Ji Won Song, Yun Seop Shin, Minjin Kim, Jaehwi Lee, Dongmin Lee, Jongdeuk Seo, YeonJeong Lee, Woosuk Lee, Hak-Beom Kim, Sung-In Mo, Jeong-Ho An, Ji-Eun Hong, Jin Young Kim, Il Jeon, Yimhyun Jo, Dong Suk Kim
The prominent chemical bath deposition (CBD) method leverages tin dioxide (SnO2) as an electron transport layer (ETL) in perovskite solar cells (PSCs), achieving exceptional efficiency. The deposition of SnO2, however, can lead to the formation of oxygen vacancies and surface defects, which subsequently contribute to performance challenges such as hysteresis and instability under light-soaking conditions. To alleviate these issues, it is crucial to address heterointerface defects and ensure the uniform coverage of SnO2 on fluorine-doped tin oxide substrates. Herein, the efficacy of tin(IV) chloride (SnCl4) post-treatment in enhancing the properties of the SnO2-ETL and the performances of PSCs are presented. The treatment with SnCl4 not only removes undesired agglomerated SnO2 nanoparticles from the surface of CBD SnO2 but also improves its crystallinity through a recrystallization process. This leads to an optimized interface between the SnO2-ETL and perovskite, effectively minimizing defects while promoting efficient electron transport. The resultant PSCs demonstrate improved performance, achieving an efficiency of 25.56% (certified with 24.92%), while retaining 95.84% of the initial PCE under ambient storage conditions. Additionally, PSCs treated with SnCl4 endure prolonged light-soaking tests, particularly when subjected to quasi-steady-state-IV measurements. This highlights the potential of SnCl4 treatment as a promising strategy for advancing PSC technology.
{"title":"Post-Treated Polycrystalline SnO2 in Perovskite Solar Cells for High Efficiency and Quasi-Steady-State-IV Stability","authors":"Ji Won Song, Yun Seop Shin, Minjin Kim, Jaehwi Lee, Dongmin Lee, Jongdeuk Seo, YeonJeong Lee, Woosuk Lee, Hak-Beom Kim, Sung-In Mo, Jeong-Ho An, Ji-Eun Hong, Jin Young Kim, Il Jeon, Yimhyun Jo, Dong Suk Kim","doi":"10.1002/aenm.202401753","DOIUrl":"https://doi.org/10.1002/aenm.202401753","url":null,"abstract":"The prominent chemical bath deposition (CBD) method leverages tin dioxide (SnO<sub>2</sub>) as an electron transport layer (ETL) in perovskite solar cells (PSCs), achieving exceptional efficiency. The deposition of SnO<sub>2</sub>, however, can lead to the formation of oxygen vacancies and surface defects, which subsequently contribute to performance challenges such as hysteresis and instability under light-soaking conditions. To alleviate these issues, it is crucial to address heterointerface defects and ensure the uniform coverage of SnO<sub>2</sub> on fluorine-doped tin oxide substrates. Herein, the efficacy of tin(IV) chloride (SnCl<sub>4</sub>) post-treatment in enhancing the properties of the SnO<sub>2</sub>-ETL and the performances of PSCs are presented. The treatment with SnCl<sub>4</sub> not only removes undesired agglomerated SnO<sub>2</sub> nanoparticles from the surface of CBD SnO<sub>2</sub> but also improves its crystallinity through a recrystallization process. This leads to an optimized interface between the SnO<sub>2</sub>-ETL and perovskite, effectively minimizing defects while promoting efficient electron transport. The resultant PSCs demonstrate improved performance, achieving an efficiency of 25.56% (certified with 24.92%), while retaining 95.84% of the initial PCE under ambient storage conditions. Additionally, PSCs treated with SnCl<sub>4</sub> endure prolonged light-soaking tests, particularly when subjected to quasi-steady-state-IV measurements. This highlights the potential of SnCl<sub>4</sub> treatment as a promising strategy for advancing PSC technology.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141495934","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}
Yingying Yin, Pengcheng Sun, Yijun Zeng, Meng Yang, Shouwei Gao, Steven Wang, Zhengyong Huang, Yingfan Zhang, Yang Wang, Zuankai Wang
Achieving year-round energy savings in buildings holds great significance toward reaching carbon neutrality and sustainability. Switchable thermal-management materials offer an energy-free solution to dynamically regulating internal building temperatures, by passively emitting heat into cold outer space in summer, and absorbing heat from hot sunlight in winter. In addition to dynamic thermal regulation, color display is another pursuit for addressing aesthetic considerations; however, most current dynamically switchable materials lack color options, due to an optical conflict between adaptive solar reflection and selective visible absorption, limiting their wide adoption in aesthetic scenarios such as commercial exterior walls. Herein, a colored temperature-adaptive cloak (CTAC) that achieves dynamically switchable thermal management in an energy-neutral way without sacrificing year-round vibrant color display is reported. This is realized by decoupling solar reflectivity modulation and color display through the choice of two individual constituent components, including thermochromic microcapsules, and fluorescent dyes. Moreover, compared to single-mode samples with similar colors, the CTAC with dual modes stays 5.6–3.4 °C warmer during cold winter and 14.9–7.9 °C cooler during hot summer (peak solar irradiance: ≈735 and 1030 W m−2, respectively), exhibiting a remarkable potential to achieve year-round building energy savings.
