Haixin Zhou, Kuo Wang, Cong Nie, Jiahao Deng, Ziye Chen, Kang Zhang, Xiaojie Zhao, Jiaojiao Liang, Di Huang, Ling Zhao, Hun Soo Jang, Jeamin Kong
In perovskite solar cells, grain boundaries are considered one of the major structural defect sites, and consequently affect solar cell performance. Therefore, a precise edge detection of perovskite grains may enable to predict resulting solar cell performance. Herein, a deep learning model, Self-UNet, is developed to extract and quantify morphological information such as grain boundary length (GBL), the number of grains (NG), and average grain surface area (AGSA) from scanning elecron microscope (SEM) images. The Self-UNet excels conventional Canny and UNet models in edge extraction; the Dice coefficient and F1-score exhibit as high as 91.22% and 93.58%, respectively. The high edge detection accuracy of Self-UNet allows for not only identifying tiny grains stuck between relatively large grains, but also distinguishing actual grain boundaries from grooves on grain surface from low quality SEM images, avoiding under- or over-estimation of grain information. Moreover, the gradient boosted decision tree (GBDT) regression integrated to the Self-UNet exhibits high accuracy in predicting solar cell efficiency with relative errors of less than 10% compared to the experimentally measured efficiencies, which is corroborated by results from the literature and the experiments. Additionally, the GBL can be verified in multiple ways as a new morphological feature.
{"title":"Quantitative Analysis of Perovskite Morphologies Employing Deep Learning Framework Enables Accurate Solar Cell Performance Prediction","authors":"Haixin Zhou, Kuo Wang, Cong Nie, Jiahao Deng, Ziye Chen, Kang Zhang, Xiaojie Zhao, Jiaojiao Liang, Di Huang, Ling Zhao, Hun Soo Jang, Jeamin Kong","doi":"10.1002/smll.202408528","DOIUrl":"https://doi.org/10.1002/smll.202408528","url":null,"abstract":"In perovskite solar cells, grain boundaries are considered one of the major structural defect sites, and consequently affect solar cell performance. Therefore, a precise edge detection of perovskite grains may enable to predict resulting solar cell performance. Herein, a deep learning model, Self-UNet, is developed to extract and quantify morphological information such as grain boundary length (GBL), the number of grains (NG), and average grain surface area (AGSA) from scanning elecron microscope (SEM) images. The Self-UNet excels conventional Canny and UNet models in edge extraction; the Dice coefficient and F1-score exhibit as high as 91.22% and 93.58%, respectively. The high edge detection accuracy of Self-UNet allows for not only identifying tiny grains stuck between relatively large grains, but also distinguishing actual grain boundaries from grooves on grain surface from low quality SEM images, avoiding under- or over-estimation of grain information. Moreover, the gradient boosted decision tree (GBDT) regression integrated to the Self-UNet exhibits high accuracy in predicting solar cell efficiency with relative errors of less than 10% compared to the experimentally measured efficiencies, which is corroborated by results from the literature and the experiments. Additionally, the GBL can be verified in multiple ways as a new morphological feature.","PeriodicalId":228,"journal":{"name":"Small","volume":"19 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660996","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Due to a typesetting mistake, the image in Figure 3e was incorrectly pasted. The following is a comparison before and after correction:
Before correction
Figure 3. a1) Cross-section image of Cell-A after LECO treatment by TEM. The box indicates the location of CFC and the dashed line indicates the edges of the pyramids before sintering for Cell-A. a2) Partial enlargement at the location of CFC by HADDF-STEM. The element distribution spectrum of a3) Ag and a4) Si element of CFC for Cell-A. (b) The line distribution of elements of CFC for Cell-A. c1) HRTEM image and the corresponding FFT of CFC for Cell-A. d1–d4,e,f1–f2) for Cell-B.
