Qingbing Xia, Cheng-Lin Ko, Emily R. Cooper, Qinfen Gu, Ruth Knibbe, Jeffrey R. Harmer
Sodium-ion batteries (SIBs) are a promising technology for advanced energy storage systems. Hard carbon (HC) is a commonly used SIB anode material; however, the Na ion storage mechanism in HC remains poorly understood and highly debated. Here, the paramagnetic species in HC during Na ion storage are systematically studied to elucidate the underlying mechanism at an electronic level using high-resolution electron paramagnetic resonance (EPR) spectroscopy, complemented by in situ Raman spectroscopy, in situ synchrotron X-ray diffraction, and density functional theory calculations. This investigation identifies and characterizes the coexistence of two distinct intercalation processes in HC: Na ion intercalation and Na+-solvent co-intercalation, which are active across both the sloping and plateau voltage regions. Additionally, in the sloping region, Na ions are also stored at in-plane Stone-Wales defect sites, which transition into a quasi-metallic state and subsequently to metallic Na as Na ion intercalation progresses. This transformation is driven by charge redistribution within the graphene layers. These insights establish a direct paramagnetic-electronic structure-electrochemical property relationship in HC, providing new insights into the Na ion storage mechanism. Furthermore, this study highlights the unique capability of EPR spectroscopy in elucidating the charge storage mechanism in electrode materials.
{"title":"Elucidating Sodium Ion Storage Mechanisms in Hard Carbon Anodes at the Electronic Level","authors":"Qingbing Xia, Cheng-Lin Ko, Emily R. Cooper, Qinfen Gu, Ruth Knibbe, Jeffrey R. Harmer","doi":"10.1002/adfm.202421976","DOIUrl":"https://doi.org/10.1002/adfm.202421976","url":null,"abstract":"Sodium-ion batteries (SIBs) are a promising technology for advanced energy storage systems. Hard carbon (HC) is a commonly used SIB anode material; however, the Na ion storage mechanism in HC remains poorly understood and highly debated. Here, the paramagnetic species in HC during Na ion storage are systematically studied to elucidate the underlying mechanism at an electronic level using high-resolution electron paramagnetic resonance (EPR) spectroscopy, complemented by in situ Raman spectroscopy, in situ synchrotron X-ray diffraction, and density functional theory calculations. This investigation identifies and characterizes the coexistence of two distinct intercalation processes in HC: Na ion intercalation and Na<sup>+</sup>-solvent co-intercalation, which are active across both the sloping and plateau voltage regions. Additionally, in the sloping region, Na ions are also stored at in-plane Stone-Wales defect sites, which transition into a quasi-metallic state and subsequently to metallic Na as Na ion intercalation progresses. This transformation is driven by charge redistribution within the graphene layers. These insights establish a direct paramagnetic-electronic structure-electrochemical property relationship in HC, providing new insights into the Na ion storage mechanism. Furthermore, this study highlights the unique capability of EPR spectroscopy in elucidating the charge storage mechanism in electrode materials.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"69 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435519","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}
Laigang Hu, Mengxue Zhang, Weiwei Wang, Jinru Hu, Wenhao Wu, Daohui Lin, Kun Yang
Developing large pore volume mesoporous metal-organic frameworks (MOFs) is a reliable strategy for adsorbing high-concentration benzene in the event of accidental leakage. Herein, a novel mesoporous Al-based MOF, named ZJU-928(Al), is synthesized using biphenyl-3,4′,5-tricarboxylic acid ligands and low toxic AlO6 cluster. It has larger pore volume (1.05 cm3 g−1), order hexagonal channel (32.10 Å), and higher specific surface area (2344 m2 g−1). As relative pressure up to 0.10, benzene adsorption of ZJU-928(Al) rises to 9.99 mmol g−1, exhibiting an excellent saturation benzene adsorption of 11.37 mmol g−1 at 298 K. The isosteric heat of adsorption for benzene on ZJU-928(Al) is only 24.52 kJ mol−1 at near-zero loading, lower than that of most reported MOFs, allowing for lower energy consumption during ZJU-928(Al) regeneration. ZJU-928(Al) has excellent cyclical benzene adsorption-desorption performance, and highest benzene diffusivity coefficient (2.65 × 10−5 cm2 s−1). Simulation shows that the excellent saturation benzene adsorption performance of ZJU-928(Al) can be attributed to the larger pore volume accommodating more benzene molecules. Consequently, this research synthesizes a novel mesoporous Al-based MOF with excellent saturation benzene adsorption, highlighting the potential of MOFs for high-concentration toxic gas adsorption.
