Pub Date : 2025-04-16DOI: 10.1016/j.joule.2024.101817
Zhou Xing , Suxiang Ma , Bin-Wen Chen , Mingwei An , Ajuan Fan , Xinqiong Hu , Yang Wang , Lin-Long Deng , Qiufeng Huang , Hiroyuki Kanda , Fahad Gallab Al-Amri , Gainluca Pozzi , Yi Zhang , Jianxing Xia , Jiazhen Wu , Xugang Guo , Mohammad Khaja Nazeeruddin
Pristine fullerene C60 is currently the best-performing electron transport layer (ETL) for perovskite solar cells (PSCs) but suffers from significant aggregation in solution. Consequently, the high-cost and complex thermal evaporation method is typically used to deposit high-quality C60 ETLs. To address this challenge, we introduce an n-type polymeric additive that can solubilize and stabilize C60 molecules for solution processing, leading to efficient and stable solution-processed-C60 (SP-C60) ETLs. The achievement is attributed to the well-matched properties of the n-type polymer and the precisely controlled intermolecular interactions between the polymer and C60. As a result, the SP-C60 ETL with 5-wt % polymer addition afforded a champion power conversion efficiency of 25.60% (certified 25.09%). This is not only the highest performance among the current SP-C60 devices but also highly competitive to the state-of-the-art thermally evaporated C60 devices. Importantly, the champion device showed significantly enhanced stability (T95, light > 1,800 h; T80, heat = 700 h).
{"title":"Solubilizing and stabilizing C60 with n-type polymer enables efficient inverted perovskite solar cells","authors":"Zhou Xing , Suxiang Ma , Bin-Wen Chen , Mingwei An , Ajuan Fan , Xinqiong Hu , Yang Wang , Lin-Long Deng , Qiufeng Huang , Hiroyuki Kanda , Fahad Gallab Al-Amri , Gainluca Pozzi , Yi Zhang , Jianxing Xia , Jiazhen Wu , Xugang Guo , Mohammad Khaja Nazeeruddin","doi":"10.1016/j.joule.2024.101817","DOIUrl":"10.1016/j.joule.2024.101817","url":null,"abstract":"<div><div>Pristine fullerene C<sub>60</sub> is currently the best-performing electron transport layer (ETL) for perovskite solar cells (PSCs) but suffers from significant aggregation in solution. Consequently, the high-cost and complex thermal evaporation method is typically used to deposit high-quality C<sub>60</sub> ETLs. To address this challenge, we introduce an n-type polymeric additive that can solubilize and stabilize C<sub>60</sub> molecules for solution processing, leading to efficient and stable solution-processed-C<sub>60</sub> (SP-C<sub>60</sub>) ETLs. The achievement is attributed to the well-matched properties of the n-type polymer and the precisely controlled intermolecular interactions between the polymer and C<sub>60</sub>. As a result, the SP-C<sub>60</sub> ETL with 5-wt % polymer addition afforded a champion power conversion efficiency of 25.60% (certified 25.09%). This is not only the highest performance among the current SP-C<sub>60</sub> devices but also highly competitive to the state-of-the-art thermally evaporated C<sub>60</sub> devices. Importantly, the champion device showed significantly enhanced stability (<em>T</em><sub>95, light</sub> > 1,800 h; <em>T</em><sub>80, heat</sub> = 700 h).</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 4","pages":"Article 101817"},"PeriodicalIF":38.6,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143124950","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}
Pub Date : 2025-04-16DOI: 10.1016/j.joule.2025.101912
Tarandeep Singh Thukral , Siavash Khodakarami , Wentao Yang , Ghassan Arissi , Pouya Kabirzadeh , Chi Wang , Dalia Ghaddar , Muhammad Jahidul Hoque , Matthew A. Pitschman , Patrick M. Fourspring , Nenad Miljkovic
Condensation enables heat transfer with superior efficiency compared with single-phase processes, making it prevalent in industry. The discovery of dropwise condensation coupled with rising global energy demands stimulated an academic fervor in the 20th century that has lasted several decades, with researchers developing complex surface modification technologies to enhance condensation heat transfer. However, practical complexities such as non-condensable gas (NCG) infiltration, accurate temperature measurements, manufacturability, and durability preclude these technologies’ industrial adoption. In this perspective, we summarize how the lack of a standard experimental procedure has led to researchers publishing data without realizing that NCGs are present in their systems. We discuss how emerging characterization techniques, such as infrared thermometry and machine learning, can overcome the limitations of traditional methods while improving data reliability and reproducibility. We also recommend topics of investigation for the heat transfer community to progress toward highly efficient thermal systems in a rapidly electrifying and decarbonizing world.
