The brittle buried interface, characterized by weak adhesion to the substrate, numerous imperfections, and unfavorable strain, poses a significant challenge that impairs the overall performance and long-term stability of perovskite solar cells (PSCs). Herein, a robust molecular zipper is constructed through in situ polymerization of self-assembly monomer 4-vinylbenzoic acid (VA), to tightly link the buried interface to the substrate in n-i-p PSCs with an adhesive strength as high as 10.77 MPa. The modified buried interface exhibits improved morphology, suppressed defects, released strain, and matched energy level alignment. The resulting PSCs deliver an absolute gain of ≥1.67% in champion power conversion efficiency based on both one-step deposition protocol and two-step one, demonstrating the universality of this strategy across different film-processing scenarios. The unencapsulated PSCs can retain 94.2% of their initial efficiency after 550 h with a linear extrapolated T90 value of 1230 h, as per the ISOS-L-2 protocol. This work provides a facile strategy to reinforce the buried interface of PSCs.
{"title":"In situ Crosslinked Robust Molecular Zipper at the Buried Interface for Perovskite Photovoltaics","authors":"Yingyi Cao, Xu Zhang, Ke Zhao, Yunxiao Wei, Liu Zhang, Hengyu Zhang, Wenchuan Wang, Can Cui, Peng Wang, Ping Lin, Xiaoping Wu, Changsheng Song, Zhenyi Ni, Jingjing Xue, Rui Wang, Lingbo Xu","doi":"10.1002/adfm.202422205","DOIUrl":"https://doi.org/10.1002/adfm.202422205","url":null,"abstract":"The brittle buried interface, characterized by weak adhesion to the substrate, numerous imperfections, and unfavorable strain, poses a significant challenge that impairs the overall performance and long-term stability of perovskite solar cells (PSCs). Herein, a robust molecular zipper is constructed through in situ polymerization of self-assembly monomer 4-vinylbenzoic acid (VA), to tightly link the buried interface to the substrate in n-i-p PSCs with an adhesive strength as high as 10.77 MPa. The modified buried interface exhibits improved morphology, suppressed defects, released strain, and matched energy level alignment. The resulting PSCs deliver an absolute gain of ≥1.67% in champion power conversion efficiency based on both one-step deposition protocol and two-step one, demonstrating the universality of this strategy across different film-processing scenarios. The unencapsulated PSCs can retain 94.2% of their initial efficiency after 550 h with a linear extrapolated <i>T</i><sub>90</sub> value of 1230 h, as per the ISOS-L-2 protocol. This work provides a facile strategy to reinforce the buried interface of PSCs.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"26 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143417967","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Wenzhen Zhang, Yunpeng Wang, Lei Liu, Yanzi Gao, Bingtao Tang, Yuyuan Yao, Wentao Wang
Structural colorants for ecological fabric dyeing are typically microscale colloidal arrays involving complex and time-consuming self-assembly, it remains a challenge to perform efficient and large-scale double-sided dyeing on disordered fabric surfaces without sacrificing wearing experience. Innovatively, A photonic nanopigment, composed of hollow silica nanospheres with disordered metasurfaces and high surface-charge is designed to overcome the aforementioned challenge. They individually generate non-iridescent structural colors without self-assembly and disperse uniformly in water. By a one-step dip-dyeing strategy, the photonic nanopigments are quickly and selectively deposited onto the yarn surface of fabrics, achieving high-quality double-sided structural coloration. Meanwhile, constructing a hydrogen bond crosslinking network between the fabric and nanospheres by adhesive and tannic acid greatly enhances colorfastness. Furthermore, the fabrics retain inherent softness and excellent breathability, as nanoscale pigments do not clog weaving holes. Such photonic nanopigments provide a versatile platform for industrial structural coloration of various fabrics with different surface roughness and weaving structures.
