Sodium-ion batteries (SIBs) present a resource-sustainable and cost-efficient paradigm poised to overcome the limitation of relying solely on lithium-ion technologies for emerging large-scale energy storage. Yet, the path of SIBs to full commercialization is hindered by unresolved uncertainties regarding thermal safety and lingering debates over the origin of thermal runaway. Herein, through multiscale equivalent analysis from Ah-grade cells to microstructures of battery components, we probe that the difference in the chemical environment for cation storage in anodes is the mechanistic origin underlying the inferior thermal safety of SIBs compared to lithium-ion batteries (LIBs). Bearing a quasi-metallic nature, sodium clusters that form in hard carbon (HC) anodes during routine sodiation predominantly initiate cell self-exothermic reactions, significantly earlier than the decomposition of the solid–electrolyte interphase (SEI) typically observed in LIBs. Solid-state NMR measurements elucidate that clustered sodium in HC exhibits electronic properties more akin to metallic states than lithium in graphite, with even higher electron state densities at the Fermi level than bulk sodium. This heightened reactivity triggers the decomposition of linear carbonates, ultimately culminating in a thermal runaway event almost on par with scenarios involving sodium plating. Our work challenges the prevailing brief that the thermal safety insights between LIBs and SIBs are interchangeable and highlights the necessity of stabilizing deeply sodiated HC for practically safe sodium-based battery chemistries.
{"title":"Sodium cluster-driven safety concerns of sodium-ion batteries","authors":"Jiaping Niu, Junyuan Dong, Xiaohu Zhang, Lang Huang, Guoli Lu, Xiaolei Han, Jinzhi Wang, Tianyu Gong, Zheng Chen, Jingwen Zhao, Guanglei Cui","doi":"10.1039/d4ee05509h","DOIUrl":"https://doi.org/10.1039/d4ee05509h","url":null,"abstract":"Sodium-ion batteries (SIBs) present a resource-sustainable and cost-efficient paradigm poised to overcome the limitation of relying solely on lithium-ion technologies for emerging large-scale energy storage. Yet, the path of SIBs to full commercialization is hindered by unresolved uncertainties regarding thermal safety and lingering debates over the origin of thermal runaway. Herein, through multiscale equivalent analysis from Ah-grade cells to microstructures of battery components, we probe that the difference in the chemical environment for cation storage in anodes is the mechanistic origin underlying the inferior thermal safety of SIBs compared to lithium-ion batteries (LIBs). Bearing a quasi-metallic nature, sodium clusters that form in hard carbon (HC) anodes during routine sodiation predominantly initiate cell self-exothermic reactions, significantly earlier than the decomposition of the solid–electrolyte interphase (SEI) typically observed in LIBs. Solid-state NMR measurements elucidate that clustered sodium in HC exhibits electronic properties more akin to metallic states than lithium in graphite, with even higher electron state densities at the Fermi level than bulk sodium. This heightened reactivity triggers the decomposition of linear carbonates, ultimately culminating in a thermal runaway event almost on par with scenarios involving sodium plating. Our work challenges the prevailing brief that the thermal safety insights between LIBs and SIBs are interchangeable and highlights the necessity of stabilizing deeply sodiated HC for practically safe sodium-based battery chemistries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"61 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143083138","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}
Shizi Luo, Shuguang Cao, Tongjun Zheng, Zhuoneng Bi, Yupeng Zheng, Yiqun Li, Biniyam Zemene Taye, Victoria V. Ozerova, Lyubov A. Frolova, Nikita A. Emelianov, Eugeniy D. Tarasov, Zheng Liang, Lavrenty G. Gutsev, Sergey M. Aldoshin, Bala R. Ramachandran, Pavel A. Troshin, Xueqing Xu
It is now well-known that moderate amounts of lead iodide (PbI2) in organic–inorganic hybrid perovskite films are capable of passivating defects and stabilizing the material. However, contrarily, excessive PbI2 instead leads to rapid degradation and thus destabilizes the perovskite solar cells (PSCs). To address this challenge, we propose to use melamine (MEA) additive to control the concentration of PbI2 in perovskite films fabricated with sequential deposition method. As demonstrated by our calculations and NMR measurement results, MEA has both donor and acceptor regions which combine well with the PbI2's surface topology: the triazine core units are capable of binding to uncoordinated lead while the amino groups of MEA are capable of coordinating with the iodide anions and effectively “trichelate” PbI2, thus passivating the defects and promoting carrier separation. Furthermore, the simultaneous introduction of MEA and cesium iodide regulated the crystallization of perovskite films, improved the degree of (111) crystal orientation, and enabled the formation of high-quality perovskite films without pinholes. As such, based on the synergistic effect of MEA and cesium iodide, we prepared inverted PSCs by sequential deposition method with a PCE of 25.66% (certified at 25.06%) and high VOC approaching 1.2 V with a steady state PCE of 25.19%. The optimized device can maintain more than 90% of the initial efficiency at the maximum power point for 1000 h. In addition, through this strategy, we also prepared a flexible device with an efficiency of up to 24.03%, which can maintain more than 90% of the initial performance after 5000 bending cycles, thus demonstrating an excellent mechanical stability.