在建筑物中实现全年节能对于实现碳中和与可持续发展具有重要意义。可切换热管理材料为动态调节建筑物内部温度提供了一种无能耗的解决方案，它在夏季被动地向寒冷的外部空间散发热量，在冬季从炎热的阳光中吸收热量。除了动态热调节外，色彩显示也是解决美学问题的另一种追求；然而，由于自适应太阳反射和选择性可见光吸收之间存在光学冲突，目前大多数动态可切换材料都缺乏色彩选择，这限制了它们在商业外墙等美学场景中的广泛应用。本文报告了一种彩色温度自适应斗篷（CTAC），它能以能源中性的方式实现动态可切换热管理，同时不影响全年鲜艳的色彩显示。通过选择热致变色微胶囊和荧光染料这两种独立的组成成分，实现了太阳能反射率调节和色彩显示的解耦。此外，与具有相似颜色的单模式样品相比，具有双模式的 CTAC 在寒冷的冬季可保持 5.6-3.4°C 的温度，在炎热的夏季可保持 14.9-7.9°C 的温度（峰值太阳辐照度分别为：≈735 W m-2 和 1030 W m-2），在实现全年建筑节能方面具有显著的潜力。
{"title":"A Colored Temperature-Adaptive Cloak for Year-Round Building Energy Saving","authors":"Yingying Yin, Pengcheng Sun, Yijun Zeng, Meng Yang, Shouwei Gao, Steven Wang, Zhengyong Huang, Yingfan Zhang, Yang Wang, Zuankai Wang","doi":"10.1002/aenm.202402202","DOIUrl":"https://doi.org/10.1002/aenm.202402202","url":null,"abstract":"Achieving year-round energy savings in buildings holds great significance toward reaching carbon neutrality and sustainability. Switchable thermal-management materials offer an energy-free solution to dynamically regulating internal building temperatures, by passively emitting heat into cold outer space in summer, and absorbing heat from hot sunlight in winter. In addition to dynamic thermal regulation, color display is another pursuit for addressing aesthetic considerations; however, most current dynamically switchable materials lack color options, due to an optical conflict between adaptive solar reflection and selective visible absorption, limiting their wide adoption in aesthetic scenarios such as commercial exterior walls. Herein, a colored temperature-adaptive cloak (CTAC) that achieves dynamically switchable thermal management in an energy-neutral way without sacrificing year-round vibrant color display is reported. This is realized by decoupling solar reflectivity modulation and color display through the choice of two individual constituent components, including thermochromic microcapsules, and fluorescent dyes. Moreover, compared to single-mode samples with similar colors, the CTAC with dual modes stays 5.6–3.4 °C warmer during cold winter and 14.9–7.9 °C cooler during hot summer (peak solar irradiance: ≈735 and 1030 W m<sup>−2</sup>, respectively), exhibiting a remarkable potential to achieve year-round building energy savings.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141489793","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}
Xiaoying Xiong, Shuo Wan, Bin Hu, Yi Li, Yunlong Ma, Guanghao Lu, Huiting Fu, Qingdong Zheng
M-series molecules are one kind of promising acceptor-donor-acceptor (A-D-A)-type acceptors for constructing high-performance organic solar cells (OSCs). However, their power conversion efficiencies (PCEs) are lagging behind that of current state-of-the-art OSCs, limited by the relatively low fill factor (FF) and photocurrent. Herein, combined strategies of layer-by-layer (LBL) deposition and interface engineering are conducted to systematically improve light utilization and thus PCEs for M36-based OSCs. Through choosing a proper processing solvent, a PCE of 17.3% with an FF of 77.9% is achieved for the resulting LBL devices, much higher than those (15.9%/74.0%) from the blend-casting devices. The improvement is assigned to the favorable morphological evolution that facilitates carrier generation and transport as well as reduces charge recombination. More importantly, light-harvesting of the active layers can be enhanced upon employing a self-assembled monolayer of (2-(9H-carbazol-9-yl)ethyl)phosphonic acid (2PACz) instead of the widely used PEDOT:PSS as the hole-selecting layer, due to the decreased parasitic absorption of the former. Consequently, 2PACz-based LBL devices exhibit significantly increased photocurrent, affording a PCE up to 18.2%, which is the highest among the reported A-D-A-type acceptor-based OSCs. These results deliver important strategies to enhance the performance of OSCs and thus highlight the great potential of M-series acceptors for practical applications.