{"title":"Photonic Nanopigments for Versatile and Scalable Coloration","authors":"Wenzhen Zhang, Yunpeng Wang, Lei Liu, Yanzi Gao, Bingtao Tang, Yuyuan Yao, Wentao Wang","doi":"10.1002/adfm.202425806","DOIUrl":"https://doi.org/10.1002/adfm.202425806","url":null,"abstract":"Structural colorants for ecological fabric dyeing are typically microscale colloidal arrays involving complex and time-consuming self-assembly, it remains a challenge to perform efficient and large-scale double-sided dyeing on disordered fabric surfaces without sacrificing wearing experience. Innovatively, A photonic nanopigment, composed of hollow silica nanospheres with disordered metasurfaces and high surface-charge is designed to overcome the aforementioned challenge. They individually generate non-iridescent structural colors without self-assembly and disperse uniformly in water. By a one-step dip-dyeing strategy, the photonic nanopigments are quickly and selectively deposited onto the yarn surface of fabrics, achieving high-quality double-sided structural coloration. Meanwhile, constructing a hydrogen bond crosslinking network between the fabric and nanospheres by adhesive and tannic acid greatly enhances colorfastness. Furthermore, the fabrics retain inherent softness and excellent breathability, as nanoscale pigments do not clog weaving holes. Such photonic nanopigments provide a versatile platform for industrial structural coloration of various fabrics with different surface roughness and weaving structures.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"64 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143417957","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Self-assembled monolayers (SAMs), particularly those molecules composed of carbazole and phosphonic acid, are widely employed as effective hole-selective layer (HSL) in inverted perovskite solar cells (PSCs). However, the insufficient chemical bond formation with metal oxides (ITO) and self-aggregation in solvents of carbazole phosphonic acid SAM led to non-uniform HSL, which in turn affect power conversion efficiency (PCE) and stability of the PSCs. Herein, a series of benzoic acid materials (BAs), including p-fluorobenzoic acid (FBA) and p-methylbenzoic acid (MBA), are used as post-assembly molecules to effectively fill the voids between the [4-(3,6-dimethyl-9H-carbazole-9-yl)butyl]phosphonic acid (Me-4PACz) molecules to form a denser HSL, which facilitates passivation of the perovskite buried interface. In addition, post-assembled BAs with different dipole moments can effectively adjust the work function of Me-4PACz HSL, facilitating the transport and extraction of charge carriers. Consequently, the PSCs based on Me-4PACz/FBA HSL realize a champion PCE of 25.58%. Moreover, the unencapsulated devices maintain 82% and 94% of the PCE after 800 h of the outdoor storage (RH≈60%) and 2000 h in glove box, respectively. This post-assembly technique enhances both the PCE and stability of the device, blazing a simple and effective pathway for further development of PSCs.
{"title":"Post-Assembled Dipole Benzoic Acids Modified Me-4PACz for Efficient and Stable Inverted Perovskite Solar Cells","authors":"Fan Yuan, Tangyue Xue, Mengzhen Du, Hailiang Huang, Rui Zeng, Linwei Li, Chenyun Wang, Zhiqiang Song, Qiang Guo, Xiaotian Hu, Erjun Zhou","doi":"10.1002/adfm.202425145","DOIUrl":"https://doi.org/10.1002/adfm.202425145","url":null,"abstract":"Self-assembled monolayers (SAMs), particularly those molecules composed of carbazole and phosphonic acid, are widely employed as effective hole-selective layer (HSL) in inverted perovskite solar cells (PSCs). However, the insufficient chemical bond formation with metal oxides (ITO) and self-aggregation in solvents of carbazole phosphonic acid SAM led to non-uniform HSL, which in turn affect power conversion efficiency (PCE) and stability of the PSCs. Herein, a series of benzoic acid materials (BAs), including p-fluorobenzoic acid (FBA) and p-methylbenzoic acid (MBA), are used as post-assembly molecules to effectively fill the voids between the [4-(3,6-dimethyl-9H-carbazole-9-yl)butyl]phosphonic acid (Me-4PACz) molecules to form a denser HSL, which facilitates passivation of the perovskite buried interface. In addition, post-assembled BAs with different dipole moments can effectively adjust the work function of Me-4PACz HSL, facilitating the transport and extraction of charge carriers. Consequently, the PSCs based on Me-4PACz/FBA HSL realize a champion PCE of 25.58%. Moreover, the unencapsulated devices maintain 82% and 94% of the PCE after 800 h of the outdoor storage (RH≈60%) and 2000 h in glove box, respectively. This post-assembly technique enhances both the PCE and stability of the device, blazing a simple and effective pathway for further development of PSCs.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"13 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143417965","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zhibin Wang, Song Zheng, Naizhong Jiang, Hailiang Huang, Ximing Wu, Ruidan Zhang, Yang Lin, Longqi Lin, Xin Zhou, Rui Zeng, Tao Pang, Tianmin Wu, Feng Huang, Daqin Chen
Perovskite light-emitting diodes (PeLEDs) have reached near-unity photoluminescent quantum yields (PLQYs), but further improvements in electroluminescent efficiency are constrained by interfacial energy losses between the emissive layer and charge transport layers. In this study, multifunctional carbon dot organic frameworks (CDOFs) are introduced as a dual-interface modification material for perovskite layer. This approach effectively passivates both the upper and buried interfaces, boosting the PLQY to nearly 100% and enabling an external quantum efficiency of 28.0%. The CDOFs also facilitate balanced charge injection, achieving a low turn-on voltage of only 1.9 V, significantly below the bandgap voltage. Additionally, the exceptional defect passivation imparted by CDOFs significantly bolsters structural stability, achieving a T50 operational lifetime of 81.7 min at an initial ultrahigh luminance of 10 000 cd m−2, with no detectable Joule heating. This study underscores the potential of CDOFs in significantly advancing PeLED performance.