{"title":"Melamine holding PbI2 with three “arms”: an effective chelation strategy to control the lead iodide to perovskite conversion for inverted perovskite solar cells","authors":"Shizi Luo, Shuguang Cao, Tongjun Zheng, Zhuoneng Bi, Yupeng Zheng, Yiqun Li, Biniyam Zemene Taye, Victoria V. Ozerova, Lyubov A. Frolova, Nikita A. Emelianov, Eugeniy D. Tarasov, Zheng Liang, Lavrenty G. Gutsev, Sergey M. Aldoshin, Bala R. Ramachandran, Pavel A. Troshin, Xueqing Xu","doi":"10.1039/d4ee04692g","DOIUrl":"https://doi.org/10.1039/d4ee04692g","url":null,"abstract":"It is now well-known that moderate amounts of lead iodide (PbI<small><sub>2</sub></small>) in organic–inorganic hybrid perovskite films are capable of passivating defects and stabilizing the material. However, contrarily, excessive PbI<small><sub>2</sub></small> instead leads to rapid degradation and thus destabilizes the perovskite solar cells (PSCs). To address this challenge, we propose to use melamine (MEA) additive to control the concentration of PbI<small><sub>2</sub></small> in perovskite films fabricated with sequential deposition method. As demonstrated by our calculations and NMR measurement results, MEA has both donor and acceptor regions which combine well with the PbI<small><sub>2</sub></small>'s surface topology: the triazine core units are capable of binding to uncoordinated lead while the amino groups of MEA are capable of coordinating with the iodide anions and effectively “trichelate” PbI<small><sub>2</sub></small>, thus passivating the defects and promoting carrier separation. Furthermore, the simultaneous introduction of MEA and cesium iodide regulated the crystallization of perovskite films, improved the degree of (111) crystal orientation, and enabled the formation of high-quality perovskite films without pinholes. As such, based on the synergistic effect of MEA and cesium iodide, we prepared inverted PSCs by sequential deposition method with a PCE of 25.66% (certified at 25.06%) and high <em>V</em><small><sub>OC</sub></small> approaching 1.2 V with a steady state PCE of 25.19%. The optimized device can maintain more than 90% of the initial efficiency at the maximum power point for 1000 h. In addition, through this strategy, we also prepared a flexible device with an efficiency of up to 24.03%, which can maintain more than 90% of the initial performance after 5000 bending cycles, thus demonstrating an excellent mechanical stability.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"31 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077375","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}
A novel asymmetric acceptor, M36-FCl, has been developed by chemically hybridizing two symmetric M-series acceptors: one with fluorinated terminal groups (M36F) and the other with chlorinated terminal groups (M36Cl). This asymmetric acceptor is systematically compared with an alloy-like composite formed by physically blending M36F with M36Cl to elucidate the advantages and limitations of the two strategies (chemical hybridization versus physical blending) in enhancing the photovoltaic performance of polymer solar cells (PSCs). Due to its asymmetric molecular structure, M36-FCl exhibits a large dipole moment and therefore has a higher relative dielectric constant of 4.85 compared to the composite acceptor (3.01). This higher dielectric constant can lower the energy barrier for exciton dissociation into free charges of the resulting devices. More importantly, the PM6:M36-FCl binary blend exhibits a more favorable morphology with improved crystallinity compared with the PM6:M36F:M36Cl ternary blend, resulting in reduced charge recombination and improved charge transport. Consequently, the optimal M36-FCl-based PSC achieves a power conversion efficiency (PCE) of 18.51%, surpassing the performance of the M36F:M36Cl-based counterpart, which has a PCE of 17.57%. The 18.51% PCE is the highest reported value among all ADA-type non-fullerene acceptors (NFAs), highlighting the significant potential of the chemical hybridization strategy for tuning the properties of NFAs to enhance PSC performance.