After Correction
Figure 3. a1) Cross-section image of Cell-A after LECO treatment by TEM. The box indicates the location of CFC and the dashed line indicates the edges of the pyramids before sintering for Cell-A. a2) Partial enlargement at the location of CFC by HADDF-STEM. The element distribution spectrum of a3) Ag and a4) Si element of CFC for Cell-A. (b) The line distribution of elements of CFC for Cell-A. c1) HRTEM image and the corresponding FFT of CFC for Cell-A. d1–d4,e,f1–f2) for Cell-B.
We apologize for this error.
{"title":"Correction to “Nano-Size Joule-Heating to Achieve Low-Ohmic Ag─Si Contact on Boron Emitters of n-TOPCon Solar Cells”","authors":"Rui Zhou, Yongsheng Li, Zhikun Zhang, Wenchang Tan, Ziwei Chen, Yuan Lin, Feng Pan","doi":"10.1002/smll.202502824","DOIUrl":"https://doi.org/10.1002/smll.202502824","url":null,"abstract":"<p><i>Small</i> <b>2024</b>, <i>9</i></p>\u0000<p>DOI: 10.1002/smll.202409628</p>\u0000<p>Due to a typesetting mistake, the image in <b>Figure 3</b>e was incorrectly pasted. The following is a comparison before and after correction:</p>\u0000<p><b>Before correction</b></p>\u0000<p><img alt=\"image\" loading=\"lazy\" src=\"/cms/asset/b242c6e3-6b43-41f8-a88f-fae3242be601/smll202502824-gra-0001.png\"/></p>\u0000<p>Figure 3. a<sub>1</sub>) Cross-section image of Cell-A after LECO treatment by TEM. The box indicates the location of CFC and the dashed line indicates the edges of the pyramids before sintering for Cell-A. a<sub>2</sub>) Partial enlargement at the location of CFC by HADDF-STEM. The element distribution spectrum of a3) Ag and a4) Si element of CFC for Cell-A. (b) The line distribution of elements of CFC for Cell-A. c<sub>1</sub>) HRTEM image and the corresponding FFT of CFC for Cell-A. d<sub>1</sub>–d<sub>4</sub>,e,f<sub>1</sub>–f<sub>2</sub>) for Cell-B.</p>\u0000<p><b>After Correction</b></p>\u0000<p><img alt=\"image\" loading=\"lazy\" src=\"/cms/asset/b332292d-0124-4f05-8cfc-07eaa223fb05/smll202502824-gra-0002.png\"/></p>\u0000<p>Figure 3. a<sub>1</sub>) Cross-section image of Cell-A after LECO treatment by TEM. The box indicates the location of CFC and the dashed line indicates the edges of the pyramids before sintering for Cell-A. a<sub>2</sub>) Partial enlargement at the location of CFC by HADDF-STEM. The element distribution spectrum of a3) Ag and a4) Si element of CFC for Cell-A. (b) The line distribution of elements of CFC for Cell-A. c<sub>1</sub>) HRTEM image and the corresponding FFT of CFC for Cell-A. d<sub>1</sub>–d<sub>4</sub>,e,f<sub>1</sub>–f<sub>2</sub>) for Cell-B.</p>\u0000<p>We apologize for this error.</p>","PeriodicalId":228,"journal":{"name":"Small","volume":"2 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143661061","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Tran Thien An Nguyen, Khoa Dang Tran, Duy Thanh Tran, Saleem Sidra, Do Hwan Kim, Nam Hoon Kim, Joong Hee Lee
To reach sustainable and robust green hydrogen energy production, the development of effective and long-lasting electrocatalysts for hydrogen and oxygen evolution reactions (HER and OER) during overall electrochemical water splitting is a critical requirement. In this study, a novel hierarchical nanosheet-based hollow heterostructure of CoxSy-CoO integrated with active iridium clusters (IrCs-CoxSy-CoO) is prepared by a straightforward chemical synthesis approach. The heterostructure offers extensive tunnels, and abundant mesopores, and features a high-density active site at the interfaces, thus greatly improving the overall catalytic performance through the promotion of synergistic effects. The IrCs-CoxSy-CoO catalyst demonstrates low overpotentials of 97 mV for HER and 243 mV for OER at 10 mA cm−2, showcasing remarkable stability and efficiency. The two-electrode cell test demonstrates reliable current response of 10 mA cm−2 at voltage of 1.497 and 1.58 V at temperature of 75 and 25 °C, respectively. Furthermore, the IrCs-CoxSy-CoO catalyst exhibits enhanced durability and performance when compared to the Pt/C(−)//RuO2(+). In practical application, significant current of 0.5/1.0 A cm−2 at 1.8/1.97 V has been achieved in an anion exchange membrane electrolyzer stack, while maintaining high efficiency (68%) and exceptional stability (over 500 h), underscoring the promising potential for sustainable H2 energy production.