{"title":"Realizing over 18% Efficiency for M-Series Acceptor-Based Polymer Solar Cells by Improving Light Utilization","authors":"Xiaoying Xiong, Shuo Wan, Bin Hu, Yi Li, Yunlong Ma, Guanghao Lu, Huiting Fu, Qingdong Zheng","doi":"10.1002/aenm.202401816","DOIUrl":"https://doi.org/10.1002/aenm.202401816","url":null,"abstract":"M-series molecules are one kind of promising acceptor-donor-acceptor (A-D-A)-type acceptors for constructing high-performance organic solar cells (OSCs). However, their power conversion efficiencies (PCEs) are lagging behind that of current state-of-the-art OSCs, limited by the relatively low fill factor (FF) and photocurrent. Herein, combined strategies of layer-by-layer (LBL) deposition and interface engineering are conducted to systematically improve light utilization and thus PCEs for M36-based OSCs. Through choosing a proper processing solvent, a PCE of 17.3% with an FF of 77.9% is achieved for the resulting LBL devices, much higher than those (15.9%/74.0%) from the blend-casting devices. The improvement is assigned to the favorable morphological evolution that facilitates carrier generation and transport as well as reduces charge recombination. More importantly, light-harvesting of the active layers can be enhanced upon employing a self-assembled monolayer of (2-(9H-carbazol-9-yl)ethyl)phosphonic acid (2PACz) instead of the widely used PEDOT:PSS as the hole-selecting layer, due to the decreased parasitic absorption of the former. Consequently, 2PACz-based LBL devices exhibit significantly increased photocurrent, affording a PCE up to 18.2%, which is the highest among the reported A-D-A-type acceptor-based OSCs. These results deliver important strategies to enhance the performance of OSCs and thus highlight the great potential of M-series acceptors for practical applications.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-07-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141489699","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}
Gyuleen Park, Sujin Kim, Jisub Kim, Sangjin Bae, Youngjun Heo, Dongmin Park, Heemin Kim, Juhun Shin, Jongseok Moon, Jang Wook Choi
A pressing need for high‐capacity anode materials beyond graphite is evident, aiming to enhance the energy density of Li‐ion batteries (LIBs). A Li‐ion/Li metal hybrid anode holds remarkable potential for high energy density through additional Li plating, while benefiting from graphite's stable intercalation chemistry. However, limited comprehension of the hybrid anode has led to improper utilization of both chemistries, causing their degradation. Herein, this study reports an effective hybrid anode design considering material properties, the ratio of intercalation‐to‐plating capacity, and Li‐ion transport phenomena on the surface. Mesocarbon microbeads (MCMB) possesses desirable properties for additional Li plating based on its spherical shape, lithiophilic functional group, and sufficient interparticle space, alongside stable intercalation‐based storage capability. Balancing the ratio of intercalation‐to‐plating capacity is also crucial, as excessive Li plating occurs on the top surface of the anode, eventually deactivating the intercalation chemistry by obstructing upper pores. To address this issue, electrospun polyvinylidene fluoride (PVDF) is introduced to prevent Li metal accumulation on the upper surface, leveraging its non‐conductive, polar nature, and high dielectric constant. By implementing these strategies, a LiNi0.8Co0.15Al0.05O2 (NCA)‐paired pouch cell delivers an outstanding energy density of 1101.0 Wh L−1, highlighting its potential as an advanced post‐LIBs with practical feasibility.