{"title":"Strategies to Improve the Photovoltaic Performance of M-Series Acceptor-Based Polymer Solar Cells: Chemical Hybridization Versus Physical Blending of Acceptors","authors":"Haiting Shi, Hui Guo, Dongdong Cai, Jin-Yun Wang, Yunlong Ma, Qingdong Zheng","doi":"10.1039/d5ee00294j","DOIUrl":"https://doi.org/10.1039/d5ee00294j","url":null,"abstract":"A novel asymmetric acceptor, M36-FCl, has been developed by chemically hybridizing two symmetric M-series acceptors: one with fluorinated terminal groups (M36F) and the other with chlorinated terminal groups (M36Cl). This asymmetric acceptor is systematically compared with an alloy-like composite formed by physically blending M36F with M36Cl to elucidate the advantages and limitations of the two strategies (chemical hybridization versus physical blending) in enhancing the photovoltaic performance of polymer solar cells (PSCs). Due to its asymmetric molecular structure, M36-FCl exhibits a large dipole moment and therefore has a higher relative dielectric constant of 4.85 compared to the composite acceptor (3.01). This higher dielectric constant can lower the energy barrier for exciton dissociation into free charges of the resulting devices. More importantly, the PM6:M36-FCl binary blend exhibits a more favorable morphology with improved crystallinity compared with the PM6:M36F:M36Cl ternary blend, resulting in reduced charge recombination and improved charge transport. Consequently, the optimal M36-FCl-based PSC achieves a power conversion efficiency (PCE) of 18.51%, surpassing the performance of the M36F:M36Cl-based counterpart, which has a PCE of 17.57%. The 18.51% PCE is the highest reported value among all ADA-type non-fullerene acceptors (NFAs), highlighting the significant potential of the chemical hybridization strategy for tuning the properties of NFAs to enhance PSC performance.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"6 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077373","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}
Leiqian Zhang, Han Ding, Haiqi Gao, Jiaming Gong, Hele Guo, Shuoqing Zhang, Yi Yu, Guanjie He, Tao Deng, Ivan P. Parkin, Johan Hofkens, Xiulin Fan, Feili Lai, Tianxi Liu
Zinc–iodine batteries (ZIBs) have long struggled with the uncontrolled spread of polyiodide in aqueous electrolytes, despite their environmentally friendly, inherently safe, and cost-effective nature. Here, we present an integral redesign of ZIBs that encompasses both the electrolyte and cell structure. The developed self-sieving polyiodide-capable liquid–liquid biphasic electrolyte can achieve an impressive polyiodide extraction efficiency of 99.98%, harnessing a meticulously iodine-containing hydrophobic solvated shell in conjunction with the salt-out effect. This advancement facilitates a membrane-free design with a Coulombic efficiency of ∼100% at 0.1C, alongside an ultra-low self-discharge rate of ∼3.4% per month and capacity retention of 83.1% after 1300 cycles (iodine areal loading: 22.2 mg cm−2). Furthermore, the integrated cell structure, paired with the low-cost electrolyte ($4.6 L−1), enables rapid assembly into A h-level batteries within hours (1.18 A h after 100 cycles with a capacity retention of 86.7%), supports electrolyte regeneration with ∼100% recycling efficiency, and extends to ZIBs with a two-electron iodine conversion reaction. This endeavor establishes a novel paradigm for the development of practical zinc–iodine batteries.