{"title":"Tunable Catalytic Performance on Iridium Clusters-Interspersed CoxSy-CoO Nanosheet-Built Hollows for Enhanced Water Splitting","authors":"Tran Thien An Nguyen, Khoa Dang Tran, Duy Thanh Tran, Saleem Sidra, Do Hwan Kim, Nam Hoon Kim, Joong Hee Lee","doi":"10.1002/smll.202412435","DOIUrl":"https://doi.org/10.1002/smll.202412435","url":null,"abstract":"To reach sustainable and robust green hydrogen energy production, the development of effective and long-lasting electrocatalysts for hydrogen and oxygen evolution reactions (HER and OER) during overall electrochemical water splitting is a critical requirement. In this study, a novel hierarchical nanosheet-based hollow heterostructure of Co<sub>x</sub>S<sub>y</sub>-CoO integrated with active iridium clusters (Ir<sub>Cs</sub>-Co<sub>x</sub>S<sub>y</sub>-CoO) is prepared by a straightforward chemical synthesis approach. The heterostructure offers extensive tunnels, and abundant mesopores, and features a high-density active site at the interfaces, thus greatly improving the overall catalytic performance through the promotion of synergistic effects. The Ir<sub>Cs</sub>-Co<sub>x</sub>S<sub>y</sub>-CoO catalyst demonstrates low overpotentials of 97 mV for HER and 243 mV for OER at 10 mA cm<sup>−2</sup>, showcasing remarkable stability and efficiency. The two-electrode cell test demonstrates reliable current response of 10 mA cm<sup>−2</sup> at voltage of 1.497 and 1.58 V at temperature of 75 and 25 °C, respectively. Furthermore, the Ir<sub>Cs</sub>-Co<sub>x</sub>S<sub>y</sub>-CoO catalyst exhibits enhanced durability and performance when compared to the Pt/C<sub>(−)</sub>//RuO<sub>2(+)</sub>. In practical application, significant current of 0.5/1.0 A cm<sup>−2</sup> at 1.8/1.97 V has been achieved in an anion exchange membrane electrolyzer stack, while maintaining high efficiency (68%) and exceptional stability (over 500 h), underscoring the promising potential for sustainable H<sub>2</sub> energy production.","PeriodicalId":228,"journal":{"name":"Small","volume":"56 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660999","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Suwoon Lee, Hansol Choi, Hyunho Lee, Hyung-Jun Song
Recent advances in quantum dot light emitting diode (QLED) technology have enhanced their stability and efficiency. Studies have demonstrated that QLEDs are robust against oxygen, moisture, and low-voltage stress. However, the impact of instantaneous high-voltage exposure on QLEDs, which can occur during manufacturing due to electrostatic discharge (ESD) from friction between non-conductive components, remains unclear. This study systematically investigates the degradation mechanisms of QLEDs caused by ESD at the level of individual layers, pixels, and the overall display panel. When subjected to ESD pulses of several thousand volts for a few nanoseconds, QLEDs exhibit increased leakage current, reduced electroluminescence intensity, and the formation of dark spots within pixels due to the degradation of electrodes rather than the degradation of QDs. Under severe ESD stress (over 10 kV), the electrodes migrate within the device and are finally disconnected. Microstructural analysis confirms that the decreased physical distance between the two electrodes intensified the electric field, potentially converting a diode into a short circuit. The directly exposed pixels are affected by ESD, and those positioned between the ESD source and the ground may also be damaged. These findings underscore the necessity of managing electrostatic accumulation during QLED fabrication to mitigate ESD-related degradation.