{"title":"Minimizing Interfacial Energy Losses with Carbon Dot Bifacial Modification Layers for High-Efficiency and Stable Perovskite LEDs","authors":"Zhibin Wang, Song Zheng, Naizhong Jiang, Hailiang Huang, Ximing Wu, Ruidan Zhang, Yang Lin, Longqi Lin, Xin Zhou, Rui Zeng, Tao Pang, Tianmin Wu, Feng Huang, Daqin Chen","doi":"10.1002/adfm.202423608","DOIUrl":"https://doi.org/10.1002/adfm.202423608","url":null,"abstract":"Perovskite light-emitting diodes (PeLEDs) have reached near-unity photoluminescent quantum yields (PLQYs), but further improvements in electroluminescent efficiency are constrained by interfacial energy losses between the emissive layer and charge transport layers. In this study, multifunctional carbon dot organic frameworks (CDOFs) are introduced as a dual-interface modification material for perovskite layer. This approach effectively passivates both the upper and buried interfaces, boosting the PLQY to nearly 100% and enabling an external quantum efficiency of 28.0%. The CDOFs also facilitate balanced charge injection, achieving a low turn-on voltage of only 1.9 V, significantly below the bandgap voltage. Additionally, the exceptional defect passivation imparted by CDOFs significantly bolsters structural stability, achieving a T<sub>50</sub> operational lifetime of 81.7 min at an initial ultrahigh luminance of 10 000 cd m<sup>−2</sup>, with no detectable Joule heating. This study underscores the potential of CDOFs in significantly advancing PeLED performance.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"68 5 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418349","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Solar vapor generation (SVG) garners significant attention as a technology for producing clean water owing to its high efficiency and zero carbon emissions. However, the widespread adoption of SVG is constrained by the high cost, low mechanical strength, and complex fabrication processes of current photothermal materials. Lignin and coal, abundant in aromatic rings, C═O bonds, and quinone structures, present natural advantages for enhancing light absorption and improving the mechanical properties of photothermal materials. This review begins with an overview of the fundamentals of SVG and strategies aimed at promoting its efficiency. It then delves into the structural characteristics and photothermal conversion mechanisms of lignin and coal, highlighting their unique contributions to the field. Further, the latest advancements in the application of lignin/coal-based photothermal materials for SVG are comprehensively summarized. This work not only lays a systematic and scientific foundation for the development of next-generation photothermal materials but also underscores the potential for value-added utilization of lignin and coal, thereby contributing to sustainable resource management.