{"title":"An integrated design for high-energy, durable zinc–iodine batteries with ultra-high recycling efficiency","authors":"Leiqian Zhang, Han Ding, Haiqi Gao, Jiaming Gong, Hele Guo, Shuoqing Zhang, Yi Yu, Guanjie He, Tao Deng, Ivan P. Parkin, Johan Hofkens, Xiulin Fan, Feili Lai, Tianxi Liu","doi":"10.1039/d4ee05873a","DOIUrl":"https://doi.org/10.1039/d4ee05873a","url":null,"abstract":"Zinc–iodine batteries (ZIBs) have long struggled with the uncontrolled spread of polyiodide in aqueous electrolytes, despite their environmentally friendly, inherently safe, and cost-effective nature. Here, we present an integral redesign of ZIBs that encompasses both the electrolyte and cell structure. The developed self-sieving polyiodide-capable liquid–liquid biphasic electrolyte can achieve an impressive polyiodide extraction efficiency of 99.98%, harnessing a meticulously iodine-containing hydrophobic solvated shell in conjunction with the salt-out effect. This advancement facilitates a membrane-free design with a Coulombic efficiency of ∼100% at 0.1C, alongside an ultra-low self-discharge rate of ∼3.4% per month and capacity retention of 83.1% after 1300 cycles (iodine areal loading: 22.2 mg cm<small><sup>−2</sup></small>). Furthermore, the integrated cell structure, paired with the low-cost electrolyte ($4.6 L<small><sup>−1</sup></small>), enables rapid assembly into A h-level batteries within hours (1.18 A h after 100 cycles with a capacity retention of 86.7%), supports electrolyte regeneration with ∼100% recycling efficiency, and extends to ZIBs with a two-electron iodine conversion reaction. This endeavor establishes a novel paradigm for the development of practical zinc–iodine batteries.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"5 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143077372","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}
Additives with strong adsorption energies coordinate with lead ions and reduce halogen vacancy defects, leading to a highly ordered atomic arrangement of the lattices and grain boundary mitigation of the perovskite for efficient perovskite solar cells (PSCs). Herein, we demonstrate efficient rigid and flexible PSCs via 1,3,5-triazine-2,4-diamine hydrochloride (TDH) passivation. This molecular passivation improves the perovskite crystallinity through reducing the aligned point vacancy defects, dislocations and distortions of the lattices. It also restrains the formation of small twin crystals through mitigating the grain boundaries. The rigid PSCs yield a PCE of 26.15% with a fill factor (FF) of 85.94%. The flexible PSCs yield a PCE of 24.68% with a FF of 86.07%. Both devices exhibit superior operational stability. The work provides a passivation strategy and valuable insights for crystalline perovskite materials and high-performance PSCs.
{"title":"Efficient rigid and flexible perovskite solar cells using strongly adsorbed molecules for lattice repair and grain boundary mitigation","authors":"Xi Fan, Jiwen Chen, Jinzhao Wang, Jing Wang, Jixi Zeng, Feng Wei, Shuai Gao, Jia Li, Jing Zhang, Feng Yan, Weijie Song","doi":"10.1039/d4ee05232c","DOIUrl":"https://doi.org/10.1039/d4ee05232c","url":null,"abstract":"Additives with strong adsorption energies coordinate with lead ions and reduce halogen vacancy defects, leading to a highly ordered atomic arrangement of the lattices and grain boundary mitigation of the perovskite for efficient perovskite solar cells (PSCs). Herein, we demonstrate efficient rigid and flexible PSCs via 1,3,5-triazine-2,4-diamine hydrochloride (TDH) passivation. This molecular passivation improves the perovskite crystallinity through reducing the aligned point vacancy defects, dislocations and distortions of the lattices. It also restrains the formation of small twin crystals through mitigating the grain boundaries. The rigid PSCs yield a PCE of 26.15% with a fill factor (FF) of 85.94%. The flexible PSCs yield a PCE of 24.68% with a FF of 86.07%. Both devices exhibit superior operational stability. The work provides a passivation strategy and valuable insights for crystalline perovskite materials and high-performance PSCs.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"60 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-01-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143072113","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Perovskite solar cells (PSCs) as new-generation photovoltaic cells have received remarkable interests due to the facile fabrication procedures and superb power conversion efficiencies (PCEs). Nevertheless, the widely used noble metal-based rear electrodes such as Ag and Au in PSCs suffer from the relatively high material costs and instability induced by halide anion degradation reaction, strongly hindering the practical applications of PSCs. Consequently, carbon-based materials are considered as one of the most encouraging candidates to substitute noble metals as rear electrodes due to the cost effectiveness, superior physical/chemical stability, superb structural flexibility and diverse/easily tuned properties to realize low-cost and highly robust PSCs. However, the carbon electrode-based PSCs still suffer from the much inferior PCEs to the noble metal-based counterparts due to the insufficient carrier transfer capability and inferior interface contact. In this paper, the recent advancements about the design and fabrication of advanced carbon-based rear electrodes for low-cost and efficient PSCs are reviewed by highlighting the unique merits of carbon-based rear electrodes over metal/metal oxide-based counterparts. Several distinct strategies are also proposed to improve the PCEs and durability of carbon electrode-based PSCs. Lastly, the current challenges and future directions of carbon rear electrode-based PSCs are also highlighted and discussed, intending to present vital insights for the future development of low-cost carbon-based PSCs towards the scalable production and widespread applications of this technology.