{"title":"Impact of Electrostatic Discharge on the Degradation from Pixel to Panel Level of Quantum-Dot Light-Emitting Diode","authors":"Suwoon Lee, Hansol Choi, Hyunho Lee, Hyung-Jun Song","doi":"10.1002/smll.202411539","DOIUrl":"https://doi.org/10.1002/smll.202411539","url":null,"abstract":"Recent advances in quantum dot light emitting diode (QLED) technology have enhanced their stability and efficiency. Studies have demonstrated that QLEDs are robust against oxygen, moisture, and low-voltage stress. However, the impact of instantaneous high-voltage exposure on QLEDs, which can occur during manufacturing due to electrostatic discharge (ESD) from friction between non-conductive components, remains unclear. This study systematically investigates the degradation mechanisms of QLEDs caused by ESD at the level of individual layers, pixels, and the overall display panel. When subjected to ESD pulses of several thousand volts for a few nanoseconds, QLEDs exhibit increased leakage current, reduced electroluminescence intensity, and the formation of dark spots within pixels due to the degradation of electrodes rather than the degradation of QDs. Under severe ESD stress (over 10 kV), the electrodes migrate within the device and are finally disconnected. Microstructural analysis confirms that the decreased physical distance between the two electrodes intensified the electric field, potentially converting a diode into a short circuit. The directly exposed pixels are affected by ESD, and those positioned between the ESD source and the ground may also be damaged. These findings underscore the necessity of managing electrostatic accumulation during QLED fabrication to mitigate ESD-related degradation.","PeriodicalId":228,"journal":{"name":"Small","volume":"90 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143661001","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sodium-ion batteries (SIBs) are emerging as a potential alternative to traditional lithium-ion batteries due to the abundant sodium resources. Carbon anodes, with their stable structure, wide availability, low cost, excellent conductivity, and tunable morphology and pore structure, exhibit outstanding performance in SIBs. This review summarizes the research progress of hard carbon anodes in SIBs, emphasizing the innovative paths and advanced performances achieved through multitrack optimization, including dimensional engineering, heteroatom doping, and microstructural tailoring. Each dimension of carbon material—0D, 1D, 2D, and 3D—offers unique advantages: 0D materials ensure uniform dispersion, 1D materials have short Na+ diffusion paths, 2D materials possess large specific surface areas, and 3D materials provide e−/Na+ conductive networks. Heteroatom doping with elements such as N, S, and P can tune electronic distribution, expand interlayer spacing of carbon, and induce Fermi level shifts, thereby enhancing sodium storage capability. In addition, defect engineering improves electrochemical performance by modifying graphitic crystal structure. Furthermore, suitable pore structure design, particularly closed pore structures, can increase capacity, minimizes side reactions, and suppress degradation. In future studies, optimizing morphology design, exploring heteroatom co-doping, and developing environmentally friendly, low-cost carbon anode methods will drive the application of high-performance and long cycle life SIBs.
