stability. This work provides a new research direction for photoelectrically controllable photocatalytic degradation in complex and special environments.
{"title":"Inkjet-Printed Flexible and Transparent Ti3C2Tx/TiO2 Composite Films: A Strategy for Photoelectrically Controllable Photocatalytic Degradation","authors":"Ziying Ji, Yiran Wu, Lu Liu, Wei Zheng, Meng Wu, Yuexia Li, Zhengming Sun, Guobing Ying","doi":"10.1002/sstr.202400214","DOIUrl":"https://doi.org/10.1002/sstr.202400214","url":null,"abstract":"The 2D Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub> MXene has a large specific surface area, abundant functional groups, and low work function, which has potential in the field of photocatalytic materials. However, the manufacturing of controllable films with high photocatalytic properties and desirable transmittance is a challenging task. Herein, low-cost, large-scale, and rapid preparation of Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub>/TiO<sub>2</sub> flexible composite films have been successfully prepared by inkjet printing technology, which can be applied in complex and special environments, as well as in photoelectrically controllable places for photocatalytic performance. With the increase of the anatase TiO<sub>2</sub>, the transmittance of Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub>/TiO<sub>2</sub> films increases from 55.37% to 73.27% at 780 nm, corresponding to the square resistance of 1.112–206.496 kΩ sq<sup>−1</sup> and the figure of merit of 0.48–0.005. When the amount of anatase TiO<sub>2</sub> is 15%, the film has the best photocatalytic effect on methylene blue (MB) dye, reaching 68.94%. After five cycles of testing, the degradation efficiency of MB dye decreases by only 5.68%, showing that the film has good cycling stability. This work provides a new research direction for photoelectrically controllable photocatalytic degradation in complex and special environments.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142218401","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Frank Sailer, Hipassia M. Moura, Taniya Purkait, Lars Vogelsang, Markus Sauer, Annette Foelske, Rainer F. Winter, Alexandre Ponrouch, Miriam M. Unterlass
Hybrid Materials
混合材料
{"title":"Covalently Linked Pigment@TiO2 Hybrid Materials by One-Pot Solvothermal Synthesis","authors":"Frank Sailer, Hipassia M. Moura, Taniya Purkait, Lars Vogelsang, Markus Sauer, Annette Foelske, Rainer F. Winter, Alexandre Ponrouch, Miriam M. Unterlass","doi":"10.1002/sstr.202470043","DOIUrl":"https://doi.org/10.1002/sstr.202470043","url":null,"abstract":"<b>Hybrid Materials</b>","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142218397","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Avi Arya, Sih-Ling Hsu, Chi-You Liu, Meng-Yuan Chang, Jeng-Kuei Chang, Elise Yu-Tzu Li, Yu-Sheng Su
The growing demand for cost-effective and sustainable energy-storage solutions has spurred interest in novel anode materials for lithium-ion batteries (LIBs). In this study, the potential of small-molecule polycyclic aromatic hydrocarbons (SMPAHs) as promising candidates for LIB anodes is explored. Through a comprehensive experimental approach involving electrode fabrication, material characterization, and electrochemical testing, the electrochemical performance of SMPAHs, including naphthalene, biphenyl, 9,9-dimethylfluorene, phenanthrene, p-terphenyl, and pyrene (Py), is thoroughly investigated. In the results, the impressive cycle stability, high specific capacity, and excellent rate capability of the SMPAH electrode are revealed. Additionally, a direct contact prelithiation strategy is implemented to enhance the initial Coulombic efficiency (ICE) of SMPAH anodes, yielding significant improvements in the ICE and cycle stability. Computational simulations provide valuable insights into the electrochemical behavior and lithium-storage mechanisms of SMPAHs, confirming their potential as effective anode materials. The simulations reveal favorable lithium adsorption sites, the predominant storage mechanisms, and the dissolution mechanism of Py through computational calculations. Overall, in this study, the promise of SMPAHs is highlighted as sustainable anode materials for LIBs, advancing energy-storage technologies toward a greener future.