{"title":"Emerging Photothermal Materials from Lignin and Coal for Solar Vapor Generation","authors":"Zhan-Ku Li, Wei-Dong Zhang, Hong-Lei Yan, An Li, Zhi-Ping Lei, Shi-Biao Ren, Zhi-Cai Wang, Heng-Fu Shui","doi":"10.1002/adfm.202424864","DOIUrl":"https://doi.org/10.1002/adfm.202424864","url":null,"abstract":"Solar vapor generation (SVG) garners significant attention as a technology for producing clean water owing to its high efficiency and zero carbon emissions. However, the widespread adoption of SVG is constrained by the high cost, low mechanical strength, and complex fabrication processes of current photothermal materials. Lignin and coal, abundant in aromatic rings, C═O bonds, and quinone structures, present natural advantages for enhancing light absorption and improving the mechanical properties of photothermal materials. This review begins with an overview of the fundamentals of SVG and strategies aimed at promoting its efficiency. It then delves into the structural characteristics and photothermal conversion mechanisms of lignin and coal, highlighting their unique contributions to the field. Further, the latest advancements in the application of lignin/coal-based photothermal materials for SVG are comprehensively summarized. This work not only lays a systematic and scientific foundation for the development of next-generation photothermal materials but also underscores the potential for value-added utilization of lignin and coal, thereby contributing to sustainable resource management.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"46 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418385","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Anuththara S. J. Alujjage, Bairav S. Vishnugopi, Avijit Karmakar, David P. Magee, Yevgen Barsukov, Partha P. Mukherjee
Lithium-ion (Li-ion) batteries have become indispensable as the energy landscape shifts toward electrification. Enhancing their cycle life while ensuring optimal safety and performance is predicated on developing advanced thermal management approaches. Most battery thermal management systems rely on external temperature sensors, which do not reflect the true dynamic changes in internal temperatures, especially under operational extremes. This study utilizes a combination of operando thermal sensing and mechanistic modeling to investigate internal temperature evolution and associated thermo-electrochemical interactions during Li-ion cell cycling. Through this analysis, the non-linear progression in cell temperature dynamics at various operating conditions and the underlying difference between the internal and external temperatures are captured. The internal temperature measurements reveal a critical asymmetry in the thermal response during charge and discharge operation, with a strong dependence on the current rate and operating temperature. In synergy with thermal sensing, a physics-based modeling framework is developed to quantify different modes of heat generation within the cell layers and correlate them with the occurrence of degradation mechanisms, including lithium plating and solid electrolyte interphase interactions. This work provides the baseline for developing onboard diagnostic tools capable of detecting internal cell temperatures and monitoring cell safety through integrated thermal sensing and physics-informed digital twins.
{"title":"Internal Temperature Evolution Metrology and Analytics in Li-Ion Cells","authors":"Anuththara S. J. Alujjage, Bairav S. Vishnugopi, Avijit Karmakar, David P. Magee, Yevgen Barsukov, Partha P. Mukherjee","doi":"10.1002/adfm.202417273","DOIUrl":"https://doi.org/10.1002/adfm.202417273","url":null,"abstract":"Lithium-ion (Li-ion) batteries have become indispensable as the energy landscape shifts toward electrification. Enhancing their cycle life while ensuring optimal safety and performance is predicated on developing advanced thermal management approaches. Most battery thermal management systems rely on external temperature sensors, which do not reflect the true dynamic changes in internal temperatures, especially under operational extremes. This study utilizes a combination of operando thermal sensing and mechanistic modeling to investigate internal temperature evolution and associated thermo-electrochemical interactions during Li-ion cell cycling. Through this analysis, the non-linear progression in cell temperature dynamics at various operating conditions and the underlying difference between the internal and external temperatures are captured. The internal temperature measurements reveal a critical asymmetry in the thermal response during charge and discharge operation, with a strong dependence on the current rate and operating temperature. In synergy with thermal sensing, a physics-based modeling framework is developed to quantify different modes of heat generation within the cell layers and correlate them with the occurrence of degradation mechanisms, including lithium plating and solid electrolyte interphase interactions. This work provides the baseline for developing onboard diagnostic tools capable of detecting internal cell temperatures and monitoring cell safety through integrated thermal sensing and physics-informed digital twins.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"48 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418390","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The growing importance of high-speed and energy-efficient photodetectors in broadband communication has sparked widespread interest in organic materials owing to their tunable optical characteristics and ease of production. However, this Schottky-type organic photodetector (OPD) has low detectivity and a high dark current, requiring additional voltage biasing. Herein, the development of a highly sensitive self-powered OPD with metal-semiconductor-insulator-metal (MSIM) structure (ITO/PEDOT:PSS/Organic photoactive layer/dielectric/silver) is presented, using polymer PM6, acceptor Y6, and its blend with parylene as a dielectric layer for broadband spectral detection spanning the visible to near-infrared (NIR) range at high speeds. Such a new class of devices can produce fast transient photocurrent signals with opposite polarity both under light ON/OFF cycles in response to pulsed optical stimuli, which makes the signals inherently more distinguishable. The detailed transient photocurrent measurements are performed for fabricated MSIM OPD with different illumination conditions at various operational frequencies, and the PM6:Y6-based devices are found to be most sensitive compared to the single-component devices due to increased charge generation and accumulation without voltage biasing. Further, the faster response time (≈nanosecond) of both the positive and negative peaks with a remarkably high cutoff frequency of 5.6 MHz outperformed most of the state-of-the-art OPD. The extraordinary performance of the MSIM photodetector demonstrated by the real-time NIR communication of various ASCII codes suggests its potential for infrared communication. The tunable polarity of the signal offers a novel platform for next-generation transient-type MSIM photodetectors, enhancing their detectivity and response time without the need for additional biasing across a wide range of applications.