{"title":"Enhancement versus practicality in steam condensation heat transfer","authors":"Tarandeep Singh Thukral , Siavash Khodakarami , Wentao Yang , Ghassan Arissi , Pouya Kabirzadeh , Chi Wang , Dalia Ghaddar , Muhammad Jahidul Hoque , Matthew A. Pitschman , Patrick M. Fourspring , Nenad Miljkovic","doi":"10.1016/j.joule.2025.101912","DOIUrl":"10.1016/j.joule.2025.101912","url":null,"abstract":"<div><div>Condensation enables heat transfer with superior efficiency compared with single-phase processes, making it prevalent in industry. The discovery of dropwise condensation coupled with rising global energy demands stimulated an academic fervor in the 20<sup>th</sup> century that has lasted several decades, with researchers developing complex surface modification technologies to enhance condensation heat transfer. However, practical complexities such as non-condensable gas (NCG) infiltration, accurate temperature measurements, manufacturability, and durability preclude these technologies’ industrial adoption. In this perspective, we summarize how the lack of a standard experimental procedure has led to researchers publishing data without realizing that NCGs are present in their systems. We discuss how emerging characterization techniques, such as infrared thermometry and machine learning, can overcome the limitations of traditional methods while improving data reliability and reproducibility. We also recommend topics of investigation for the heat transfer community to progress toward highly efficient thermal systems in a rapidly electrifying and decarbonizing world.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 4","pages":"Article 101912"},"PeriodicalIF":38.6,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143767113","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}
Pub Date : 2025-04-16DOI: 10.1016/j.joule.2025.101846
Ling Lv , Haikuo Zhang , Di Lu , Ruhong Li , Haotian Zhu , Baochen Ma , Shuoqing Zhang , Yiqiang Huang , Tao Zhou , Zunhao Fan , Jing Zhang , Lixin Chen , Xiayin Yao , Tao Deng , Xiulin Fan
The advancement of additive engineering in high-voltage LiCoO2 (LCO)-based lithium-ion batteries (LIBs) is limited by the lack of effective guiding principles. Here, we report a lattice coupling mechanism for designing nitrile additives, systematically evaluating 20 candidates to quantify their enhancement effects on LCO performance. Key to this mechanism are two motif descriptors: the O 2p band center energy and the energy gap (ΔE) between the O 2p band center and the Co 3d band center, which significantly improve the structural and interfacial stability of the LCO cathode. Guided by this principle, we developed 1,2,2,3-propanetetracarbonitrile (PCN) as a representative additive, achieving 80% capacity retention in 4.55 V 1.0 Ah artificial graphite (AG)||LCO pouch cells after over 770 and 380 cycles at 25°C and 45°C, respectively. This work provides new insights into the exploration and evaluation of additive chemistry for high-voltage LCO cathode.
{"title":"Additive engineering enables aggressive high-voltage LiCoO2 lithium-ion batteries","authors":"Ling Lv , Haikuo Zhang , Di Lu , Ruhong Li , Haotian Zhu , Baochen Ma , Shuoqing Zhang , Yiqiang Huang , Tao Zhou , Zunhao Fan , Jing Zhang , Lixin Chen , Xiayin Yao , Tao Deng , Xiulin Fan","doi":"10.1016/j.joule.2025.101846","DOIUrl":"10.1016/j.joule.2025.101846","url":null,"abstract":"<div><div>The advancement of additive engineering in high-voltage LiCoO<sub>2</sub> (LCO)-based lithium-ion batteries (LIBs) is limited by the lack of effective guiding principles. Here, we report a lattice coupling mechanism for designing nitrile additives, systematically evaluating 20 candidates to quantify their enhancement effects on LCO performance. Key to this mechanism are two motif descriptors: the O 2<em>p</em> band center energy and the energy gap (<em>ΔE</em>) between the O 2<em>p</em> band center and the Co <em>3d</em> band center, which significantly improve the structural and interfacial stability of the LCO cathode. Guided by this principle, we developed 1,2,2,3-propanetetracarbonitrile (PCN) as a representative additive, achieving 80% capacity retention in 4.55 V 1.0 Ah artificial graphite (AG)||LCO pouch cells after over 770 and 380 cycles at 25°C and 45°C, respectively. This work provides new insights into the exploration and evaluation of additive chemistry for high-voltage LCO cathode.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 4","pages":"Article 101846"},"PeriodicalIF":38.6,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143375526","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}
