JoulePub Date : 2025-03-14DOI: 10.1016/j.joule.2025.101874
Guanjie Li, Dengpan Dong, Dmitry Bedrov, Qinqin Cai, Haojun Wu, Zixing Wang, Jilei Liu, Kang Xu, Lidan Xing, Weishan Li
{"title":"Correlating electrode nano-confinement to interphase chemistry","authors":"Guanjie Li, Dengpan Dong, Dmitry Bedrov, Qinqin Cai, Haojun Wu, Zixing Wang, Jilei Liu, Kang Xu, Lidan Xing, Weishan Li","doi":"10.1016/j.joule.2025.101874","DOIUrl":"https://doi.org/10.1016/j.joule.2025.101874","url":null,"abstract":"The electrode/electrolyte interphases in advanced batteries are critical for their performance, influencing the reversibility and rate capability of cell reactions. Although much research has focused on the electrolyte side, our study reveals the significant impact of the electrode’s interlayer distance on interphasial chemistry. We discovered that smaller interlayer distances in graphitic anodes lead to higher sensitivity to co-intercalation of Li<sup>+</sup> and solvents, resulting in LiF-poor interphases that reduce stability. Conversely, larger interlayer distances allow anion-rich solvation structures, resulting in LiF-rich interphases and facilitating reversible intercalation/deintercalation reactions. This correlation between interlayer distance and interphasial chemistry offers new strategies for designing next-generation battery electrolytes and electrodes, moving beyond electrolyte engineering to include electrode structural considerations. Our findings are universally applicable across diverse electrolyte systems, providing a robust framework for optimizing battery performance.","PeriodicalId":343,"journal":{"name":"Joule","volume":"183 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143618887","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}
{"title":"Enhancing electron transport for efficiency -recorded HTL-free inverted perovskite solar cells by molecular complementary passivation","authors":"Qingbin Cai, Qin Tan, Jiacheng He, Siyuan Tang, Qiang Sun, Dong He, Tianle Cheng, Guoqiang Ma, Jinfeng Huang, Gangsen Su, Chuanxin Chen, Hao Gu, Bingzhe Wang, Jing Fan, Guichuan Xing, Zhubing He","doi":"10.1016/j.joule.2025.101880","DOIUrl":"https://doi.org/10.1016/j.joule.2025.101880","url":null,"abstract":"Inverted perovskite solar cells without pre-depositing a layer of hole-transport materials (HTL-free PSCs) still suffer from the non-irradiative recombination at the perovskite/electron-transport layer (ETL) interface. In this work, we report a molecular complementary passivation (MCP) strategy by employing propylphosphonic acid 3-ammonium bromide (PPAABr) to cooperate with phenethylammonium bromide (PEABr) to mutually passivate surface defects of I and formamidinium (FA) vacancies by multi-coordination. This passivation led to an obvious decrease in interfacial defect-state density and greatly improved exciton and carrier lifetime for the perovskite film. Moreover, MCP surface treatment pushes the perovskite surface Fermi level closer to that of ETL, thereby enhancing interfacial electron extraction. As a result, MCP-based HTL-free PSC achieved a record efficiency of 26.40% (25.92% certified). The encapsulated device retains 94.8% of its initial efficiency after 1,000 h of light soaking. The generality of the MCP strategy also generated a competitive efficiency of 23.66% for 1.68 eV wide-band-gap PSCs.","PeriodicalId":343,"journal":{"name":"Joule","volume":"8 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143618886","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}
{"title":"Spinodal decomposition promoting high thermoelectric performance in half-Heusler","authors":"Sichen Duan, Xin Bao, Jiawei Huang, Rongpei Shi, Linfeng Fei, Wenhua Xue, Honghao Yao, Xiaofang Li, Jian Wang, Xingjun Liu, Jun Mao, Feng Cao, Yumei Wang, Qian Zhang","doi":"10.1016/j.joule.2025.101854","DOIUrl":"https://doi.org/10.1016/j.joule.2025.101854","url":null,"abstract":"Spinodal decomposition typically manifests in partially miscible solid solutions in relevant phase diagrams as primarily dictated by the underlying thermodynamics, which is viewed as a powerful means for enhancing thermoelectric performance. Yet, the incomplete ternary phase diagrams of thermoelectric materials pose a challenge for microstructure design via spinodal decomposition. In addition, experimental investigation of microstructure evolution upon spinodal decomposition in thermoelectric alloys is rare, and its influence on electron and phonon transport remains largely unexplored. Herein, we constructed the (Ti, Zr, Hf)NiSn phase diagram experimentally, revealing a miscibility gap within 973–1,273 K. Spinodal decomposition with anisotropic composition modulation was observed in Ti<sub>0.5</sub>Zr<sub>0.25</sub>Hf<sub>0.25</sub>NiSn<sub>0.99</sub>Sb<sub>0.01</sub> by <em>in situ</em> transmission electron microscopy. The phase-field simulation further elucidates the microstructure evolution upon spinodal decomposition and provides insights into the generation of dislocations during further heat treatment. The annealing process not only induces dense dislocation arrays