{"title":"A Novel Mesoporous Aluminum-Based MOF with Large Pore Volume for High Concentration Benzene Adsorption","authors":"Laigang Hu, Mengxue Zhang, Weiwei Wang, Jinru Hu, Wenhao Wu, Daohui Lin, Kun Yang","doi":"10.1002/adfm.202425429","DOIUrl":"https://doi.org/10.1002/adfm.202425429","url":null,"abstract":"Developing large pore volume mesoporous metal-organic frameworks (MOFs) is a reliable strategy for adsorbing high-concentration benzene in the event of accidental leakage. Herein, a novel mesoporous Al-based MOF, named ZJU-928(Al), is synthesized using biphenyl-3,4′,5-tricarboxylic acid ligands and low toxic AlO<sub>6</sub> cluster. It has larger pore volume (1.05 cm<sup>3</sup> g<sup>−1</sup>), order hexagonal channel (32.10 Å), and higher specific surface area (2344 m<sup>2</sup> g<sup>−1</sup>). As relative pressure up to 0.10, benzene adsorption of ZJU-928(Al) rises to 9.99 mmol g<sup>−1</sup>, exhibiting an excellent saturation benzene adsorption of 11.37 mmol g<sup>−1</sup> at 298 K. The isosteric heat of adsorption for benzene on ZJU-928(Al) is only 24.52 kJ mol<sup>−1</sup> at near-zero loading, lower than that of most reported MOFs, allowing for lower energy consumption during ZJU-928(Al) regeneration. ZJU-928(Al) has excellent cyclical benzene adsorption-desorption performance, and highest benzene diffusivity coefficient (2.65 × 10<sup>−5</sup> cm<sup>2</sup> s<sup>−1</sup>). Simulation shows that the excellent saturation benzene adsorption performance of ZJU-928(Al) can be attributed to the larger pore volume accommodating more benzene molecules. Consequently, this research synthesizes a novel mesoporous Al-based MOF with excellent saturation benzene adsorption, highlighting the potential of MOFs for high-concentration toxic gas adsorption.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"112 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435520","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}
Xuning Zhang, Feixiang Tang, Bo Sun, Xingyue Liu, Guanglan Liao, Weihua Li, Sheng Liu
Perovskite-based image sensors are widely explored and recognized as the technology of choice for future optoelectronics. Suffering from the incompatibility between perovskite and conventional lithography technology, the challenges of developing high-resolution image sensors come from how to pattern the perovskite film with high precision and integrate it with pixel circuits. Recently, a four-mask technique for manufacturing perovskite-on-silicon sensor arrays, which are composed of a pixeled perovskite film and a planar crossbar circuit is demonstrated. Patterning precision for perovskite films attained 2 µm, ranking top among the previous research. The circuit is also proven to have the highest level of integration, theoretically. A proof-of-concept image sensor showing the first demonstration of monolithic integration of patterned perovskite film with the bottom pixel circuit is successfully made public. Electro-optical performance of its pixels is further characterized and showed high uniformity, benefitting the image sensor in capturing the input light distribution with good spatial resolution. This work has thus set a milestone for perovskite-based image sensors and showed the potential of perovskites in micro-nanoelectronics.