{"title":"Small-Molecule Polycyclic Aromatic Hydrocarbons as Exceptional Long-Cycle-Life Li-Ion Battery Anode Materials","authors":"Avi Arya, Sih-Ling Hsu, Chi-You Liu, Meng-Yuan Chang, Jeng-Kuei Chang, Elise Yu-Tzu Li, Yu-Sheng Su","doi":"10.1002/sstr.202400273","DOIUrl":"https://doi.org/10.1002/sstr.202400273","url":null,"abstract":"The growing demand for cost-effective and sustainable energy-storage solutions has spurred interest in novel anode materials for lithium-ion batteries (LIBs). In this study, the potential of small-molecule polycyclic aromatic hydrocarbons (SMPAHs) as promising candidates for LIB anodes is explored. Through a comprehensive experimental approach involving electrode fabrication, material characterization, and electrochemical testing, the electrochemical performance of SMPAHs, including naphthalene, biphenyl, 9,9-dimethylfluorene, phenanthrene, <i>p</i>-terphenyl, and pyrene (Py), is thoroughly investigated. In the results, the impressive cycle stability, high specific capacity, and excellent rate capability of the SMPAH electrode are revealed. Additionally, a direct contact prelithiation strategy is implemented to enhance the initial Coulombic efficiency (ICE) of SMPAH anodes, yielding significant improvements in the ICE and cycle stability. Computational simulations provide valuable insights into the electrochemical behavior and lithium-storage mechanisms of SMPAHs, confirming their potential as effective anode materials. The simulations reveal favorable lithium adsorption sites, the predominant storage mechanisms, and the dissolution mechanism of Py through computational calculations. Overall, in this study, the promise of SMPAHs is highlighted as sustainable anode materials for LIBs, advancing energy-storage technologies toward a greener future.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142218408","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Immunoglobulins are important building blocks in biology and biotechnology. With the emergence of comprehensive deep-learning approaches, there are enormous opportunities for fast and accurate methods of classification of protein–protein interactions to arise. Herein, widely accessible image classification algorithms for species-specific typification of a range of different immunoglobulin G (IgG) complexes are repurposed. Droplets of various immunoglobulins mixed with a B-cell superantigen (SAg) (recombinant staphylococcal Protein A) are deposited onto hydrophobic polymer substrates and the resulting protein stains are imaged using polarized light microscopy. A comprehensive study based on 23 745 images finds that the pretrained convolutional neural network (CNN) InceptionV3 not only successfully categorizes IgGs from four different species but also predicts their binding affinity to Protein A: averaged over 36 binding pairs, the following are observed: 1) an overall accuracy of 81.4%, 2) the highest prediction accuracy for human IgG, the antibody with the highest binding affinity for Protein A, and 3) that the classification accuracy regarding the various IgG/Protein A ratios generally correlates with the binding strength of the protein–protein–complex as determined via circular dichroism spectroscopy. In addition, the CNN pretrained with IgG/Protein A stain images has been challenged with a new set of images using a different superantigen (SAg, Protein G). Despite the use of the unknown SAg, the CNN correctly classifies the images of human IgG and Protein G as indicated by a 94% accuracy over the various molar binding ratios. These findings are noteworthy because they demonstrate that appropriately pretrained CNNs can be used for the prediction of protein–protein interactions beyond the scope of the original training set. Aided by deep-learning methods, simple stains of mixed protein solutions may serve as accurate predictors of the strength of protein–protein interactions with relevance to protein engineering, self-aggregation, or protein stability in complex media.
免疫球蛋白是生物学和生物技术的重要组成部分。随着综合深度学习方法的出现，出现了快速、准确的蛋白质-蛋白质相互作用分类方法的巨大机遇。在此，我们将广泛使用的图像分类算法重新用于对一系列不同的免疫球蛋白 G（IgG）复合物进行物种特异性分型。将各种免疫球蛋白与 B 细胞超抗原（SAg）（重组葡萄球菌蛋白 A）混合后的液滴沉积在疏水性聚合物基底上，并使用偏振光显微镜对所产生的蛋白染色进行成像。一项基于 23 745 张图像的综合研究发现，预训练卷积神经网络（CNN）InceptionV3 不仅能成功地对来自四个不同物种的 IgG 进行分类，还能预测它们与蛋白 A 的结合亲和力：对 36 对结合对进行平均，观察到以下结果：1) 整体准确率为 81.4%；2) 人类 IgG 的预测准确率最高，它是与蛋白 A 结合亲和力最高的抗体；3) 不同 IgG/Protein A 比率的分类准确率通常与通过圆二色光谱测定的蛋白质-蛋白质-复合物的结合强度相关。此外，使用不同超抗原（SAg，蛋白质 G）的一组新图像对使用 IgG/Protein A 染色图像预训练的 CNN 进行了挑战。尽管使用了未知的 SAg，但 CNN 仍能正确地对人类 IgG 和蛋白质 G 的图像进行分类，在各种摩尔结合率下的准确率高达 94%。这些发现值得注意，因为它们证明了经过适当预训练的 CNN 可用于预测超出原始训练集范围的蛋白质-蛋白质相互作用。在深度学习方法的帮助下，混合蛋白质溶液的简单染色可以准确预测蛋白质-蛋白质相互作用的强度，这与蛋白质工程、自聚集或蛋白质在复杂介质中的稳定性息息相关。