{"title":"Understanding and Strategies for High Energy Density Lithium‐Ion/Lithium Metal Hybrid Batteries","authors":"Gyuleen Park, Sujin Kim, Jisub Kim, Sangjin Bae, Youngjun Heo, Dongmin Park, Heemin Kim, Juhun Shin, Jongseok Moon, Jang Wook Choi","doi":"10.1002/aenm.202401289","DOIUrl":"https://doi.org/10.1002/aenm.202401289","url":null,"abstract":"A pressing need for high‐capacity anode materials beyond graphite is evident, aiming to enhance the energy density of Li‐ion batteries (LIBs). A Li‐ion/Li metal hybrid anode holds remarkable potential for high energy density through additional Li plating, while benefiting from graphite's stable intercalation chemistry. However, limited comprehension of the hybrid anode has led to improper utilization of both chemistries, causing their degradation. Herein, this study reports an effective hybrid anode design considering material properties, the ratio of intercalation‐to‐plating capacity, and Li‐ion transport phenomena on the surface. Mesocarbon microbeads (MCMB) possesses desirable properties for additional Li plating based on its spherical shape, lithiophilic functional group, and sufficient interparticle space, alongside stable intercalation‐based storage capability. Balancing the ratio of intercalation‐to‐plating capacity is also crucial, as excessive Li plating occurs on the top surface of the anode, eventually deactivating the intercalation chemistry by obstructing upper pores. To address this issue, electrospun polyvinylidene fluoride (PVDF) is introduced to prevent Li metal accumulation on the upper surface, leveraging its non‐conductive, polar nature, and high dielectric constant. By implementing these strategies, a LiNi<jats:sub>0.8</jats:sub>Co<jats:sub>0.15</jats:sub>Al<jats:sub>0.05</jats:sub>O<jats:sub>2</jats:sub> (NCA)‐paired pouch cell delivers an outstanding energy density of 1101.0 Wh L<jats:sup>−1</jats:sup>, highlighting its potential as an advanced post‐LIBs with practical feasibility.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141489179","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}
Christian Wölke, Anass Benayad, Thanh‐Loan Lai, Felix Hanke, Giorgio Baraldi, María Echeverría, Ekin Esen, Elixabete Ayerbe, Alex R. Neale, Jacqui Everitt, Laurence J. Hardwick, Peng Yan, Marcin Poterała, Władysław Wieczorek, Martin Winter, Isidora Cekic‐Laskovic
Lithium nickel oxide (LNO) is an attractive positive electrode active material for lithium ion batteries (LIBs) due to its high reversible specific capacity and absence of cobalt. Nevertheless, it is prone to structural instabilities that lead to rapid capacity fading, safety concerns and shows in average a lower voltage than mixtures with cobalt, limiting its applicability to date. Herein this study introduces the sulfur‐based electrolyte additive, benzo[d][1,3,2]dioxathiole 2,2‐dioxide (DTDPh), to stabilize the LNO electrode and study its effects on interphase compositions by means of complementary electrochemical and spectroscopic techniques. Obtained results demonstrate an improved galvanostatic cycling performance in terms of cycle life and achievable specific discharge capacity that significantly outperform the common film‐forming additive vinylene carbonate (VC). The cycle life is increased from 102 to 147 cycles compared to the baseline electrolyte and the accumulated discharge energy until end of life is increased by 45%. This study furthermore provides strong evidence of a significant cross‐talk and negative interplay between DTDPh and VC when both are present in the electrolyte formulation. Mechanistic consideration based on density functional theory (DFT) calculations suggest the formation of mobile poly(VC) species, which is supported by the results of post mortem analysis of the resulting interphases.
{"title":"Single Versus Blended Electrolyte Additives: Impact of a Sulfur‐Based Electrolyte Additive on Electrode Cross‐Talk and Electrochemical Performance of LiNiO2||Graphite Cells","authors":"Christian Wölke, Anass Benayad, Thanh‐Loan Lai, Felix Hanke, Giorgio Baraldi, María Echeverría, Ekin Esen, Elixabete Ayerbe, Alex R. Neale, Jacqui Everitt, Laurence J. Hardwick, Peng Yan, Marcin Poterała, Władysław Wieczorek, Martin Winter, Isidora Cekic‐Laskovic","doi":"10.1002/aenm.202402152","DOIUrl":"https://doi.org/10.1002/aenm.202402152","url":null,"abstract":"Lithium nickel oxide (LNO) is an attractive positive electrode active material for lithium ion batteries (LIBs) due to its high reversible specific capacity and absence of cobalt. Nevertheless, it is prone to structural instabilities that lead to rapid capacity fading, safety concerns and shows in average a lower voltage than mixtures with cobalt, limiting its applicability to date. Herein this study introduces the sulfur‐based electrolyte additive, benzo[<jats:italic>d</jats:italic>][1,3,2]dioxathiole 2,2‐dioxide (DTDPh), to stabilize the LNO electrode and study its effects on interphase compositions by means of complementary electrochemical and spectroscopic techniques. Obtained results demonstrate an improved galvanostatic cycling performance in terms of cycle life and achievable specific discharge capacity that significantly outperform the common film‐forming additive vinylene carbonate (VC). The cycle life is increased from 102 to 147 cycles compared to the baseline electrolyte and the accumulated discharge energy until end of life is increased by 45%. This study furthermore provides strong evidence of a significant cross‐talk and negative interplay between DTDPh and VC when both are present in the electrolyte formulation. Mechanistic consideration based on density functional theory (DFT) calculations suggest the formation of mobile poly(VC) species, which is supported by the results of <jats:italic>post mortem</jats:italic> analysis of the resulting interphases.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141489269","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}
Shan Wang, Jiarui Yang, Wenrui Cai, Guojiang Wen, Sifan Yang, Kai Ke, Bo Yin, Xuewei Fu, Wei Yang, Yu Wang
Achieving precisely defined and stable component binding is of great interest for composite materials and batteries, but very challenging owing to the lack of effective strategies to manipulate the binder itself. Here, a concept of single‐particle binding (SPB) strategy is proposed based on a polymer‐sol binder to conquer the above challenge. To do that, a polymer‐sol binder is first prepared by dispersing commercial poly(vinylidene fluoride) (PVDF) powder into a mixture of its solvent and non‐solvent with a rational weight ratio of 8:2. Then, by manipulating this PVDF‐sol microfluid, PVDF particles are uniformly and singly introduced onto the surface of other components, such as graphene oxide nanosheets and battery separators. Results further show that the temperature‐induced sol–gel transition of the microfluid finally generates single‐particle fusion and strong component binding with commercial separators (31.6 N m−1). Meanwhile, a surface‐swelling model is proposed to understand its binding mechanism. Finally, this unique SPB strategy has been employed to fabricate nacre‐like nanocomposites with advanced self‐polarized piezoelectricity (23.0 mV N−1), and component‐integrated batteries with robust separator/electrode interphases. This SPB strategy with the PVDF‐sol binder may inspire significant studies on polymer sol, microfluidics, nanocomposites, battery interfaces and beyond.