{"title":"Four-Mask Technique for Manufacturing the Perovskite-on-Silicon Sensor Array for Ultraviolet Light Imaging","authors":"Xuning Zhang, Feixiang Tang, Bo Sun, Xingyue Liu, Guanglan Liao, Weihua Li, Sheng Liu","doi":"10.1002/adfm.202423281","DOIUrl":"https://doi.org/10.1002/adfm.202423281","url":null,"abstract":"Perovskite-based image sensors are widely explored and recognized as the technology of choice for future optoelectronics. Suffering from the incompatibility between perovskite and conventional lithography technology, the challenges of developing high-resolution image sensors come from how to pattern the perovskite film with high precision and integrate it with pixel circuits. Recently, a four-mask technique for manufacturing perovskite-on-silicon sensor arrays, which are composed of a pixeled perovskite film and a planar crossbar circuit is demonstrated. Patterning precision for perovskite films attained 2 µm, ranking top among the previous research. The circuit is also proven to have the highest level of integration, theoretically. A proof-of-concept image sensor showing the first demonstration of monolithic integration of patterned perovskite film with the bottom pixel circuit is successfully made public. Electro-optical performance of its pixels is further characterized and showed high uniformity, benefitting the image sensor in capturing the input light distribution with good spatial resolution. This work has thus set a milestone for perovskite-based image sensors and showed the potential of perovskites in micro-nanoelectronics.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"29 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435556","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}
Designing highly stable anion exchange membranes (AEMs) is of vital importance for anion exchange membrane fuel cells (AEMFCs). Herein, the study presents that elevating current density and reducing relative humidity can dramatically lower local hydration number (λ) of the cathode in AEMFCs and therefore result in the rapid degradation of AEMs. To address this issue, a water-retention strategy has been proposed to alleviate the hydroxide attack. The crosslinked poly (aryl N-silanylmethyl-piperidinium) (Si-TP-100-x) AEMs are prepared to increase the amount of bound water on cations by introducing hydrophilic Si─O bonds, and thus improving the alkali stability under low λ conditions. The Si-TP-100-4 exhibits improved ex-situ stability than the benchmark AEM in 2 m KOH-MeOH solution (λ = 4) at 80 °C. The in situ cell tests demonstrate that the AEMFC with Si-TP-100-4 can achieve a high peak power density of 1.32 W cm−2 and simultaneously offer lower voltage decay rate than the controlled experiment at 1000 mA cm−2 at 95 °C. The post-mortem analysis of membrane-electrode assembly further reveals that membrane and ionomer in cathode concurrently suffer from a significant degradation. This work provides an avenue for developing highly stable anion exchange polymers from the perspective of cation hydration.
{"title":"Improving Alkali Stability of Anion Exchange Membrane by a Super Water-Retention Strategy","authors":"Zhiwei Ren, Yun Zhao, Yangkai Han, Tao Wei, Jiaqi Sun, Zhilin Jiao, Xinyi Liu, Haitao Zhang, Zhigang Shao","doi":"10.1002/adfm.202423460","DOIUrl":"https://doi.org/10.1002/adfm.202423460","url":null,"abstract":"Designing highly stable anion exchange membranes (AEMs) is of vital importance for anion exchange membrane fuel cells (AEMFCs). Herein, the study presents that elevating current density and reducing relative humidity can dramatically lower local hydration number (λ) of the cathode in AEMFCs and therefore result in the rapid degradation of AEMs. To address this issue, a water-retention strategy has been proposed to alleviate the hydroxide attack. The crosslinked poly (aryl N-silanylmethyl-piperidinium) (Si-TP-100-x) AEMs are prepared to increase the amount of bound water on cations by introducing hydrophilic Si─O bonds, and thus improving the alkali stability under low λ conditions. The Si-TP-100-4 exhibits improved ex-situ stability than the benchmark AEM in 2 <span>m</span> KOH-MeOH solution (λ = 4) at 80 °C. The in situ cell tests demonstrate that the AEMFC with Si-TP-100-4 can achieve a high peak power density of 1.32 W cm<sup>−2</sup> and simultaneously offer lower voltage decay rate than the controlled experiment at 1000 mA cm<sup>−2</sup> at 95 °C. The post-mortem analysis of membrane-electrode assembly further reveals that membrane and ionomer in cathode concurrently suffer from a significant degradation. This work provides an avenue for developing highly stable anion exchange polymers from the perspective of cation hydration.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"1 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435559","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}
2D MXenes are a rapidly expanding class of 2D materials with a broad spectrum of electrochemical applications, particularly in the electrochemical energy storage area. Concurrently, 3D and 4D printing techniques have garnered significant research attention offering customized designs, rapid prototyping, and cost-effective scalable production. Integrating MXene into the 3D/4D printed structures offers a promising path for the development of advanced electrochemical energy storage devices, with the combination of outstanding properties of MXene and the versatility of printing technology. The present article provides a comprehensive report on MXene printing technologies, focusing on their rheological characteristics, surface chemistry, ink formulation, stability, and storage. Different printing techniques, including 3D/4D printing, screen printing, inkjet printing, and continuous liquid interface production (CLIP) methods—are discussed in the context of MXene integration. Additionally, the application of printed MXene materials in electrochemical energy storage devices, such as supercapacitors and batteries, is explored along with future directions in evolving fields.