{"title":"Deep-Learning-Assisted Affinity Classification for Humoral Immunoprotein Complexes","authors":"Bahar Dadfar, Safoura Vaez, Cristian Haret, Meike Koenig, Tahereh Mohammadi Hafshejani, Matthias Franzreb, Joerg Lahann","doi":"10.1002/sstr.202400204","DOIUrl":"https://doi.org/10.1002/sstr.202400204","url":null,"abstract":"Immunoglobulins are important building blocks in biology and biotechnology. With the emergence of comprehensive deep-learning approaches, there are enormous opportunities for fast and accurate methods of classification of protein–protein interactions to arise. Herein, widely accessible image classification algorithms for species-specific typification of a range of different immunoglobulin G (IgG) complexes are repurposed. Droplets of various immunoglobulins mixed with a B-cell superantigen (SAg) (recombinant staphylococcal Protein A) are deposited onto hydrophobic polymer substrates and the resulting protein stains are imaged using polarized light microscopy. A comprehensive study based on 23 745 images finds that the pretrained convolutional neural network (CNN) InceptionV3 not only successfully categorizes IgGs from four different species but also predicts their binding affinity to Protein A: averaged over 36 binding pairs, the following are observed: 1) an overall accuracy of 81.4%, 2) the highest prediction accuracy for human IgG, the antibody with the highest binding affinity for Protein A, and 3) that the classification accuracy regarding the various IgG/Protein A ratios generally correlates with the binding strength of the protein–protein–complex as determined via circular dichroism spectroscopy. In addition, the CNN pretrained with IgG/Protein A stain images has been challenged with a new set of images using a different superantigen (SAg, Protein G). Despite the use of the unknown SAg, the CNN correctly classifies the images of human IgG and Protein G as indicated by a 94% accuracy over the various molar binding ratios. These findings are noteworthy because they demonstrate that appropriately pretrained CNNs can be used for the prediction of protein–protein interactions beyond the scope of the original training set. Aided by deep-learning methods, simple stains of mixed protein solutions may serve as accurate predictors of the strength of protein–protein interactions with relevance to protein engineering, self-aggregation, or protein stability in complex media.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142218404","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hyeongmin Je, Sukyoung Won, Jeong Jae Wie, Sanha Kim
Untethered magnetic actuation is an attractive technique for controlling a batch of micrometer-sized soft robots. Recent advancements have enabled each robot to follow its path independently using a single magnetic device. However, applications of magnetic soft microrobots are mostly biased toward the biomedical field. In this study, thermoplastic polyurethane–Fe3O4 nanocomposite soft spinning microrobots, that is, spinbots that actuate on a tabletop magnetic stirrer, were utilized as innovative precision manufacturing tools for spatially selective precision polishing and cleaning. The pivot motion of the revolving spinbots, which involves repetitive sweeping during rotation cycles, is explored. This sweeping action physically removes nanometer-sized surface contaminants from the workpiece, achieving a cleaning efficiency of 99.6%. Multiple spinbots, up to 42 in total, simultaneously operated along their own orbital pathways on three vertically stacked wafers, thereby demonstrating an unprecedented cleaning method. In addition, the spinbots precisely removed materials from the workpiece using a three-body abrasion mechanism. Furthermore, the spinbots contributed to precise material removal, resulting in remarkable surface polishing (Ra ≈ 1.8 nm). This novel polishing system, which uses the collective behavior of multiple spinbots on a tabletop magnetic stirrer, is 1000-fold lighter than current state-of-the-art equipment aimed at achieving similar levels of fine finishing.