{"title":"A Polymer‐Sol Binder Realizes Single‐Particle Binding for Nacre‐Like Piezoelectric Nanocomposites and Component‐Integrated Batteries","authors":"Shan Wang, Jiarui Yang, Wenrui Cai, Guojiang Wen, Sifan Yang, Kai Ke, Bo Yin, Xuewei Fu, Wei Yang, Yu Wang","doi":"10.1002/aenm.202401937","DOIUrl":"https://doi.org/10.1002/aenm.202401937","url":null,"abstract":"Achieving precisely defined and stable component binding is of great interest for composite materials and batteries, but very challenging owing to the lack of effective strategies to manipulate the binder itself. Here, a concept of single‐particle binding (SPB) strategy is proposed based on a polymer‐sol binder to conquer the above challenge. To do that, a polymer‐sol binder is first prepared by dispersing commercial poly(vinylidene fluoride) (PVDF) powder into a mixture of its solvent and non‐solvent with a rational weight ratio of 8:2. Then, by manipulating this PVDF‐sol microfluid, PVDF particles are uniformly and singly introduced onto the surface of other components, such as graphene oxide nanosheets and battery separators. Results further show that the temperature‐induced sol–gel transition of the microfluid finally generates single‐particle fusion and strong component binding with commercial separators (31.6 N m<jats:sup>−1</jats:sup>). Meanwhile, a surface‐swelling model is proposed to understand its binding mechanism. Finally, this unique SPB strategy has been employed to fabricate nacre‐like nanocomposites with advanced self‐polarized piezoelectricity (23.0 mV N<jats:sup>−1</jats:sup>), and component‐integrated batteries with robust separator/electrode interphases. This SPB strategy with the PVDF‐sol binder may inspire significant studies on polymer sol, microfluidics, nanocomposites, battery interfaces and beyond.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141489240","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}
Shu Zhang, Zhuo Yang, Yong Lu, Weiwei Xie, Zhenhua Yan, Jun Chen
Cathode materials are the core components of lithium-ion batteries owing to the determination of the practical voltage and effective energy of the battery system. However, advanced cathodes have faced challenges related to cation migration and cation intermixing. In this review, the study summarizes the structural failure mechanisms due to the cation mixing of advanced cathodes, including Ni-rich and Li-rich layered cathodes, spinel, olivine, and disordered rock-salt materials. This review starts by discussing the structural degradation mechanisms caused by cation intermixing in different cathodes, focusing on the electronic structure, crystal structure, and electrode structure. Furthermore, the optimization strategies for effective inhibition of cation migration and rational utilization of cation mixing are systematically encapsulated. Last but not least, the remaining challenges and proposed perspectives are highlighted for the future development of advanced cathodes. The accurate analysis of cation migration using advanced characterization, precise control of material synthesis, and multi-dimensional synergistic modification will be the key research areas for cation migration in cathodes. This review provides a comprehensive understanding of cation migration and intermixing in advanced cathodes. The effective inhibition of cation migration and the rational utilization of cation intermixing will emerge as pivotal and controllable factors for the further development of advanced cathodes.