{"title":"MXene 3D/4D Printing: Ink Formulation and Electrochemical Energy Storage Applications","authors":"Shaista Nouseen, Martin Pumera","doi":"10.1002/adfm.202421987","DOIUrl":"https://doi.org/10.1002/adfm.202421987","url":null,"abstract":"2D MXenes are a rapidly expanding class of 2D materials with a broad spectrum of electrochemical applications, particularly in the electrochemical energy storage area. Concurrently, 3D and 4D printing techniques have garnered significant research attention offering customized designs, rapid prototyping, and cost-effective scalable production. Integrating MXene into the 3D/4D printed structures offers a promising path for the development of advanced electrochemical energy storage devices, with the combination of outstanding properties of MXene and the versatility of printing technology. The present article provides a comprehensive report on MXene printing technologies, focusing on their rheological characteristics, surface chemistry, ink formulation, stability, and storage. Different printing techniques, including 3D/4D printing, screen printing, inkjet printing, and continuous liquid interface production (CLIP) methods—are discussed in the context of MXene integration. Additionally, the application of printed MXene materials in electrochemical energy storage devices, such as supercapacitors and batteries, is explored along with future directions in evolving fields.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"10 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435561","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}
Potassium ion batteries (PIBs) are highly anticipated beside lithium-ion batteries (LIBs) owing to the abundant K resources, comparable standard electrode potential, and high theoretical capacity & high energy density, while the large radius of K+ ion usually results in the anode materials challenged by structural collapse, sluggish kinetics, and fast capacity decay. Herein, a composite with Cu9S5/NiS2 nanoparticle (≈15 nm) uniformly inlaid on hollow carbon-sphere (NCS) is designed, where the firmly anchored Cu9S5/NiS2 particle and sturdy carbon-sphere skeleton synergistically endow high structural-stability and satisfactory electron/ion accessibility for the NCS composite and inter-doping for Cu9S5/NiS2 from the introduction of highly conductive copper have further improved the conductivity of NCS composite for conversion reactions during potassiation/depotassiation. The structural features enable the NCS electrode to achieve a high capacity of ≈600 mAh g−1 even at a mass loading of 3.76 mg cm−2, stable cyclic performance for 1500 cycles, and fast electrochemical kinetics in half-cell, and the full-cell has also demonstrated a high capacity of ≈600 mAh g−1 and long-term cyclic performance for 550 cycles. The electrochemical mechanism has also been revealed experimentally and theoretically, providing an instructive strategy for the construction of highly stable and fast electrode materials for potassium ion storage.
{"title":"Carbon-Sphere Supported Cu9S5/NiS2 Involving Inter-Doping to Promote Fast and Stable Potassium Ion Storage","authors":"Lu Wang, Zhen Kong, Mamoor Muhammad, Bin Wang, Fengbo Wang, Zhongxin Jing, Guangmeng Qu, Xiaofan Yang, Jinkui Feng, Jianmin Dou, Yueyue Kong, Liqiang Xu","doi":"10.1002/adfm.202423524","DOIUrl":"https://doi.org/10.1002/adfm.202423524","url":null,"abstract":"Potassium ion batteries (PIBs) are highly anticipated beside lithium-ion batteries (LIBs) owing to the abundant K resources, comparable standard electrode potential, and high theoretical capacity & high energy density, while the large radius of K<sup>+</sup> ion usually results in the anode materials challenged by structural collapse, sluggish kinetics, and fast capacity decay. Herein, a composite with Cu<sub>9</sub>S<sub>5</sub>/NiS<sub>2</sub> nanoparticle (≈15 nm) uniformly inlaid on hollow carbon-sphere (NCS) is designed, where the firmly anchored Cu<sub>9</sub>S<sub>5</sub>/NiS<sub>2</sub> particle and sturdy carbon-sphere skeleton synergistically endow high structural-stability and satisfactory electron/ion accessibility for the NCS composite and inter-doping for Cu<sub>9</sub>S<sub>5</sub>/NiS<sub>2</sub> from the introduction of highly conductive copper have further improved the conductivity of NCS composite for conversion reactions during potassiation/depotassiation. The structural features enable the NCS electrode to achieve a high capacity of ≈600 mAh g<sup>−1</sup> even at a mass loading of 3.76 mg cm<sup>−2</sup>, stable cyclic performance for 1500 cycles, and fast electrochemical kinetics in half-cell, and the full-cell has also demonstrated a high capacity of ≈600 mAh g<sup>−1</sup> and long-term cyclic performance for 550 cycles. The electrochemical mechanism has also been revealed experimentally and theoretically, providing an instructive strategy for the construction of highly stable and fast electrode materials for potassium ion storage.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"13 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435518","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}
Jongdeuk Seo, Yun Seop Shin, Dong Gyu Lee, Jaehwi Lee, Jina Roe, Jung Geon Son, Woojin Lee, Yeonjeong Lee, Dongmin Lee, Ji Won Song, Tae Kyung Lee, Dong Suk Kim, Jin Young Kim