formed by spinodal evolution but also homogenizes the multiphase to facilitate electron transport. Consequently, a record-high average <em>zT</em> of ∼1.1 between 300 and 973 K has been realized in n-type Ti<sub>0.5</sub>Zr<sub>0.25</sub>Hf<sub>0.25</sub>NiSn<sub>0.99</sub>Sb<sub>0.01</sub>. Importantly, the half-Heusler module achieves a maximum conversion efficiency of ∼12% and an output power density of ∼3.7 W cm<sup>−2</sup> at a temperature difference of 653 K. This “double-high” result outperforms all of the current devices. Our results highlight spinodal decomposition as an effective avenue to advance materials for highly efficient thermoelectric power generation.","PeriodicalId":343,"journal":{"name":"Joule","volume":"1 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-03-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143560950","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}
JoulePub Date : 2025-03-05DOI: 10.1016/j.joule.2025.101850
Jin Hyuck Heo, Seok Young Hong, Jin Kyoung Park, Hyong Joon Lee, Fei Zhang, Sang Hyuk Im
{"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, Sang Hyuk Im","doi":"10.1016/j.joule.2025.101850","DOIUrl":"https://doi.org/10.1016/j.joule.2025.101850","url":null,"abstract":"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.","PeriodicalId":343,"journal":{"name":"Joule","volume":"131 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-03-05","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}
{"title":"Efficient and stable high-entropy organic photovoltaics","authors":"Ming Zhang, Lei Zhu, Jun Yan, Xiaonan Xue, Zaiyu Wang, Flurin Eisner, Guanqing Zhou, Rui Zeng, Lixuan Kan, Liang Wu, Wenkai Zhong, Anyang Zhang, Fei Han, Jingnan Song, Nicolai Hartmann, Zichun Zhou, Hao Jing, Haiming Zhu, Shengjie Xu, Jenny Nelson, Feng Liu","doi":"10.1016/j.joule.2025.101851","DOIUrl":"https://doi.org/10.1016/j.joule.2025.101851","url":null,"abstract":"The lack of simultaneous high efficiency and long-term stability in organic photovoltaics (OPVs) poses a major challenge to commercialization. Here, we introduce a high-entropy (HE) methodology by both physical blending and chemical synthesis, where multiple components are mixed to improve system entropy. Our findings show that physically blended HE blends maintained strong π–π interactions due to acceptors’ identical backbones. The different halogens or alkyl chains reduced structure order and fostered an optimal mixture, where a redistribution of the conduction-band density of states was found, leading to a higher effective band gap, reduced non-radiative recombination, and elevated open-circuit voltage. This HE design rule was then extended to chemical synthesis to make HE materials, which yielded a maximum power conversion efficiency of 20.6% (20.3% ± 0.2%, certified as 20.0%) in OPV devices. Moreover, both operational and thermal stability were improved, measured in conventional encapsulated devices under continuous illumination.","PeriodicalId":343,"journal":{"name":"Joule","volume":"41 1","pages":""},"PeriodicalIF":39.8,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539141","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}
JoulePub Date : 2025-02-19DOI: 10.1016/j.joule.2024.11.012
Toby Wong , Yijie Yang , Rui Tan , Anqi Wang , Zhou Zhou , Zhizhang Yuan , Jiaxi Li , Dezhi Liu , Alberto Alvarez-Fernandez , Chunchun Ye , Mark Sankey , David Ainsworth , Stefan Guldin , Fabrizia Foglia , Neil B. McKeown , Kim E. Jelfs , Xianfeng Li , Qilei Song
{"title":"Sulfonated poly(ether-ether-ketone) membranes with intrinsic microporosity enable efficient redox flow batteries for energy storage","authors":"Toby Wong , Yijie Yang , Rui Tan , Anqi Wang , Zhou Zhou , Zhizhang Yuan , Jiaxi Li , Dezhi Liu , Alberto Alvarez-Fernandez , Chunchun Ye , Mark Sankey , David Ainsworth , Stefan Guldin , Fabrizia Foglia , Neil B. McKeown , Kim E. Jelfs , Xianfeng Li , Qilei Song","doi":"10.1016/j.joule.2024.11.012","DOIUrl":"10.1016/j.joule.2024.11.012","url":null,"abstract":"<div><div>Redox flow batteries (RFBs) are promising for long-duration grid-scale sustainable energy storage. The ion-exchange membrane is a key component that determines energy efficiency and cycling stability. However, it remains challenging to develop membranes with high ionic conductivity and high selectivity toward redox-active electrolytes. We report the development of ion-conductive polymer membranes with record-breaking energy efficiency. By incorporating triptycene into poly(ether-ether-ketone) and controlled sulfonation, the resulting intrinsically microporous polymer membranes form highly interconnected water channels that facilitate transport of charge-balancing ions, particularly hydroxide anions. These microporous membranes showed high ionic conductivity without compromising the selectivity toward redox-active species. The membranes enabled excellent performance in alkaline aqueous organic and zinc-iron flow batteries, demonstrating long-term stability, high power density, and an operational current density up to 700 mA cm<sup>−2</sup>. The membranes also improved performance in neutral pH aqueous RFBs with high capacity utilization and retention, enhanced energy efficiency, and boosted power density.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 2","pages":"Article 101795"},"PeriodicalIF":38.6,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142849735","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