Pub Date : 2025-04-16DOI: 10.1016/j.joule.2025.101850
Jin Hyuck Heo , Seok Young Hong , Jin Kyoung Park , Hyong Joon Lee , Fei Zhang (张飞) , Sang Hyuk Im
The stability of perovskite solar modules has rarely been reported due to inefficient coating reproducibility and charge extraction, especially for the slot-die-coating process. In this study, we regulated the energy-level mismatch and improved the surface wettability by chemical oxidization between antimony trichloride (SbCl3) and poly[bis(4-phenyl)](2,4,6-trimethylphenyl)amine (PTAA) through a Lewis acid-base interaction. As a result, charge extraction and coating reproducibility of the slot-die-coated perovskite film were improved. The modules’ power conversion efficiency (PCE) was enhanced to 22.05% and 20.65% (certified 20.33%) with aperture areas of 25 and 64 cm2 for the rigid substrates and 18.86% with an aperture area of 12 cm2 for the flexible substrates. Furthermore, the encapsulated SbCl3-doped PTAA module devices with an aperture area of 64 cm2 maintain 90% of the initial PCE after a durability test under continuous 1 sun illumination for 1,000 h at 85°C and 85% relative humidity.
{"title":"Chemical oxidization of PTAA enables stable slot-die-coated perovskite solar modules","authors":"Jin Hyuck Heo , Seok Young Hong , Jin Kyoung Park , Hyong Joon Lee , Fei Zhang (张飞) , Sang Hyuk Im","doi":"10.1016/j.joule.2025.101850","DOIUrl":"10.1016/j.joule.2025.101850","url":null,"abstract":"<div><div>The stability of perovskite solar modules has rarely been reported due to inefficient coating reproducibility and charge extraction, especially for the slot-die-coating process. In this study, we regulated the energy-level mismatch and improved the surface wettability by chemical oxidization between antimony trichloride (SbCl<sub>3</sub>) and poly[bis(4-phenyl)](2,4,6-trimethylphenyl)amine (PTAA) through a Lewis acid-base interaction. As a result, charge extraction and coating reproducibility of the slot-die-coated perovskite film were improved. The modules’ power conversion efficiency (PCE) was enhanced to 22.05% and 20.65% (certified 20.33%) with aperture areas of 25 and 64 cm<sup>2</sup> for the rigid substrates and 18.86% with an aperture area of 12 cm<sup>2</sup> for the flexible substrates. Furthermore, the encapsulated SbCl<sub>3</sub>-doped PTAA module devices with an aperture area of 64 cm<sup>2</sup> maintain 90% of the initial PCE after a durability test under continuous 1 sun illumination for 1,000 h at 85°C and 85% relative humidity.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 4","pages":"Article 101850"},"PeriodicalIF":38.6,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143547043","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}
Pub Date : 2025-04-16DOI: 10.1016/j.joule.2024.101818
Jinxuan Cheng , Wenhua Xue , Tianyu Zhang , Xiaofang Li , Yichen Zhu , Li Yin , Honghao Yao , Zixuan Fu , Longzhi Wu , Chen Chen , Peng Zhao , Xiaojing Ma , Feng Jiang , Xiaodong Wang , Mingyu Li , Jun Mao , Yumei Wang , Feng Cao , Qian Zhang
Thermoelectric modules fabricated by traditional welding fall short of achieving optimal conversion efficiencies, primarily due to performance degradation of materials at high temperatures, severe elemental diffusion, and residual thermal stress at the interface. Transient liquid phase bonding enables the realization of joints with high-melting-point compounds at low bonding temperatures, providing a promising solution for achieving “low-temperature bonding and high-temperature service.” Owing to the low eutectic point of the solder and high melting points of compounds, we optimize the design of a germanium-telluride-based module at 533 K, which is successfully applied at the hot-side temperature of 773 K. Attributed to high-performance materials and reliable joints, the module realizes a high conversion efficiency of ∼15.1% and remains stable throughout 150 h of service. By adopting the same approach, the low- (Bi2Te3) and high-temperature (half-Heusler) modules are assembled. We provide a promising and general route for the assembly of full-temperature-range thermoelectric devices.