{"title":"Ultrafast Highly Sensitive Self-Powered MSIM Photodetector Based on Organic Semiconductor/Dielectric Interfaces for Broadband Visible to Near-Infrared Communication","authors":"Suryakant Singh, Rakesh Suthar, Akihiro Tomimatsu, Pooja Rani, Michio M. Matsushita, Kunio Awaga, Supravat Karak","doi":"10.1002/adfm.202425426","DOIUrl":"https://doi.org/10.1002/adfm.202425426","url":null,"abstract":"The growing importance of high-speed and energy-efficient photodetectors in broadband communication has sparked widespread interest in organic materials owing to their tunable optical characteristics and ease of production. However, this Schottky-type organic photodetector (OPD) has low detectivity and a high dark current, requiring additional voltage biasing. Herein, the development of a highly sensitive self-powered OPD with metal-semiconductor-insulator-metal (MSIM) structure (ITO/PEDOT:PSS/Organic photoactive layer/dielectric/silver) is presented, using polymer PM6, acceptor Y6, and its blend with parylene as a dielectric layer for broadband spectral detection spanning the visible to near-infrared (NIR) range at high speeds. Such a new class of devices can produce fast transient photocurrent signals with opposite polarity both under light ON/OFF cycles in response to pulsed optical stimuli, which makes the signals inherently more distinguishable. The detailed transient photocurrent measurements are performed for fabricated MSIM OPD with different illumination conditions at various operational frequencies, and the PM6:Y6-based devices are found to be most sensitive compared to the single-component devices due to increased charge generation and accumulation without voltage biasing. Further, the faster response time (≈nanosecond) of both the positive and negative peaks with a remarkably high cutoff frequency of 5.6 MHz outperformed most of the state-of-the-art OPD. The extraordinary performance of the MSIM photodetector demonstrated by the real-time NIR communication of various ASCII codes suggests its potential for infrared communication. The tunable polarity of the signal offers a novel platform for next-generation transient-type MSIM photodetectors, enhancing their detectivity and response time without the need for additional biasing across a wide range of applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"183 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143417953","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Tianke Zhu, Gang Wang, Junyu Hou, Wu Sun, Changsheng Song, Qunyao Yuan, Ce Zhang, Xingyu Lei, Yang Su, Min Chen, Yun Song, Jie Zhao
Solid-state lithium metal batteries (LMBs) with high safety and energy density are the ultimate goal for energy storage systems. The bottleneck lies in the solid electrolytes, which must maintain perfect solid–solid contact and be electrochemically stable for both Li anode and high-voltage cathode. Here, we develop an in situ polymerized hetero-layered electrolyte that simultaneously broadens the electrochemical window and addresses interfacial issues between multiple components. The polyvinylidene fluoride (PVDF) layer toward the cathode improves high voltage compatibility to 4.8 V, while the boron nitride (BN) layer toward the anode provides sufficient mechanical strength, regulates Li-ions transport and promotes the formation of an inorganic-rich solid electrolyte interphase (SEI). The effect of the hetero-layered structure is then verified in an easy-to-process in situ polymerized poly(1,3-dioxane) (PDOL) electrolyte, that seamlessly integrates multiple interfaces, bridging cathode, PVDF, BN, and Li metal. This solid electrolyte is characterized by high room temperature (RT) ionic conductivity (2.1 × 10−3 Scm−1), and high Li-ions transference number (0.801). Most importantly, the Li|LiNi0.6Co0.2Mn0.2O2(NCM622) full batteries show remarkable cycling performance with capacity retention of 90.3% over 200 cycles at 0.5 C. The hetero-layered structure with a seamless in situ polymerized interface provides a new avenue for high-energy, solid-state LMBs.