{"title":"Insights into Cation Migration and Intermixing in Advanced Cathode Materials for Lithium-Ion Batteries","authors":"Shu Zhang, Zhuo Yang, Yong Lu, Weiwei Xie, Zhenhua Yan, Jun Chen","doi":"10.1002/aenm.202402068","DOIUrl":"https://doi.org/10.1002/aenm.202402068","url":null,"abstract":"Cathode materials are the core components of lithium-ion batteries owing to the determination of the practical voltage and effective energy of the battery system. However, advanced cathodes have faced challenges related to cation migration and cation intermixing. In this review, the study summarizes the structural failure mechanisms due to the cation mixing of advanced cathodes, including Ni-rich and Li-rich layered cathodes, spinel, olivine, and disordered rock-salt materials. This review starts by discussing the structural degradation mechanisms caused by cation intermixing in different cathodes, focusing on the electronic structure, crystal structure, and electrode structure. Furthermore, the optimization strategies for effective inhibition of cation migration and rational utilization of cation mixing are systematically encapsulated. Last but not least, the remaining challenges and proposed perspectives are highlighted for the future development of advanced cathodes. The accurate analysis of cation migration using advanced characterization, precise control of material synthesis, and multi-dimensional synergistic modification will be the key research areas for cation migration in cathodes. This review provides a comprehensive understanding of cation migration and intermixing in advanced cathodes. The effective inhibition of cation migration and the rational utilization of cation intermixing will emerge as pivotal and controllable factors for the further development of advanced cathodes.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141463686","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}
All-solid-state sodium batteries offer the advantage of both sustainability and safety. Solid-state electrolytes play a key role, and an oxygen-incorporated NaAlCl4 composite electrolyte is presented with a high ambient-temperature ionic conductivity of > 0.1 mS cm−1. The electrolyte synthesized with a mechanochemical reaction consists of in situ-formed Al2O3 nanoparticles that provide enhanced conduction through an oxychloride phase at the interface. Magic angle spinning nuclear magnetic resonance spectroscopy confirms the formation of Al2O3 and the oxychloride phases at the interface and sheds insights into the origin of the enhanced ionic conductivity of the composite electrolyte. Additionally, simply adding Al2O3 nanoparticles to NaAlCl4 before mechanochemical synthesis is investigated, and a relationship between Al2O3 surface area and composite electrolyte ionic conductivity is identified. All-solid-state sodium batteries assembled with the composite electrolyte demonstrate a high specific capacity of 124 mA h g−1, clearly outperforming the baseline NaAlCl4 electrolyte. Furthermore, X-ray photoelectron spectroscopy is utilized to understand the origin of capacity fade and obtain insights into electrolyte decomposition products. This work provides a deeper understanding of methods for boosting the ion transport in a low-cost halide solid electrolyte for practical viability of all-solid-state sodium batteries.
全固态钠电池具有可持续性和安全性的优点。固态电解质起着关键作用，本文介绍了一种氧掺杂 NaAlCl4 复合电解质，其常温离子电导率高达 > 0.1 mS cm-1。通过机械化学反应合成的电解质包含原位形成的 Al2O3 纳米粒子，可通过界面上的氧氯化相增强传导性。魔角旋转核磁共振光谱证实了 Al2O3 和氧氯化相在界面上的形成，并揭示了复合电解质离子传导性增强的原因。此外，还研究了在机械化学合成之前向 NaAlCl4 中简单添加 Al2O3 纳米颗粒的方法，并确定了 Al2O3 表面积与复合电解质离子电导率之间的关系。用复合电解质组装的全固态钠电池显示出 124 mA h g-1 的高比容量，明显优于基准 NaAlCl4 电解质。此外，还利用 X 射线光电子能谱来了解容量衰减的原因，并深入了解电解质分解产物。这项研究加深了人们对提高低成本卤化物固体电解质离子传输的方法的理解，从而提高了全固态钠电池的实际可行性。
{"title":"Enhanced Interfacial Conduction in Low-Cost NaAlCl4 Composite Solid Electrolyte for Solid-State Sodium Batteries","authors":"Erick Ruoff, Steven Kmiec, Arumugam Manthiram","doi":"10.1002/aenm.202402091","DOIUrl":"https://doi.org/10.1002/aenm.202402091","url":null,"abstract":"All-solid-state sodium batteries offer the advantage of both sustainability and safety. Solid-state electrolytes play a key role, and an oxygen-incorporated NaAlCl<sub>4</sub> composite electrolyte is presented with a high ambient-temperature ionic conductivity of > 0.1 mS cm<sup>−1</sup>. The electrolyte synthesized with a mechanochemical reaction consists of in situ-formed Al<sub>2</sub>O<sub>3</sub> nanoparticles that provide enhanced conduction through an oxychloride phase at the interface. Magic angle spinning nuclear magnetic resonance spectroscopy confirms the formation of Al<sub>2</sub>O<sub>3</sub> and the oxychloride phases at the interface and sheds insights into the origin of the enhanced ionic conductivity of the composite electrolyte. Additionally, simply adding Al<sub>2</sub>O<sub>3</sub> nanoparticles to NaAlCl<sub>4</sub> before mechanochemical synthesis is investigated, and a relationship between Al<sub>2</sub>O<sub>3</sub> surface area and composite electrolyte ionic conductivity is identified. All-solid-state sodium batteries assembled with the composite electrolyte demonstrate a high specific capacity of 124 mA h g<sup>−1</sup>, clearly outperforming the baseline NaAlCl<sub>4</sub> electrolyte. Furthermore, X-ray photoelectron spectroscopy is utilized to understand the origin of capacity fade and obtain insights into electrolyte decomposition products. This work provides a deeper understanding of methods for boosting the ion transport in a low-cost halide solid electrolyte for practical viability of all-solid-state sodium batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141463622","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}
Carbon anode‐based Li‐ion batteries (LIBs) have been widely used ranging from portable electronics to electric vehicles (EVs). Here a novel carbon material called microzonal carbon is introduced, synthesized from waste hard rubber (WHR), as an anode material for next‐generation LIBs. This material consists of a hybrid carbon structure embedded with short range ordered carbon zones, including expanded graphene sheets and nanopores. Two types of microzonal carbons (M‐5H and M‐10H) are tested in LIBs to unveil their electrochemical performance. The anode fabricated with M‐10H provides a high initial coulombic efficiency (60%), reversible capacity (377 mA h g−1 at 0.13 C), rate capability (275 mA h g−1 at 2.6 C) and cyclic stability (capacity retention of 99% at 0.13 C after 100 cycles). The electrochemical properties of microzonal carbon can be attributed to its unique hybrid carbon structure, facilitating fast ion diffusion, high electronic conductivity, and the ability to form stable interphase. Therefore, this work presents new insights into the electrochemical behavior of microzonal carbon as an anode material in next‐generation LIBs.