{"title":"A universal approach to high-performance thermoelectric module design for power generation","authors":"Jinxuan Cheng , Wenhua Xue , Tianyu Zhang , Xiaofang Li , Yichen Zhu , Li Yin , Honghao Yao , Zixuan Fu , Longzhi Wu , Chen Chen , Peng Zhao , Xiaojing Ma , Feng Jiang , Xiaodong Wang , Mingyu Li , Jun Mao , Yumei Wang , Feng Cao , Qian Zhang","doi":"10.1016/j.joule.2024.101818","DOIUrl":"10.1016/j.joule.2024.101818","url":null,"abstract":"<div><div>Thermoelectric modules fabricated by traditional welding fall short of achieving optimal conversion efficiencies, primarily due to performance degradation of materials at high temperatures, severe elemental diffusion, and residual thermal stress at the interface. Transient liquid phase bonding enables the realization of joints with high-melting-point compounds at low bonding temperatures, providing a promising solution for achieving “low-temperature bonding and high-temperature service.” Owing to the low eutectic point of the solder and high melting points of compounds, we optimize the design of a germanium-telluride-based module at 533 K, which is successfully applied at the hot-side temperature of 773 K. Attributed to high-performance materials and reliable joints, the module realizes a high conversion efficiency of ∼15.1% and remains stable throughout 150 h of service. By adopting the same approach, the low- (Bi<sub>2</sub>Te<sub>3</sub>) and high-temperature (half-Heusler) modules are assembled. We provide a promising and general route for the assembly of full-temperature-range thermoelectric devices.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 4","pages":"Article 101818"},"PeriodicalIF":38.6,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020968","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}
Pub Date : 2025-04-14DOI: 10.1016/j.joule.2025.101919
Xuejie Zhu, Dongqi Yu, Xin Zhou, Nan Wang, Hong Liu, Zihui Liang, Congcong Wu, Kai Wang, Dayong Jin, Shengzhong Liu, Dong Yang
Ambient blade coating of perovskite solar modules shows great potential for large-scale manufacture and commercialization. However, blade coating nanometer-thick buffer layers typically results in a nonuniform surface due to particle instability and aggregation, often leading to insufficient integration and destabilization of the crystallographic lattice in the overlying perovskite layer. Herein, we introduce a layer of “molecular glue” that can effectively anchor the solute that suspends the monodisperse SnO2 nanoparticles into a uniform thin film and adhere it to the top perovskite during the mechanical blading process. Leveraging this holistic nanoparticle-anchoring strategy, we have achieved a seamlessly bonded cathode heterojunction, resulting in a record efficiency of 26.11% for small cells and the highest efficiency so far of 22.76% (certified at 21.60%) for mini-modules. Importantly, these ambiently all-blade-coated devices exhibit an extended lifetime of approximately 1,500 h, as verified by ISOS-O testing, indicating great promise for commercialization.
{"title":"Interfacial molecular anchor for ambient all-bladed perovskite solar modules","authors":"Xuejie Zhu, Dongqi Yu, Xin Zhou, Nan Wang, Hong Liu, Zihui Liang, Congcong Wu, Kai Wang, Dayong Jin, Shengzhong Liu, Dong Yang","doi":"10.1016/j.joule.2025.101919","DOIUrl":"https://doi.org/10.1016/j.joule.2025.101919","url":null,"abstract":"Ambient blade coating of perovskite solar modules shows great potential for large-scale manufacture and commercialization. However, blade coating nanometer-thick buffer layers typically results in a nonuniform surface due to particle instability and aggregation, often leading to insufficient integration and destabilization of the crystallographic lattice in the overlying perovskite layer. Herein, we introduce a layer of “molecular glue” that can effectively anchor the solute that suspends the monodisperse SnO<sub>2</sub> nanoparticles into a uniform thin film and adhere it to the top perovskite during the mechanical blading process. Leveraging this holistic nanoparticle-anchoring strategy, we have achieved a seamlessly bonded cathode heterojunction, resulting in a record efficiency of 26.11% for small cells and the highest efficiency so far of 22.76% (certified at 21.60%) for mini-modules. Importantly, these ambiently all-blade-coated devices exhibit an extended lifetime of approximately 1,500 h, as verified by ISOS-O testing, indicating great promise for commercialization.","PeriodicalId":343,"journal":{"name":"Joule","volume":"90 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143827397","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}