{"title":"Multitrack Boosted Hard Carbon Anodes: Innovative Paths and Advanced Performances in Sodium-Ion Batteries","authors":"Mingyang Li, Zijian Li, Fangyuan Bai, Haw Jiunn Woo, Zurina Osman, Bin Fei","doi":"10.1002/smll.202500645","DOIUrl":"https://doi.org/10.1002/smll.202500645","url":null,"abstract":"Sodium-ion batteries (SIBs) are emerging as a potential alternative to traditional lithium-ion batteries due to the abundant sodium resources. Carbon anodes, with their stable structure, wide availability, low cost, excellent conductivity, and tunable morphology and pore structure, exhibit outstanding performance in SIBs. This review summarizes the research progress of hard carbon anodes in SIBs, emphasizing the innovative paths and advanced performances achieved through multitrack optimization, including dimensional engineering, heteroatom doping, and microstructural tailoring. Each dimension of carbon material—0D, 1D, 2D, and 3D—offers unique advantages: 0D materials ensure uniform dispersion, 1D materials have short Na<sup>+</sup> diffusion paths, 2D materials possess large specific surface areas, and 3D materials provide e<sup>−</sup>/Na<sup>+</sup> conductive networks. Heteroatom doping with elements such as N, S, and P can tune electronic distribution, expand interlayer spacing of carbon, and induce Fermi level shifts, thereby enhancing sodium storage capability. In addition, defect engineering improves electrochemical performance by modifying graphitic crystal structure. Furthermore, suitable pore structure design, particularly closed pore structures, can increase capacity, minimizes side reactions, and suppress degradation. In future studies, optimizing morphology design, exploring heteroatom co-doping, and developing environmentally friendly, low-cost carbon anode methods will drive the application of high-performance and long cycle life SIBs.","PeriodicalId":228,"journal":{"name":"Small","volume":"69 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143661057","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The sluggish reaction kinetics of oxygen evolution reaction (OER) significantly limit the efficiency of electrochemical water splitting (EWS) process, making the development of efficient and stable OER electrocatalysts for sustainable EWS important but still challenging to achieve. Herein, a light-assisted improved design of low-budget carbonized wood (CW) with outstanding OER performance is developed by firmly growing CoFe2O4 nanorods and Ag nanoparticles on the CW channels to form self-supporting electrode (CoFe2O4/Ag-CW). The coordination of active CoFe2O4/Ag and porous CW framework results in substantial effective interfaces and abundant electrochemical active sites, and accelerated electrolyte diffusion, electron transfer, and oxygen escaping. Electrochemical measurements and density functional theory calculations suggest the presence of dual microparticle synergies, conducive to optimizing the electronic structure of CoFe2O4/Ag-CW and lowering the energy barrier of O-H bond breaking in H2O for remarkably enhanced OER activity. Under light field assistance, CoFe2O4/Ag-CW exhibits excellent photothermal effect and carrier separation efficiency with ultralow overpotential of 258 mV and long-term stability at 100 mA cm−2. The photothermal effect and the generation of photogenerated carriers enhance OER dynamics and charge transfer efficiency, leading to improved OER performance under light exposure. Overall, the proposed strategy looks promising for efficient and low-cost oxygen generation.
{"title":"CoFe2O4/Ag Heterocatalysts Grown on Carbonized Wood for Light-Promoted Oxygen Evolution Reaction","authors":"Suyue Luo, Zhenzhong Liu, Xinran Yin, Shuo Zhang, Minghui Guo","doi":"10.1002/smll.202410968","DOIUrl":"https://doi.org/10.1002/smll.202410968","url":null,"abstract":"The sluggish reaction kinetics of oxygen evolution reaction (OER) significantly limit the efficiency of electrochemical water splitting (EWS) process, making the development of efficient and stable OER electrocatalysts for sustainable EWS important but still challenging to achieve. Herein, a light-assisted improved design of low-budget carbonized wood (CW) with outstanding OER performance is developed by firmly growing CoFe<sub>2</sub>O<sub>4</sub> nanorods and Ag nanoparticles on the CW channels to form self-supporting electrode (CoFe<sub>2</sub>O<sub>4</sub>/Ag-CW). The coordination of active CoFe<sub>2</sub>O<sub>4</sub>/Ag and porous CW framework results in substantial effective interfaces and abundant electrochemical active sites, and accelerated electrolyte diffusion, electron transfer, and oxygen escaping. Electrochemical measurements and density functional theory calculations suggest the presence of dual microparticle synergies, conducive to optimizing the electronic structure of CoFe<sub>2</sub>O<sub>4</sub>/Ag-CW and lowering the energy barrier of O-H bond breaking in H<sub>2</sub>O for remarkably enhanced OER activity. Under light field assistance, CoFe<sub>2</sub>O<sub>4</sub>/Ag-CW exhibits excellent photothermal effect and carrier separation efficiency with ultralow overpotential of 258 mV and long-term stability at 100 mA cm<sup>−2</sup>. The photothermal effect and the generation of photogenerated carriers enhance OER dynamics and charge transfer efficiency, leading to improved OER performance under light exposure. Overall, the proposed strategy looks promising for efficient and low-cost oxygen generation.","PeriodicalId":228,"journal":{"name":"Small","volume":"21 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143661060","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In the above-mentioned article, the affiliation of the fourth author is partially incorrect. The correct affiliation is “Smart Devices, Brewer Science Inc., Springfield, MO 65806, USA.” Please remove the affiliation of “Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831 USA.”