{"title":"Advanced carbon-based rear electrodes for low-cost and efficient perovskite solar cells","authors":"Jingsheng He, Yu Bai, Zhixin (Veela) Luo, Ran Ran, Wei Zhou, Wei Wang, Zongping Shao","doi":"10.1039/d4ee05462h","DOIUrl":"https://doi.org/10.1039/d4ee05462h","url":null,"abstract":"Perovskite solar cells (PSCs) as new-generation photovoltaic cells have received remarkable interests due to the facile fabrication procedures and superb power conversion efficiencies (PCEs). Nevertheless, the widely used noble metal-based rear electrodes such as Ag and Au in PSCs suffer from the relatively high material costs and instability induced by halide anion degradation reaction, strongly hindering the practical applications of PSCs. Consequently, carbon-based materials are considered as one of the most encouraging candidates to substitute noble metals as rear electrodes due to the cost effectiveness, superior physical/chemical stability, superb structural flexibility and diverse/easily tuned properties to realize low-cost and highly robust PSCs. However, the carbon electrode-based PSCs still suffer from the much inferior PCEs to the noble metal-based counterparts due to the insufficient carrier transfer capability and inferior interface contact. In this paper, the recent advancements about the design and fabrication of advanced carbon-based rear electrodes for low-cost and efficient PSCs are reviewed by highlighting the unique merits of carbon-based rear electrodes over metal/metal oxide-based counterparts. Several distinct strategies are also proposed to improve the PCEs and durability of carbon electrode-based PSCs. Lastly, the current challenges and future directions of carbon rear electrode-based PSCs are also highlighted and discussed, intending to present vital insights for the future development of low-cost carbon-based PSCs towards the scalable production and widespread applications of this technology.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"11 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143056728","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}
Lithium-ion batteries (LIBs) are highly sensitive to cycling conditions and show a nonlinear degradation pattern, typically noticeable in later stages. This affects the accuracy of most battery health prognostic models, especially those relying on long-term data collected under varying operational conditions. To tackle these challenges, we propose using statistical features extracted from the battery surface temperature during the first 10 cycles and developing a data-driven machine learning (ML) model for early-cycle lifetime prediction. Models are trained on each of the selected open-source datasets comprising 223 LIBs and tested on their respective datasets with non-stratified data splits using a balanced ratio. These datasets include lithium iron phosphate (LFP), nickel cobalt aluminum oxide (NCA), and nickel manganese cobalt oxide (NMC) cells, tested under different environmental temperatures and cycling protocols. In one comprehensive dataset, our model achieved competitive performance compared to state-of-the-art studies that rely on features extracted from much longer cycling data—up to ten times the duration. This work provides valuable insights into the strong correlation between early-cycle surface temperature and battery lifetime across various battery chemistries, cycling rates, and environmental temperatures.