从便携式电子产品到电动汽车，基于碳阳极的锂离子电池（LIB）已得到广泛应用。本文介绍了一种名为微带碳的新型碳材料，该材料由废硬橡胶（WHR）合成，可作为下一代锂离子电池的阳极材料。这种材料由混合碳结构组成，内嵌短程有序碳区，包括膨胀石墨烯片和纳米孔。在 LIB 中测试了两种类型的微带碳（M-5H 和 M-10H），以揭示它们的电化学性能。用 M-10H 制作的阳极具有较高的初始库仑效率（60%）、可逆容量（0.13 C 时为 377 mA h g-1）、速率能力（2.6 C 时为 275 mA h g-1）和循环稳定性（100 次循环后，0.13 C 时的容量保持率为 99%）。微带碳的电化学特性可归因于其独特的混合碳结构，这种结构有利于离子的快速扩散、高电子传导性以及形成稳定相间的能力。因此，这项研究对微宗炭作为下一代 LIB 负极材料的电化学行为提出了新的见解。
{"title":"Electrochemical Compatibility of Microzonal Carbon in Ion Uptake and Molecular Insights into Interphase Evolution for Next‐Generation Li‐Ion Batteries","authors":"Montajar Sarkar, Rumana Hossain, Jian Peng, Neeraj Sharma, Veena Sahajwalla","doi":"10.1002/aenm.202401977","DOIUrl":"https://doi.org/10.1002/aenm.202401977","url":null,"abstract":"Carbon anode‐based Li‐ion batteries (LIBs) have been widely used ranging from portable electronics to electric vehicles (EVs). Here a novel carbon material called microzonal carbon is introduced, synthesized from waste hard rubber (WHR), as an anode material for next‐generation LIBs. This material consists of a hybrid carbon structure embedded with short range ordered carbon zones, including expanded graphene sheets and nanopores. Two types of microzonal carbons (M‐5H and M‐10H) are tested in LIBs to unveil their electrochemical performance. The anode fabricated with M‐10H provides a high initial coulombic efficiency (60%), reversible capacity (377 mA h g<jats:sup>−1</jats:sup> at 0.13 C), rate capability (275 mA h g<jats:sup>−1</jats:sup> at 2.6 C) and cyclic stability (capacity retention of 99% at 0.13 C after 100 cycles). The electrochemical properties of microzonal carbon can be attributed to its unique hybrid carbon structure, facilitating fast ion diffusion, high electronic conductivity, and the ability to form stable interphase. Therefore, this work presents new insights into the electrochemical behavior of microzonal carbon as an anode material in next‐generation LIBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141462970","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}
Caizhen Yue, Xiaobo Yang, Xiong Zhang, Shifu Wang, Wei Xu, Ruru Chen, Jiuyi Wang, Jie Yin, Yanqiang Huang, Xuning Li
The regulation of the local microenvironment in the single‐atom catalysts affords a scheme for accelerating the overall reaction kinetics of electrochemical CO2 reduction reaction (CO2RR), which is of vital importance but remains challenging. Herein, a carbon nanotube‐supported single‐Sn‐atom catalyst (P‐SnN4‐CNT) is developed by a modified pyrolysis procedure with P‐doping into the second coordination shell of SnN4 moiety to modulate the electron structure of metal Sn center. The resulting P‐SnN4‐CNT delivered a high CO partial current density of −380 mA cm−2 with Faradaic efficiency (FE) of CO above 90% across a wide range of −0.5 to −0.8 V versus reversible hydrogen electrode (vs RHE), along with optimal FE (CO) of ≈98.5% at −0.6 V versus RHE in a flow cell. Moreover, P‐SnN4‐CNT achieved an extremely high turnover frequency of 126 471 h−1 with an applied potential of −0.8 V versus RHE, which ranks the best among the reported M─N─C catalysts for electrocatalytic CO2 reduction. The combination of in situ characterization techniques and density functional theory calculation revealed that the doping of P atoms benefited the activation and hydrogenation steps of CO2 and promoted the Sn4+ reduction to Sn2+ during the reaction process, where Sn2+ is identified as the active site for the CO generation. The work provides a clear mechanistic insight for both electron structure optimization and identification of active sites by local microenvironment regulation of single‐Sn‐atom, which shall pave a way for the exploitation of other M─N─C catalysts with high CO2RR performance.