Pub Date : 2025-03-31DOI: 10.1016/j.joule.2025.101888
Xiang Li, Yu Wei, Xiang Gao, Zhongqiang Zhang, Zhong Lin Wang, Di Wei
Maxwell’s demon seemingly violates the second law of thermodynamics, but in reality, it requires external energy for information processing and particle control, thereby ensuring an overall increase in system entropy. Here, triboiontronic Maxwell’s demon was established by triboelectric-induced polarization, enabling remote regulation of charge migration within electrical double layers (EDLs). For energy flow, an enhanced physical-adsorption triboiontronic nanogenerator (EP-TING) achieved a remarkable transferred charge density of 2,347.12 mC/m2, surpassing conventional EDL-based technologies by several orders of magnitude. Furthermore, the advanced synergy-enhanced strategy TING (ES-TING), integrating redox reactions, further increased the charge density to 5,237.51 mC/m2, marking a significant breakthrough in energy conversion efficiency. For information flow, bionic neural circuits utilizing EP-TINGs/ES-TINGs enabled highly portable, interference-resistant underwater transmission systems with minimal energy consumption, effectively addressing challenges of acoustic multipath interference, environmental noise, and severe signal attenuation. Therefore, harnessing triboiontronic Maxwell’s demon provides an efficient energy-information flow, proving crucial in the post-Moore era.
{"title":"Harnessing triboiontronic Maxwell’s demon by triboelectric-induced polarization for efficient energy-information flow","authors":"Xiang Li, Yu Wei, Xiang Gao, Zhongqiang Zhang, Zhong Lin Wang, Di Wei","doi":"10.1016/j.joule.2025.101888","DOIUrl":"https://doi.org/10.1016/j.joule.2025.101888","url":null,"abstract":"Maxwell’s demon seemingly violates the second law of thermodynamics, but in reality, it requires external energy for information processing and particle control, thereby ensuring an overall increase in system entropy. Here, triboiontronic Maxwell’s demon was established by triboelectric-induced polarization, enabling remote regulation of charge migration within electrical double layers (EDLs). For energy flow, an enhanced physical-adsorption triboiontronic nanogenerator (EP-TING) achieved a remarkable transferred charge density of 2,347.12 mC/m<sup>2</sup>, surpassing conventional EDL-based technologies by several orders of magnitude. Furthermore, the advanced synergy-enhanced strategy TING (ES-TING), integrating redox reactions, further increased the charge density to 5,237.51 mC/m<sup>2</sup>, marking a significant breakthrough in energy conversion efficiency. For information flow, bionic neural circuits utilizing EP-TINGs/ES-TINGs enabled highly portable, interference-resistant underwater transmission systems with minimal energy consumption, effectively addressing challenges of acoustic multipath interference, environmental noise, and severe signal attenuation. Therefore, harnessing triboiontronic Maxwell’s demon provides an efficient energy-information flow, proving crucial in the post-Moore era.","PeriodicalId":343,"journal":{"name":"Joule","volume":"5 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143737271","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}
Pub Date : 2025-03-28DOI: 10.1016/j.joule.2025.101884
Jinwook Rhyu, Joachim Schaeffer, Michael L. Li, Xiao Cui, William C. Chueh, Martin Z. Bazant, Richard D. Braatz
Optimization of the formation step in lithium-ion battery manufacturing is challenging due to limited physical understanding of solid-electrolyte interphase formation and the long testing time (∼100 days) for cells to reach the end of life. We propose a systematic feature-design framework that requires minimal domain knowledge for accurate cycle life prediction during formation. By only using two simple features designed from our framework, extracted from formation data without any additional diagnostic cycles, we achieved an average of 9.87% error for cycle life prediction. The physics-based investigation guided by the two designed features shows that the voltage ranges identified by our framework capture the effects of formation temperature and microscopic-particle resistance heterogeneity. By designing highly predictive, robust, and interpretable features, our approach can accelerate industrial battery formation research, leveraging the interplay between data-driven feature design and mechanistic understanding.