{"title":"Battery Lifetime Prediction Using Surface Temperature Features from Early Cycle Data","authors":"Lawnardo Sugiarto, Zijie Huang, Yi-Chun Lu","doi":"10.1039/d4ee05179c","DOIUrl":"https://doi.org/10.1039/d4ee05179c","url":null,"abstract":"Lithium-ion batteries (LIBs) are highly sensitive to cycling conditions and show a nonlinear degradation pattern, typically noticeable in later stages. This affects the accuracy of most battery health prognostic models, especially those relying on long-term data collected under varying operational conditions. To tackle these challenges, we propose using statistical features extracted from the battery surface temperature during the first 10 cycles and developing a data-driven machine learning (ML) model for early-cycle lifetime prediction. Models are trained on each of the selected open-source datasets comprising 223 LIBs and tested on their respective datasets with non-stratified data splits using a balanced ratio. These datasets include lithium iron phosphate (LFP), nickel cobalt aluminum oxide (NCA), and nickel manganese cobalt oxide (NMC) cells, tested under different environmental temperatures and cycling protocols. In one comprehensive dataset, our model achieved competitive performance compared to state-of-the-art studies that rely on features extracted from much longer cycling data—up to ten times the duration. This work provides valuable insights into the strong correlation between early-cycle surface temperature and battery lifetime across various battery chemistries, cycling rates, and environmental temperatures.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"23 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143056729","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}
Efficient and cost-effective recovery technologies are needed to harvest the abundant energy stored in low-grade heat sources (＜ 100 °C). Thermally regenerative electrochemical cycle (TREC) is a promising approach for low-grade heat harvesting with high energy conversion efficiency. Here, we achieved co-optimization of temperature coefficient (−3.96 mV K−1), specific charge capacity (theoretical, 97.36 Ah L−1) and specific heat capacity in TREC by applying a thermosensitive slurry electrolyte system, in which Fe(CN)64−-based thermosensitive crystallization were incorporated into the Fe(CN)63−/4− solution. We demonstrated an electrically assisted TREC system with Fe(CN)63−/4− catholyte and an Ag/AgCl anode, and a charging-free TREC system with Fe(CN)63−/4− catholyte and I3−/I− anolyte. Both two systems perform high absolute heat-to-electricity energy conversion efficiency of 4.42% and 2.51%, respectively, in the absence of heat recuperation. This study provides a general approach of electrolyte design aimed at enhancing temperature coefficient and specific charge capacity, while simultaneously optimizing specific heat capacity, thereby facilitating the development of more efficient TREC systems.
{"title":"Thermosensitive slurry electrolyte design for efficient electrochemical heat harvesting","authors":"Pei Liu, Boyang Yu, Yilin Zeng, Yifan Zhang, Xuan Cai, Xue Long, Hua Jiang, Wendong Yang, Shuangyan Gui, Jinhua Guo, Jia Li, Jun Zhou, Jiangjiang Duan","doi":"10.1039/d4ee04976d","DOIUrl":"https://doi.org/10.1039/d4ee04976d","url":null,"abstract":"Efficient and cost-effective recovery technologies are needed to harvest the abundant energy stored in low-grade heat sources (＜ 100 °C). Thermally regenerative electrochemical cycle (TREC) is a promising approach for low-grade heat harvesting with high energy conversion efficiency. Here, we achieved co-optimization of temperature coefficient (−3.96 mV K<small><sup>−1</sup></small>), specific charge capacity (theoretical, 97.36 Ah L<small><sup>−1</sup></small>) and specific heat capacity in TREC by applying a thermosensitive slurry electrolyte system, in which Fe(CN)<small><sub>6</sub></small><small><sup>4−</sup></small>-based thermosensitive crystallization were incorporated into the Fe(CN)<small><sub>6</sub></small><small><sup>3−/4−</sup></small> solution. We demonstrated an electrically assisted TREC system with Fe(CN)<small><sub>6</sub></small><small><sup>3−/4−</sup></small> catholyte and an Ag/AgCl anode, and a charging-free TREC system with Fe(CN)<small><sub>6</sub></small><small><sup>3−/4−</sup></small> catholyte and I<small><sub>3</sub></small><small><sup>−</sup></small>/I<small><sup>−</sup></small> anolyte. Both two systems perform high absolute heat-to-electricity energy conversion efficiency of 4.42% and 2.51%, respectively, in the absence of heat recuperation. This study provides a general approach of electrolyte design aimed at enhancing temperature coefficient and specific charge capacity, while simultaneously optimizing specific heat capacity, thereby facilitating the development of more efficient TREC systems.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"35 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055645","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}