JoulePub Date : 2025-02-19DOI: 10.1016/j.joule.2025.101845
Xueting Zhao , Jiefeng Pan
{"title":"Keeping photovoltaics cool","authors":"Xueting Zhao , Jiefeng Pan","doi":"10.1016/j.joule.2025.101845","DOIUrl":"10.1016/j.joule.2025.101845","url":null,"abstract":"<div><div>In a recent issue of <em>Device</em>, Yip and co-workers reported a self-adaptive interfacial evaporation system that integrates passive evaporative cooling with an active water management pathway. The semi-passive/semi-active system offers a novel and intelligent paradigm for high-efficiency photovoltaic cooling, characterized by near-zero energy usage and low water consumption.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 2","pages":"Article 101845"},"PeriodicalIF":38.6,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143445325","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}
JoulePub Date : 2025-02-19DOI: 10.1016/j.joule.2024.101814
Toby Wong, Yijie Yang, Rui Tan, Anqi Wang, Zhou Zhou, Zhizhang Yuan, Jiaxi Li, Dezhi Liu, Alberto Alvarez-Fernandez, Chunchun Ye, Mark Sankey, David Ainsworth, Stefan Guldin, Fabrizia Foglia, Neil B. McKeown, Kim E. Jelfs, Xianfeng Li, Qilei Song
{"title":"Sulfonated poly(ether-ether-ketone) membranes with intrinsic microporosity enable efficient redox flow batteries for energy storage","authors":"Toby Wong, Yijie Yang, Rui Tan, Anqi Wang, Zhou Zhou, Zhizhang Yuan, Jiaxi Li, Dezhi Liu, Alberto Alvarez-Fernandez, Chunchun Ye, Mark Sankey, David Ainsworth, Stefan Guldin, Fabrizia Foglia, Neil B. McKeown, Kim E. Jelfs, Xianfeng Li, Qilei Song","doi":"10.1016/j.joule.2024.101814","DOIUrl":"10.1016/j.joule.2024.101814","url":null,"abstract":"","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 2","pages":"Article 101814"},"PeriodicalIF":38.6,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142908360","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
JoulePub Date : 2025-02-19DOI: 10.1016/j.joule.2024.12.006
Yifan Gao , Ming Lei , Bachu Sravan Kumar , Hugh Barrett Smith , Seok Hee Han , Lokesh Sangabattula , Ju Li , Iwnetim I. Abate
{"title":"Geological ammonia: Stimulated NH3 production from rocks","authors":"Yifan Gao , Ming Lei , Bachu Sravan Kumar , Hugh Barrett Smith , Seok Hee Han , Lokesh Sangabattula , Ju Li , Iwnetim I. Abate","doi":"10.1016/j.joule.2024.12.006","DOIUrl":"10.1016/j.joule.2024.12.006","url":null,"abstract":"<div><div>Although ammonia production is crucial for global agriculture, it comes with substantial carbon footprints. Here, for the first time, we propose and demonstrate a different method for stimulated (proactive) and <em>in situ</em> geological ammonia (Geo-NH<sub>3</sub>) production directly from rocks. Our approach demonstrated that NH<sub>3</sub> can be efficiently generated by reacting natural (Fe,Mg)<sub>2</sub>SiO<sub>4</sub> (olivine) minerals with nitrate-source water at 130°C–300°C and 0.25–8.5 MPa, and even at ambient temperature and pressure. Using both actual rocks and synthetic mineral Fe(OH)<sub>2</sub>, we investigated mechanisms and optimized conditions through experiments and theoretical calculations. We revealed the basic chemistry enabling Geo-NH<sub>3</sub> production: Fe<sup>2+</sup> contained in rocks reduces the nitrate source to NH<sub>3</sub>. Our approach, involving only the injection of nitrate-source water into the subsurface to utilize <em>in situ</em> subsurface heat and pressure, requires no external H<sub>2</sub> or electric current and emits no direct CO<sub>2</sub>, offering a feasible alternative to sustainable NH<sub>3</sub> production at scale.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 2","pages":"Article 101805"},"PeriodicalIF":38.6,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991188","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
JoulePub Date : 2025-02-19DOI: 10.1016/j.joule.2025.101848
Wenjie Shao , Shuang Li
{"title":"Tandem electrochemical hydrogen pumps with ion-pair membranes","authors":"Wenjie Shao , Shuang Li","doi":"10.1016/j.joule.2025.101848","DOIUrl":"10.1016/j.joule.2025.101848","url":null,"abstract":"<div><div>The low H<sub>2</sub> concentration in most natural gas pipelines poses challenges, leading to high separation/compression costs. In a recent issue of <em>Nature Energy</em>, Kim and co-workers demonstrated a tandem electrochemical hydrogen pump system that reveals high-purity and low-cost H<sub>2</sub> extraction from mixtures, providing a possibility for transport from H<sub>2</sub> stations to end users.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 2","pages":"Article 101848"},"PeriodicalIF":38.6,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143445326","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}