We apologize for this error.
{"title":"Correction to “Sponge-Like Porous-Conductive Polymer Coating for Ultrastable Silicon Anodes in Lithium-Ion Batteries”","authors":"Yuanyuan Yu, Chen Yang, Yan Jiang, Jiadeng Zhu, Yingying Zhao, Shuheng Liang, Kaixiang Wang, Yulin Zhou, Yuying Liu, Junhua Zhang, Mengjin Jiang","doi":"10.1002/smll.202502962","DOIUrl":"https://doi.org/10.1002/smll.202502962","url":null,"abstract":"<p>Small <b>2023</b>, <i>19</i>, 2303779</p>\u0000<p>DOI: 10.1002/smll.202303779</p>\u0000<p>In the above-mentioned article, the affiliation of the fourth author is partially incorrect. The correct affiliation is “Smart Devices, Brewer Science Inc., Springfield, MO 65806, USA.” Please remove the affiliation of “Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, TN, 37831 USA.”</p>\u0000<p>We apologize for this error.</p>","PeriodicalId":228,"journal":{"name":"Small","volume":"32 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660995","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Wen-Tse Huang, Yi-Shin Chen, Yen-Huei Lin, Agata Lazarowska, Natalia Majewska, Sebastian Mahlik, Grzegorz Leniec, Hsiao-Yu Huang, Amol Singh, Di-Jing Huang, Pengfei Fu, Zewen Xiao, Ru-Shi Liu
Organic manganese halides have gained attention as luminescent materials due to their characteristics, such as low toxicity, ease of synthesis, and high photoluminescence quantum yield (PLQY). This study challenges the common belief that increasing the Mn–Mn distance invariably boosts PLQY. It introduces a 3D diagram illustrating the importance of ground-state and excited-state band alignments in influencing PLQY. The research identifies how different organic cations result in two distinct band alignments, thus impacting PLQY. Additionally, the research delves into the effects of temperature and pressure on the stability of three organic manganese bromides. Findings indicate that the structural attributes of organic cations significantly influence the materials' responses to thermal stress and pressure. For instance, (PPh4)2MnBr4, characterized by a strong conjugation effect and stable structure, displays superior thermal stability and pressure resistance. Conversely, (N-BHMTA)2MnBr4, with a more intricate structure and lower stability, exhibits susceptibility to irreversible structural alterations under elevated temperature and pressure. These insights are pivotal for developing stable, efficient luminescent materials across diverse applications.