{"title":"Spatially Selective Ultraprecision Polishing and Cleaning by Collective Behavior of Micro Spinbots","authors":"Hyeongmin Je, Sukyoung Won, Jeong Jae Wie, Sanha Kim","doi":"10.1002/sstr.202400245","DOIUrl":"https://doi.org/10.1002/sstr.202400245","url":null,"abstract":"Untethered magnetic actuation is an attractive technique for controlling a batch of micrometer-sized soft robots. Recent advancements have enabled each robot to follow its path independently using a single magnetic device. However, applications of magnetic soft microrobots are mostly biased toward the biomedical field. In this study, thermoplastic polyurethane–Fe<sub>3</sub>O<sub>4</sub> nanocomposite soft spinning microrobots, that is, spinbots that actuate on a tabletop magnetic stirrer, were utilized as innovative precision manufacturing tools for spatially selective precision polishing and cleaning. The pivot motion of the revolving spinbots, which involves repetitive sweeping during rotation cycles, is explored. This sweeping action physically removes nanometer-sized surface contaminants from the workpiece, achieving a cleaning efficiency of 99.6%. Multiple spinbots, up to 42 in total, simultaneously operated along their own orbital pathways on three vertically stacked wafers, thereby demonstrating an unprecedented cleaning method. In addition, the spinbots precisely removed materials from the workpiece using a three-body abrasion mechanism. Furthermore, the spinbots contributed to precise material removal, resulting in remarkable surface polishing (<i>R</i>\u0000<sub>a</sub> ≈ 1.8 nm). This novel polishing system, which uses the collective behavior of multiple spinbots on a tabletop magnetic stirrer, is 1000-fold lighter than current state-of-the-art equipment aimed at achieving similar levels of fine finishing.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142218400","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ángela Matarín, Félix Sánchez, Laura Collado, Mariam Barawi, Victor A. de la Peña O'Shea, Avelina Arnanz, Marta Liras, Marta Iglesias
Herein, the synthesis and characterization of two robust tungsten and rhenium carbonyl complexes integrated into an organic polymer (CPP-Re, CPP-W) are reported. These polymers are obtained by a Suzuki coupling reaction between the corresponding dibromo metal-carbonyl substituted dipyrido[3,2-a:2′,3′-c]phenazine complex and 1,3,5-triphenylbenzene-4′,4″,4″,4‴-triboronic acid and integrated catalytic active sites and photosensitizer since they have not only nitrogen sites to coordinate metal active centers as rhenium or tungsten but photoactive units with good charge-separating ability which can significantly improve the CO2 photoreduction reaction (CO2PRR). These polymers show similar activity in solid–gas CO2PRR in absence of sacrificial agents to produce syn gas (CO + H2) but CPP-W selectivity to products change regarding CPP-Re being able to produce also large amount of more demanding electron products such as methane and ethane. Moreover, the single-site Re- or W-CPP catalysts could prevent the dimerization of complexes that produces its deactivation. This work shows the potential of CPPs as matrices to support single active centers for heterogeneous catalysis.
{"title":"Single Site W(0) versus Re(I)-Dipyridophenazine- Based Conjugated Porous Polymer for CO2 Photoreduction","authors":"Ángela Matarín, Félix Sánchez, Laura Collado, Mariam Barawi, Victor A. de la Peña O'Shea, Avelina Arnanz, Marta Liras, Marta Iglesias","doi":"10.1002/sstr.202400185","DOIUrl":"https://doi.org/10.1002/sstr.202400185","url":null,"abstract":"Herein, the synthesis and characterization of two robust tungsten and rhenium carbonyl complexes integrated into an organic polymer (<b>CPP-Re</b>, <b>CPP-W</b>) are reported. These polymers are obtained by a Suzuki coupling reaction between the corresponding dibromo metal-carbonyl substituted dipyrido[3,2-a:2′,3′-c]phenazine complex and 1,3,5-triphenylbenzene-4′,4″,4″,4‴-triboronic acid and integrated catalytic active sites and photosensitizer since they have not only nitrogen sites to coordinate metal active centers as rhenium or tungsten but photoactive units with good charge-separating ability which can significantly improve the CO<sub>2</sub> photoreduction reaction (CO<sub>2</sub>PRR). These polymers show similar activity in solid–gas CO<sub>2</sub>PRR in absence of sacrificial agents to produce syn gas (CO + H<sub>2</sub>) but <b>CPP</b><b>-W</b> selectivity to products change regarding <b>CPP-Re</b> being able to produce also large amount of more demanding electron products such as methane and ethane. Moreover, the single-site <b>Re-</b> or <b>W-CPP</b> catalysts could prevent the dimerization of complexes that produces its deactivation. This work shows the potential of CPPs as matrices to support single active centers for heterogeneous catalysis.","PeriodicalId":21841,"journal":{"name":"Small Structures","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142218402","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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