调节单原子催化剂的局部微环境为加速电化学二氧化碳还原反应（CO2RR）的整体反应动力学提供了方案，这一点至关重要，但仍具有挑战性。本文通过改进的热解过程，在 SnN4 分子的第二配位层中掺入 P，以调节金属 Sn 中心的电子结构，从而开发出一种碳纳米管支撑的单 Sn 原子催化剂（P-SnN4-CNT）。所制备的 P-SnN4-CNT 在-0.5 至 -0.8 V 的宽电压范围内与可逆氢电极（vs RHE）相比，可提供 -380 mA cm-2 的高 CO 部分电流密度，CO 的法拉第效率（FE）超过 90%，在-0.6 V 的电压范围内与 RHE 相比，流动池中的最佳 FE（CO）≈98.5%。此外，P-SnN4-CNT 在-0.8 V 相对于 RHE 的应用电位下实现了 126 471 h-1 的极高周转频率，在已报道的 M─N─C 催化剂电催化二氧化碳还原中名列前茅。结合原位表征技术和密度泛函理论计算发现，P 原子的掺杂有利于 CO2 的活化和氢化步骤，并在反应过程中促进 Sn4+ 还原成 Sn2+，其中 Sn2+ 被确定为 CO 生成的活性位点。这项工作为电子结构优化和通过单个 Sn 原子的局部微环境调节确定活性位点提供了清晰的机理认识，这将为开发其他具有高 CO2RR 性能的 M─N─C 催化剂铺平道路。
{"title":"Secondary Coordination Sphere Engineering of Single‐Sn‐Atom catalyst via P Doping for Efficient CO2 Electroreduction","authors":"Caizhen Yue, Xiaobo Yang, Xiong Zhang, Shifu Wang, Wei Xu, Ruru Chen, Jiuyi Wang, Jie Yin, Yanqiang Huang, Xuning Li","doi":"10.1002/aenm.202401448","DOIUrl":"https://doi.org/10.1002/aenm.202401448","url":null,"abstract":"The regulation of the local microenvironment in the single‐atom catalysts affords a scheme for accelerating the overall reaction kinetics of electrochemical CO<jats:sub>2</jats:sub> reduction reaction (CO<jats:sub>2</jats:sub>RR), which is of vital importance but remains challenging. Herein, a carbon nanotube‐supported single‐Sn‐atom catalyst (P‐SnN<jats:sub>4</jats:sub>‐CNT) is developed by a modified pyrolysis procedure with P‐doping into the second coordination shell of SnN<jats:sub>4</jats:sub> moiety to modulate the electron structure of metal Sn center. The resulting P‐SnN<jats:sub>4</jats:sub>‐CNT delivered a high CO partial current density of −380 mA cm<jats:sup>−2</jats:sup> with Faradaic efficiency (FE) of CO above 90% across a wide range of −0.5 to −0.8 V versus reversible hydrogen electrode (vs RHE), along with optimal FE (CO) of ≈98.5% at −0.6 V versus RHE in a flow cell. Moreover, P‐SnN<jats:sub>4</jats:sub>‐CNT achieved an extremely high turnover frequency of 126 471 h<jats:sup>−1</jats:sup> with an applied potential of −0.8 V versus RHE, which ranks the best among the reported M─N─C catalysts for electrocatalytic CO<jats:sub>2</jats:sub> reduction. The combination of in situ characterization techniques and density functional theory calculation revealed that the doping of P atoms benefited the activation and hydrogenation steps of CO<jats:sub>2</jats:sub> and promoted the Sn<jats:sup>4+</jats:sup> reduction to Sn<jats:sup>2+</jats:sup> during the reaction process, where Sn<jats:sup>2+</jats:sup> is identified as the active site for the CO generation. The work provides a clear mechanistic insight for both electron structure optimization and identification of active sites by local microenvironment regulation of single‐Sn‐atom, which shall pave a way for the exploitation of other M─N─C catalysts with high CO<jats:sub>2</jats:sub>RR performance.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":27.8,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141462853","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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