{"title":"Systematic feature design for cycle life prediction of lithium-ion batteries during formation","authors":"Jinwook Rhyu, Joachim Schaeffer, Michael L. Li, Xiao Cui, William C. Chueh, Martin Z. Bazant, Richard D. Braatz","doi":"10.1016/j.joule.2025.101884","DOIUrl":"https://doi.org/10.1016/j.joule.2025.101884","url":null,"abstract":"Optimization of the formation step in lithium-ion battery manufacturing is challenging due to limited physical understanding of solid-electrolyte interphase formation and the long testing time (∼100 days) for cells to reach the end of life. We propose a systematic feature-design framework that requires minimal domain knowledge for accurate cycle life prediction during formation. By only using two simple <span><span style=\"\"></span><span data-mathml='<math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow is=\"true\"><mi is=\"true\">Q</mi><mrow is=\"true\"><mo is=\"true\">(</mo><mi is=\"true\">V</mi><mo is=\"true\">)</mo></mrow></mrow></math>' role=\"presentation\" style=\"font-size: 90%; display: inline-block; position: relative;\" tabindex=\"0\"><svg aria-hidden=\"true\" focusable=\"false\" height=\"2.779ex\" role=\"img\" style=\"vertical-align: -0.812ex;\" viewbox=\"0 -846.5 2506.7 1196.3\" width=\"5.822ex\" xmlns:xlink=\"http://www.w3.org/1999/xlink\"><g fill=\"currentColor\" stroke=\"currentColor\" stroke-width=\"0\" transform=\"matrix(1 0 0 -1 0 0)\"><g is=\"true\"><g is=\"true\"><use xlink:href=\"#MJMATHI-51\"></use></g><g is=\"true\" transform=\"translate(958,0)\"><g is=\"true\"><use xlink:href=\"#MJMAIN-28\"></use></g><g is=\"true\" transform=\"translate(389,0)\"><use xlink:href=\"#MJMATHI-56\"></use></g><g is=\"true\" transform=\"translate(1159,0)\"><use xlink:href=\"#MJMAIN-29\"></use></g></g></g></g></svg><span role=\"presentation\"><math xmlns=\"http://www.w3.org/1998/Math/MathML\"><mrow is=\"true\"><mi is=\"true\">Q</mi><mrow is=\"true\"><mo is=\"true\">(</mo><mi is=\"true\">V</mi><mo is=\"true\">)</mo></mrow></mrow></math></span></span><script type=\"math/mml\"><math><mrow is=\"true\"><mi is=\"true\">Q</mi><mrow is=\"true\"><mo is=\"true\">(</mo><mi is=\"true\">V</mi><mo is=\"true\">)</mo></mrow></mrow></math></script></span> features designed from our framework, extracted from formation data without any additional diagnostic cycles, we achieved an average of 9.87% error for cycle life prediction. The physics-based investigation guided by the two designed features shows that the voltage ranges identified by our framework capture the effects of formation temperature and microscopic-particle resistance heterogeneity. By designing highly predictive, robust, and interpretable features, our approach can accelerate industrial battery formation research, leveraging the interplay between data-driven feature design and mechanistic understanding.","PeriodicalId":343,"journal":{"name":"Joule","volume":"72 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723841","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}
Pub Date : 2025-03-27DOI: 10.1016/j.joule.2025.101885
Yawei Chen, Menghao Li, Yulin Jie, Yue Liu, Zhengfeng Zhang, Peiping Yu, Wanxia Li, Yang Liu, Xinpeng Li, Zhanwu Lei, Pengfei Yan, Tao Cheng, M. Danny Gu, Shuhong Jiao, Ruiguo Cao
High-voltage lithium (Li) metal batteries (HVLMBs) have attracted tremendous research interest in the past decade owing to their high energy densities. Electrode-electrolyte interphases in HVLMBs play critical roles in dictating their electrochemical performance. However, despite the intensive research on solid-electrolyte interphase (SEI) of Li anode, the cathode-electrolyte interphase (CEI) on high-voltage cathodes remains elusive. Herein, we report the formation and dynamic evolution of CEI on LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes in ether-based electrolytes. We reveal that the solvent-derived interphase predominates the initial CEI, which subsequently evolves into a Li fluoride (LiF)-rich CEI during cycling. Through solvent design, the weak-solvation electrolyte with branched ether solvents promotes the formation of a conformal CEI layer featuring the monodispersing LiF nanocrystals (∼8 nm), thereby enabling NMC811 cathodes to sustain up to 2,000 cycles. This work addresses the long-standing questions regarding CEI evolution and provides valuable guidance for the rational electrolyte design for HVLMBs.