Long-term stability remains challenging due to persistent defects within the perovskite material, particularly at buried interfaces. Strategies to address these issues have focused on refining interfaces and managing residual lead iodide (PbI2), which impedes electron transport and compromises stability under prolonged light exposure. This study explores the impact of lead formate (PbFo2) treatment on SnO2 electron transporting layer (ETL) substrates and its subsequent influence on the performance of perovskite solar cells (PSCs). The carboxylate functionality of Fo− ions exerts multifaceted effects, influencing not only the electrical properties of the SnO2 ETL but also the morphological characteristics and crystallization mechanism of the overlying perovskite film. The ionized Fo− ions aid in forming bulk perovskite as intermediate phases during the perovskite crystallization. By stabilizing intermediate phases, their incorporation suppresses indiscriminate phase transitions from δ-phase to α-phase perovskite, ensuring the production of highly crystalline pure α-phase perovskite with alleviated tensile strain throughout the perovskite film, particularly near the buried interface. Consequently, the strategy showcases enhanced performance with a power conversion efficiency (PCE) of 25.69% and enables a refined buried interface, devoid of residual PbI2, ensuring long-term stability under continuous light-soaking for 1,000 h. Overall, PbFo2 treatment stands as a pioneering approach poised to expedite commercialization.
{"title":"Stabilized Intermediate Phase Via Pseudo-Halide Anions Toward Highly Efficient and Light-Soaking Stable Perovskite Solar Cells","authors":"Jongdeuk Seo, Yun Seop Shin, Dong Gyu Lee, Jaehwi Lee, Jina Roe, Jung Geon Son, Woojin Lee, Yeonjeong Lee, Dongmin Lee, Ji Won Song, Tae Kyung Lee, Dong Suk Kim, Jin Young Kim","doi":"10.1002/adfm.202413390","DOIUrl":"https://doi.org/10.1002/adfm.202413390","url":null,"abstract":"Long-term stability remains challenging due to persistent defects within the perovskite material, particularly at buried interfaces. Strategies to address these issues have focused on refining interfaces and managing residual lead iodide (PbI<sub>2</sub>), which impedes electron transport and compromises stability under prolonged light exposure. This study explores the impact of lead formate (PbFo<sub>2</sub>) treatment on SnO<sub>2</sub> electron transporting layer (ETL) substrates and its subsequent influence on the performance of perovskite solar cells (PSCs). The carboxylate functionality of Fo<sup>−</sup> ions exerts multifaceted effects, influencing not only the electrical properties of the SnO<sub>2</sub> ETL but also the morphological characteristics and crystallization mechanism of the overlying perovskite film. The ionized Fo<sup>−</sup> ions aid in forming bulk perovskite as intermediate phases during the perovskite crystallization. By stabilizing intermediate phases, their incorporation suppresses indiscriminate phase transitions from <i>δ</i>-phase to <i>α</i>-phase perovskite, ensuring the production of highly crystalline pure <i>α</i>-phase perovskite with alleviated tensile strain throughout the perovskite film, particularly near the buried interface. Consequently, the strategy showcases enhanced performance with a power conversion efficiency (PCE) of 25.69% and enables a refined buried interface, devoid of residual PbI<sub>2</sub>, ensuring long-term stability under continuous light-soaking for 1,000 h. Overall, PbFo<sub>2</sub> treatment stands as a pioneering approach poised to expedite commercialization.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"70 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435523","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}
Xin Li, Yu Bai, Jiaxin Jing, Tao Ren, Zhenhua Wang, Jianmin Ma, Kening Sun
Lithium metal batteries (LMBs) operating at high voltages are attractive for their energy storage capacity but suffer from challenges: cathode instability, electrolyte consumption, and lithium dendrite growth. Modulating the electrode/electrolyte interphase (EEI) with functional additives is a practical strategy. Herein, a cyano (-CN)-functionalized hybrid EEI strategy is proposed to develop electrolytes for high-voltage Li||LiNi0.8Co0.1Mn0.1O2 (Li||NCM811) battery with -CN-substituted tetrafluorobenzene derivatives (tetrafluorophthalonitrile (o-TFPN), tetrafluoroisophthalonitrile (m-TFPN)), and tetrafluoroterephthalonitrile (p-TFPN)) as additives. The results demonstrate that the electrolyte-containing additives, particularly o-TFPN-contained electrolyte, can derive a robust, and thermally stable cathode electrolyte interphase (CEI) enriched with LiF and -CN groups. Furthermore, the o-TFPN-contained electrolyte forms a stable solid electrolyte interface (SEI) with Li2O, LiF, and -CN. The -CN group generates electrostatic attraction, guiding Li+ flux, while LiF and Li2O with high ionic conductivity facilitate rapid Li+ deposition. The excellent EEI suppresses cathode degradation, electrolyte consumption, and dendrite formation. Therefore, the Li||NCM811 battery achieves stable performance over 200 cycles at 4.6 V, while the Li||Li symmetric cell stably cycles for over 350 h at a current density of 1 mA cm−2.