{"title":"Heterogeneous Engineered Solid Electrolyte for Seamless and Stable Integration of Anode and Cathode","authors":"Tianke Zhu, Gang Wang, Junyu Hou, Wu Sun, Changsheng Song, Qunyao Yuan, Ce Zhang, Xingyu Lei, Yang Su, Min Chen, Yun Song, Jie Zhao","doi":"10.1002/adfm.202501870","DOIUrl":"https://doi.org/10.1002/adfm.202501870","url":null,"abstract":"Solid-state lithium metal batteries (LMBs) with high safety and energy density are the ultimate goal for energy storage systems. The bottleneck lies in the solid electrolytes, which must maintain perfect solid–solid contact and be electrochemically stable for both Li anode and high-voltage cathode. Here, we develop an in situ polymerized hetero-layered electrolyte that simultaneously broadens the electrochemical window and addresses interfacial issues between multiple components. The polyvinylidene fluoride (PVDF) layer toward the cathode improves high voltage compatibility to 4.8 V, while the boron nitride (BN) layer toward the anode provides sufficient mechanical strength, regulates Li-ions transport and promotes the formation of an inorganic-rich solid electrolyte interphase (SEI). The effect of the hetero-layered structure is then verified in an easy-to-process in situ polymerized poly(1,3-dioxane) (PDOL) electrolyte, that seamlessly integrates multiple interfaces, bridging cathode, PVDF, BN, and Li metal. This solid electrolyte is characterized by high room temperature (RT) ionic conductivity (2.1 × 10<sup>−3</sup> S<sup> </sup>cm<sup>−1</sup>), and high Li-ions transference number (0.801). Most importantly, the Li|LiNi<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub>(NCM622) full batteries show remarkable cycling performance with capacity retention of 90.3% over 200 cycles at 0.5 C. The hetero-layered structure with a seamless in situ polymerized interface provides a new avenue for high-energy, solid-state LMBs.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"64 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418388","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Dong Ma, Jingchun Hou, Guanxiang Zhang, Sen Meng, Runze Zhang, Jie Xiong, Weichen He, Xiao Zhang, Meirong Zhang, Zhicheng Zhang
To meet the increasing demands of modern power electronics for high-temperature resistance and energy storage performance and avoid the trade-off between high energy storage (Ue) performance and prominent processability, a strategy to modify polypropylene (PP) by introducing polar electron-deficient 8-hydroxyquinoline (8-HQ) physically during melt extrusion granulation is proposed. 8-HQ molecules are initially designed to capture charges injected under a high electric field and depress the leakage current density. Unexpectedly, they are found to reside at PP grain boundaries, promoting grain growth and thereby enhancing PP films' mechanical strength. Both effects may address the enhanced breakdown strength (Eb) up to 814 MV m−1. Besides, 8-HQ increases the permittivity of modified PP films. Due to simultaneously enhanced Eb and dielectric constant, an impressive Ue of 9.87 J cm−3 with a discharge efficiency above 90% is obtained in the optimal sample, and an Ue of 6.96 J cm−3 at 83% efficiency is well retained up to 125 °C, far exceeding the previously reported results. This study offers a novel strategy to modify PP film physically by manipulating its crystalline behavior for high-pulse energy storage capacitor applications.