{"title":"Rational Design of Organic Manganese Halides for High Quantum Efficiency and Stability","authors":"Wen-Tse Huang, Yi-Shin Chen, Yen-Huei Lin, Agata Lazarowska, Natalia Majewska, Sebastian Mahlik, Grzegorz Leniec, Hsiao-Yu Huang, Amol Singh, Di-Jing Huang, Pengfei Fu, Zewen Xiao, Ru-Shi Liu","doi":"10.1002/smll.202501075","DOIUrl":"https://doi.org/10.1002/smll.202501075","url":null,"abstract":"Organic manganese halides have gained attention as luminescent materials due to their characteristics, such as low toxicity, ease of synthesis, and high photoluminescence quantum yield (PLQY). This study challenges the common belief that increasing the Mn–Mn distance invariably boosts PLQY. It introduces a 3D diagram illustrating the importance of ground-state and excited-state band alignments in influencing PLQY. The research identifies how different organic cations result in two distinct band alignments, thus impacting PLQY. Additionally, the research delves into the effects of temperature and pressure on the stability of three organic manganese bromides. Findings indicate that the structural attributes of organic cations significantly influence the materials' responses to thermal stress and pressure. For instance, (PPh4)2MnBr4, characterized by a strong conjugation effect and stable structure, displays superior thermal stability and pressure resistance. Conversely, (N-BHMTA)<sub>2</sub>MnBr<sub>4</sub>, with a more intricate structure and lower stability, exhibits susceptibility to irreversible structural alterations under elevated temperature and pressure. These insights are pivotal for developing stable, efficient luminescent materials across diverse applications.","PeriodicalId":228,"journal":{"name":"Small","volume":"183 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143661062","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Weijie Zhang, Zhou Lu, Cailing Chen, Peter Vannatta, Chenxin Yang, Abdullah M. Al-Enizi, Ayman Nafady, Shengqian Ma
Despite recent progress in 3D covalent organic frameworks (3D-COFs), their design and synthesis still pose significant challenges, mainly due to a limited mechanistic understanding of their synthesis. Herein, a linker exchange approach has been utilized to synthesize a series of new 3D-COFs by first preparing an imine-linked 3D-COF followed by exchanging with selected linear diamine linkers. This approach can be widely applicable to different types of diamines, enabling rational-designed synthesis of 3D frameworks that are previously inaccessible via direct polymerization in a one-pot reaction. Mechanistic aspects associated with the improved 3D-COF synthesis via the linker exchange approach, are investigated by density functional theory calculations, in which the possibility of the departure of the leaving linker is a spontaneous process with a decrease in enthalpy. Catalytic and computational results revealed that incorporating benzoxazole moiety into the 3D-COF frameworks enables a significant increase in the capability of visible-light-driven catalysis. The overall findings of the present study will pave the way toward the development of 3D-COFs with tunable structures and functions for other promising and challenging applications.
{"title":"Expanded Synthesis of 3D Covalent Organic Frameworks via Linker Exchange for Efficient Photocatalytic Aerobic Oxidation","authors":"Weijie Zhang, Zhou Lu, Cailing Chen, Peter Vannatta, Chenxin Yang, Abdullah M. Al-Enizi, Ayman Nafady, Shengqian Ma","doi":"10.1002/smll.202502316","DOIUrl":"https://doi.org/10.1002/smll.202502316","url":null,"abstract":"Despite recent progress in 3D covalent organic frameworks (3D-COFs), their design and synthesis still pose significant challenges, mainly due to a limited mechanistic understanding of their synthesis. Herein, a linker exchange approach has been utilized to synthesize a series of new 3D-COFs by first preparing an imine-linked 3D-COF followed by exchanging with selected linear diamine linkers. This approach can be widely applicable to different types of diamines, enabling rational-designed synthesis of 3D frameworks that are previously inaccessible via direct polymerization in a one-pot reaction. Mechanistic aspects associated with the improved 3D-COF synthesis via the linker exchange approach, are investigated by density functional theory calculations, in which the possibility of the departure of the leaving linker is a spontaneous process with a decrease in enthalpy. Catalytic and computational results revealed that incorporating