{"title":"Cyano-Functionalized Hybrid Electrode-Electrolyte Interphases Enabled by Cyano-Substituted Tetrafluorobenzene Derivatives Additives for High-Voltage Lithium Metal Batteries","authors":"Xin Li, Yu Bai, Jiaxin Jing, Tao Ren, Zhenhua Wang, Jianmin Ma, Kening Sun","doi":"10.1002/adfm.202421329","DOIUrl":"https://doi.org/10.1002/adfm.202421329","url":null,"abstract":"Lithium metal batteries (LMBs) operating at high voltages are attractive for their energy storage capacity but suffer from challenges: cathode instability, electrolyte consumption, and lithium dendrite growth. Modulating the electrode/electrolyte interphase (EEI) with functional additives is a practical strategy. Herein, a cyano (-CN)-functionalized hybrid EEI strategy is proposed to develop electrolytes for high-voltage Li||LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (Li||NCM811) battery with -CN-substituted tetrafluorobenzene derivatives (tetrafluorophthalonitrile (o-TFPN), tetrafluoroisophthalonitrile (m-TFPN)), and tetrafluoroterephthalonitrile (p-TFPN)) as additives. The results demonstrate that the electrolyte-containing additives, particularly o-TFPN-contained electrolyte, can derive a robust, and thermally stable cathode electrolyte interphase (CEI) enriched with LiF and -CN groups. Furthermore, the o-TFPN-contained electrolyte forms a stable solid electrolyte interface (SEI) with Li<sub>2</sub>O, LiF, and -CN. The -CN group generates electrostatic attraction, guiding Li<sup>+</sup> flux, while LiF and Li<sub>2</sub>O with high ionic conductivity facilitate rapid Li<sup>+</sup> deposition. The excellent EEI suppresses cathode degradation, electrolyte consumption, and dendrite formation. Therefore, the Li||NCM811 battery achieves stable performance over 200 cycles at 4.6 V, while the Li||Li symmetric cell stably cycles for over 350 h at a current density of 1 mA cm<sup>−2</sup>.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"28 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435521","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 piezomagnetic effect driven by magnetic-strain coupling effectively generates and controls magnetization, making it pivotal for antiferromagnetic spintronics, a rapidly growing research field. However, the practical application of piezomagnetism to realize a large and stable piezomagnetic response over a wide temperature range remains a significant challenge due to the limited efficiency of magnetic-strain coupling and thermal failure at room-temperature. Here, the giant piezomagnetic effect in frustrated antiferromagnetic Mn₃Ir is reported for the first time, characterized by superior thermal stability and an exceptionally high Néel temperature of 950 K. The piezomagnetic coefficient of Mn3Ir reaches 0.55 µB f.u.−1 (1%), exceeding those of conventional antiferromagnetic piezomagnetic materials by an order of magnitude. Moreover, the direction of the piezomagnetic moment can be efficiently manipulated by the driving strain. The piezomagnetic effect, stable over a wide temperature range from 75 to 553 K, is attributed to a synergistic compensatory effect between the strains arising from lattice mismatch and temperature variation. These results provide a new paradigm for achieving thermally stable piezomagnetism and effectively manipulating antiferromagnetic states in variable-temperature environments, thereby advancing spin manipulation in antiferromagnetic piezospintronics.