{"title":"Significantly Enhancing the Energy-Storage Properties of Polypropylene Films by Physically Manipulating Their Permittivity and Crystalline Behavior with Polar Organic Molecules","authors":"Dong Ma, Jingchun Hou, Guanxiang Zhang, Sen Meng, Runze Zhang, Jie Xiong, Weichen He, Xiao Zhang, Meirong Zhang, Zhicheng Zhang","doi":"10.1002/adfm.202418631","DOIUrl":"https://doi.org/10.1002/adfm.202418631","url":null,"abstract":"To meet the increasing demands of modern power electronics for high-temperature resistance and energy storage performance and avoid the trade-off between high energy storage (<i>U</i><sub>e</sub>) performance and prominent processability, a strategy to modify polypropylene (PP) by introducing polar electron-deficient 8-hydroxyquinoline (8-HQ) physically during melt extrusion granulation is proposed. 8-HQ molecules are initially designed to capture charges injected under a high electric field and depress the leakage current density. Unexpectedly, they are found to reside at PP grain boundaries, promoting grain growth and thereby enhancing PP films' mechanical strength. Both effects may address the enhanced breakdown strength (<i>E</i><sub>b</sub>) up to 814 MV m<sup>−1</sup>. Besides, 8-HQ increases the permittivity of modified PP films. Due to simultaneously enhanced <i>E</i><sub>b</sub> and dielectric constant, an impressive <i>U</i><sub>e</sub> of 9.87 J cm<sup>−</sup><sup>3</sup> with a discharge efficiency above 90% is obtained in the optimal sample, and an <i>U</i><sub>e</sub> of 6.96 J cm<sup>−</sup><sup>3</sup> at 83% efficiency is well retained up to 125 °C, far exceeding the previously reported results. This study offers a novel strategy to modify PP film physically by manipulating its crystalline behavior for high-pulse energy storage capacitor applications.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"56 35 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418012","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jie Jiang, Miaomiao Tong, Di Shen, Zhijian Liang, Ziyun Li, Guirong Duan, Lei Wang, Honggang Fu
Tailoring the electronic structure of later transition metal-based electrocatalysts by incorporating early transition metal based on the electronic complementary effect is anticipated to enhance the electrocatalytic activity. Herein, the modulation of the electronic structure of Fe3C through the utilization of Mo2C to promote oxygen reduction reaction (ORR) activity is reported. In situ characterizations combined with theoretical calculations reveal that the electron-donating capability of molybdenum in Mo2C to the active center of iron in Fe3C optimizes the adsorption and activation of oxygen. Concurrently, the d-band center of Fe is much closer to the Fermi level, which reduces the energy barrier for the rate-determining step (*OOH → *O), thereby enhancing the ORR activity. In alkaline media, the catalyst delivers a half-wave potential (E1/2) of 0.89 V and maintains its efficiency with a mere 8 mV decay after 10 000 cycles, surpassing that of Pt/C. Moreover, it can serve as an air cathode in both liquid-state and all-solid-state zinc-air batteries (ZABs) and shows promising applications in portable devices. This work brings an innovative design concept for highly efficient electrocatalysts suitable for advanced energy devices.
{"title":"Utilizing Molybdenum to Tailor the Electronic Structure of Iron Through Electron Complementary Effect for Promoting Oxygen Reduction Activity","authors":"Jie Jiang, Miaomiao Tong, Di Shen, Zhijian Liang, Ziyun Li, Guirong Duan, Lei Wang, Honggang Fu","doi":"10.1002/adfm.202500065","DOIUrl":"https://doi.org/10.1002/adfm.202500065","url":null,"abstract":"Tailoring the electronic structure of later transition metal-based electrocatalysts by incorporating early transition metal based on the electronic complementary effect is anticipated to enhance the electrocatalytic activity. Herein, the modulation of the electronic structure of Fe<sub>3</sub>C through the utilization of Mo<sub>2</sub>C to promote oxygen reduction reaction (ORR) activity is reported. In situ characterizations combined with theoretical calculations reveal that the electron-donating capability of molybdenum in Mo<sub>2</sub>C to the active center of iron in Fe<sub>3</sub>C optimizes the adsorption and activation of oxygen. Concurrently, the d-band center of Fe is much closer to the Fermi level, which reduces the energy barrier for the rate-determining step (<sup>*</sup>OOH → <sup>*</sup>O), thereby enhancing the ORR activity. In alkaline media, the catalyst delivers a half-wave potential (<i>E</i><sub>1/2</sub>) of 0.89 V and maintains its efficiency with a mere 8 mV decay after 10 000 cycles, surpassing that of Pt/C. Moreover, it can serve as an air cathode in both liquid-state and all-solid-state zinc-air batteries (ZABs) and shows promising applications in portable devices. This work brings an innovative design concept for highly efficient electrocatalysts suitable for advanced energy devices.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"13 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418322","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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