{"title":"Dynamic evolution of cathode-electrolyte interphase in lithium metal batteries with ether electrolytes","authors":"Yawei Chen, Menghao Li, Yulin Jie, Yue Liu, Zhengfeng Zhang, Peiping Yu, Wanxia Li, Yang Liu, Xinpeng Li, Zhanwu Lei, Pengfei Yan, Tao Cheng, M. Danny Gu, Shuhong Jiao, Ruiguo Cao","doi":"10.1016/j.joule.2025.101885","DOIUrl":"https://doi.org/10.1016/j.joule.2025.101885","url":null,"abstract":"High-voltage lithium (Li) metal batteries (HVLMBs) have attracted tremendous research interest in the past decade owing to their high energy densities. Electrode-electrolyte interphases in HVLMBs play critical roles in dictating their electrochemical performance. However, despite the intensive research on solid-electrolyte interphase (SEI) of Li anode, the cathode-electrolyte interphase (CEI) on high-voltage cathodes remains elusive. Herein, we report the formation and dynamic evolution of CEI on LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> (NMC811) cathodes in ether-based electrolytes. We reveal that the solvent-derived interphase predominates the initial CEI, which subsequently evolves into a Li fluoride (LiF)-rich CEI during cycling. Through solvent design, the weak-solvation electrolyte with branched ether solvents promotes the formation of a conformal CEI layer featuring the monodispersing LiF nanocrystals (∼8 nm), thereby enabling NMC811 cathodes to sustain up to 2,000 cycles. This work addresses the long-standing questions regarding CEI evolution and provides valuable guidance for the rational electrolyte design for HVLMBs.","PeriodicalId":343,"journal":{"name":"Joule","volume":"133 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713656","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}
Pub Date : 2025-03-26DOI: 10.1016/j.joule.2025.101883
Bei Zhou, Hengzhou Liu, Guangcan Su, Heejong Shin, Xiao-Yan Li, Huajie Ze, Yongxiang Liang, Bosi Peng, Weiyan Ni, Yuanjun Chen, Wenjin Zhu, Christine Yu, Yiqing Chen, Pengfei Ou, Ke Xie, Edward H. Sargent
Electrified reactive capture upgrades CO2 from post-air-capture alkali carbonate liquid to value-added products while regenerating the capture medium. Previous processes exhibited limited energy efficiency (<18%) due to high full-cell voltage (>3.7 V) and modest CO selectivity (<45%). To address this, we developed a Co molecular catalyst featuring an electron-deficient Co center, lowering the required reduction voltage. We then grafted the catalyst onto a conductive support, enhancing charge transfer. An electrified pH-downshifter improved CO2 availability, increasing CO selectivity. The system achieved 70% CO selectivity at 2.7 V and 100 mA cm−2, corresponding to an energy intensity of 35 GJ/ton CO. The energy cost is comparable to that of direct air capture (DAC) followed by reverse water-gas shift (RWGS), but it offers ambient temperature operation.
{"title":"Electrosynthesis of CO from an electrically pH-shifted DAC post-capture liquid using a catalyst:support amide linkage","authors":"Bei Zhou, Hengzhou Liu, Guangcan Su, Heejong Shin, Xiao-Yan Li, Huajie Ze, Yongxiang Liang, Bosi Peng, Weiyan Ni, Yuanjun Chen, Wenjin Zhu, Christine Yu, Yiqing Chen, Pengfei Ou, Ke Xie, Edward H. Sargent","doi":"10.1016/j.joule.2025.101883","DOIUrl":"https://doi.org/10.1016/j.joule.2025.101883","url":null,"abstract":"Electrified reactive capture upgrades CO<sub>2</sub> from post-air-capture alkali carbonate liquid to value-added products while regenerating the capture medium. Previous processes exhibited limited energy efficiency (<18%) due to high full-cell voltage (>3.7 V) and modest CO selectivity (<45%). To address this, we developed a Co molecular catalyst featuring an electron-deficient Co center, lowering the required reduction voltage. We then grafted the catalyst onto a conductive support, enhancing charge transfer. An electrified pH-downshifter improved CO<sub>2</sub> availability, increasing CO selectivity. The system achieved 70% CO selectivity at 2.7 V and 100 mA cm<sup>−2</sup>, corresponding to an energy intensity of 35 GJ/ton CO. The energy cost is comparable to that of direct air capture (DAC) followed by reverse water-gas shift (RWGS), but it offers ambient temperature operation.","PeriodicalId":343,"journal":{"name":"Joule","volume":"99 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703354","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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