benzoxazole moiety into the 3D-COF frameworks enables a significant increase in the capability of visible-light-driven catalysis. The overall findings of the present study will pave the way toward the development of 3D-COFs with tunable structures and functions for other promising and challenging applications.","PeriodicalId":228,"journal":{"name":"Small","volume":"56 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660677","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Shasha Guo, Mohamed Ait Tamerd, Changyuan Li, Xinyue Shi, Menghao Yang, Jingrong Hou, Jie Liu, Mingxue Tang, Shu-Chih Haw, Chien-Te Chen, Ting-Shan Chan, Chang-Yang Kuo, Zhiwei Hu, Long Yang, Jiwei Ma
Magnetite (Fe3O4), a conversion-type anode material, possesses high capacity, cost-effectiveness and environmental friendliness, positioning it as a promising candidate for the large-scale energy storage applications. However, the multi-electron reactions in sodium-ion batteries face challenges originated from the electrochemical inactivity of Na+ intercalation in the conversion-type oxides. In this work, controllable Fe vacancies are tailored in Fe3O4 lattice through the gradient Mo doping. The pair distribution function local structure analysis reveals that the key to stabilizing more Fe vacancies lies in the uniform occupation of Mo dopants at both tetrahedral (8a) and octahedral (16d) sites. The vacancy-rich structure, featuring 7.3% Fe vacancies, achieves a significantly enhanced capacity of 127 mAh g−1 after 150 cycles at 100 mA g−1, in comparison with the 37 mAh g−1 for defect-free Fe3O4. A comprehensive understanding of how the defective structure relates to electrochemical performance is presented, combining physical-electrochemical characterizations with theoretical calculations. The occurred Mo-O interactions enhances electronic conductivity and diminishes electrostatic interactions between intercalated Na+ and lattice O2−. Concurrently, Fe vacancies facilitate bulk Na+ migration with lower energy barrier. This study presents a prospect for modulating the defective structure in transition metal oxides to activate fast and reversible sodium intercalation toward high-performance sodium-ion batteries.
{"title":"Activating Sodium Intercalation in Cation-Deficient Fe3O4 Through Mo Substitution","authors":"Shasha Guo, Mohamed Ait Tamerd, Changyuan Li, Xinyue Shi, Menghao Yang, Jingrong Hou, Jie Liu, Mingxue Tang, Shu-Chih Haw, Chien-Te Chen, Ting-Shan Chan, Chang-Yang Kuo, Zhiwei Hu, Long Yang, Jiwei Ma","doi":"10.1002/smll.202408212","DOIUrl":"https://doi.org/10.1002/smll.202408212","url":null,"abstract":"Magnetite (Fe<sub>3</sub>O<sub>4</sub>), a conversion-type anode material, possesses high capacity, cost-effectiveness and environmental friendliness, positioning it as a promising candidate for the large-scale energy storage applications. However, the multi-electron reactions in sodium-ion batteries face challenges originated from the electrochemical inactivity of Na<sup>+</sup> intercalation in the conversion-type oxides. In this work, controllable Fe vacancies are tailored in Fe<sub>3</sub>O<sub>4</sub> lattice through the gradient Mo doping. The pair distribution function local structure analysis reveals that the key to stabilizing more Fe vacancies lies in the uniform occupation of Mo dopants at both tetrahedral (8<i>a</i>) and octahedral (16<i>d</i>) sites. The vacancy-rich structure, featuring 7.3% Fe vacancies, achieves a significantly enhanced capacity of 127 mAh g<sup>−1</sup> after 150 cycles at 100 mA g<sup>−1</sup>, in comparison with the 37 mAh g<sup>−1</sup> for defect-free Fe<sub>3</sub>O<sub>4</sub>. A comprehensive understanding of how the defective structure relates to electrochemical performance is presented, combining physical-electrochemical characterizations with theoretical calculations. The occurred Mo-O interactions enhances electronic conductivity and diminishes electrostatic interactions between intercalated Na<sup>+</sup> and lattice O<sup>2−</sup>. Concurrently, Fe vacancies facilitate bulk Na<sup>+</sup> migration with lower energy barrier. This study presents a prospect for modulating the defective structure in transition metal oxides to activate fast and reversible sodium intercalation toward high-performance sodium-ion batteries.","PeriodicalId":228,"journal":{"name":"Small","volume":"25 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143660957","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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