{"title":"Superior Thermally Stable Giant Piezomagnetism in Spin Frustrated Mn3Ir","authors":"Kaiqi Zhang, Zhijie Ma, Ying Sun, Kewen Shi, Yuyan Wang, Qisong Sun, YongJie Li, Sihao Deng, Jin Cui, Zhengcai Xia, Weisheng Zhao, Cong Wang","doi":"10.1002/adfm.202424472","DOIUrl":"https://doi.org/10.1002/adfm.202424472","url":null,"abstract":"The piezomagnetic effect driven by magnetic-strain coupling effectively generates and controls magnetization, making it pivotal for antiferromagnetic spintronics, a rapidly growing research field. However, the practical application of piezomagnetism to realize a large and stable piezomagnetic response over a wide temperature range remains a significant challenge due to the limited efficiency of magnetic-strain coupling and thermal failure at room-temperature. Here, the giant piezomagnetic effect in frustrated antiferromagnetic Mn₃Ir is reported for the first time, characterized by superior thermal stability and an exceptionally high Néel temperature of 950 K. The piezomagnetic coefficient of Mn<sub>3</sub>Ir reaches 0.55 <i>µ</i><sub>B</sub> f.u.<sup>−1</sup> (1%), exceeding those of conventional antiferromagnetic piezomagnetic materials by an order of magnitude. Moreover, the direction of the piezomagnetic moment can be efficiently manipulated by the driving strain. The piezomagnetic effect, stable over a wide temperature range from 75 to 553 K, is attributed to a synergistic compensatory effect between the strains arising from lattice mismatch and temperature variation. These results provide a new paradigm for achieving thermally stable piezomagnetism and effectively manipulating antiferromagnetic states in variable-temperature environments, thereby advancing spin manipulation in antiferromagnetic piezospintronics.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"85 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435524","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}
Perovskite solar cells (PSCs) have gained significant attention for their high efficiency, low cost, and versatile application possibilities, which are expected to play a critical role in shaping the future of photovoltaics (PV) markets. However, the power conversion efficiency (PCE) and stability of large-area PSCs still cannot meet the industrialization requirements, which are mainly associated with the unsatisfactory quality of large-area perovskite films. This review first identifies the factors contributing to the film quality difference between small-area and large-area perovskite films, such as the solvent evaporation process, reaction and crystallization kinetics, etc. This results in undesired film quality for large-area perovskites, e.g. film inhomogeneity in terms of morphology, composition, phase, crystal size, and orientation. Solvent systems are customed for different scalable preparation process based on their volatility, solubility, and coordination ability with perovskite. Furthermore, various additives are incorporated to further regulate surface tension change and intermediate phase evolution. Finally, we transition from the perovskite film level to the device level to explore the current advancements and challenges related to PCE and stability in the commercialization process.
{"title":"Fabricating Perovskite Films for Solar Modules from Small to Large Scale","authors":"Ruiyang Yin, Yuetong Wu, Zijian Huang, Andrey S. Vasenko, Shuoyang Xu, Huanping Zhou","doi":"10.1002/adfm.202419184","DOIUrl":"https://doi.org/10.1002/adfm.202419184","url":null,"abstract":"Perovskite solar cells (PSCs) have gained significant attention for their high efficiency, low cost, and versatile application possibilities, which are expected to play a critical role in shaping the future of photovoltaics (PV) markets. However, the power conversion efficiency (PCE) and stability of large-area PSCs still cannot meet the industrialization requirements, which are mainly associated with the unsatisfactory quality of large-area perovskite films. This review first identifies the factors contributing to the film quality difference between small-area and large-area perovskite films, such as the solvent evaporation process, reaction and crystallization kinetics, etc. This results in undesired film quality for large-area perovskites, e.g. film inhomogeneity in terms of morphology, composition, phase, crystal size, and orientation. Solvent systems are customed for different scalable preparation process based on their volatility, solubility, and coordination ability with perovskite. Furthermore, various additives are incorporated to further regulate surface tension change and intermediate phase evolution. Finally, we transition from the perovskite film level to the device level to explore the current advancements and challenges related to PCE and stability in the commercialization process.","PeriodicalId":112,"journal":{"name":"Advanced Functional Materials","volume":"1 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435554","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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