Zishuai Zhang, Aubry S. R. Williams, Shaoxuan Ren, Benjamin A. W. Mowbray, Colin T. E. Parkyn, Yongwook Kim, Tengxiao Ji, Curtis P. Berlinguette
Electrochemical reactors can reduce the carbon intensity of cement production by using electricity to convert limestone (CaCO3) into Ca(OH)2, which can be converted into cement clinker by reacting with silica (SiO2) at high temperatures. A key challenge with electrochemical reactors is that the deposition of solid Ca(OH)2 at the membrane leads to unacceptably low energy efficiencies. To address this challenge, we connected the electrochemical reactor used for limestone calcination (“cement electrolyser”) to a distinctive chemical reactor (“calcium reactor”) so that Ca(OH)2 forms in the calcium reactor instead of within the electrochemical reactor. In this tandem system, the cement electrolyser generates H+ and OH− in the respective chemical and cathode compartments. The H+ then reacts with CaCO3 to release Ca2+, which is diverted into the calcium reactor to react with the OH− to form Ca(OH)2. We fabricated a composite membrane to selectively block the transport of Ca2+ into the cathode compartment. Charge balance in the cement electrolyser was enabled with monovalent ions (e.g., K+) as the positive charge carrier. This orthogonalized ion management was validated by operando imaging. The tandem reactor enabled the electrolysis process to operate for 50 hours at 100 mA cm−2 without any voltage increase, which represents a meaningful step forward for electrochemical cement clinker precursor production.
{"title":"Electrolytic cement clinker precursor production sustained through orthogonalization of ion vectors","authors":"Zishuai Zhang, Aubry S. R. Williams, Shaoxuan Ren, Benjamin A. W. Mowbray, Colin T. E. Parkyn, Yongwook Kim, Tengxiao Ji, Curtis P. Berlinguette","doi":"10.1039/d4ee04881d","DOIUrl":"https://doi.org/10.1039/d4ee04881d","url":null,"abstract":"Electrochemical reactors can reduce the carbon intensity of cement production by using electricity to convert limestone (CaCO<small><sub>3</sub></small>) into Ca(OH)<small><sub>2</sub></small>, which can be converted into cement clinker by reacting with silica (SiO<small><sub>2</sub></small>) at high temperatures. A key challenge with electrochemical reactors is that the deposition of solid Ca(OH)<small><sub>2</sub></small> at the membrane leads to unacceptably low energy efficiencies. To address this challenge, we connected the electrochemical reactor used for limestone calcination (“cement electrolyser”) to a distinctive chemical reactor (“calcium reactor”) so that Ca(OH)<small><sub>2</sub></small> forms in the calcium reactor instead of within the electrochemical reactor. In this tandem system, the cement electrolyser generates H<small><sup>+</sup></small> and OH<small><sup>−</sup></small> in the respective chemical and cathode compartments. The H<small><sup>+</sup></small> then reacts with CaCO<small><sub>3</sub></small> to release Ca<small><sup>2+</sup></small>, which is diverted into the calcium reactor to react with the OH<small><sup>−</sup></small> to form Ca(OH)<small><sub>2</sub></small>. We fabricated a composite membrane to selectively block the transport of Ca<small><sup>2+</sup></small> into the cathode compartment. Charge balance in the cement electrolyser was enabled with monovalent ions (<em>e.g.</em>, K<small><sup>+</sup></small>) as the positive charge carrier. This orthogonalized ion management was validated by <em>operando</em> imaging. The tandem reactor enabled the electrolysis process to operate for 50 hours at 100 mA cm<small><sup>−2</sup></small> without any voltage increase, which represents a meaningful step forward for electrochemical cement clinker precursor production.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"79 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143056740","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}
Zhenzhen Qin, Mengjiong Chen, Ziyang Zhang, Yanbo Wang, Liyuan Han
High-quality crystallization is the most effective way to eliminate high-dimensional defects. However, it remains a critical challenge for the perovskites grown on self-assembled monolayers. Here, a double-side treatment strategy is proposed and a tailor-made 4-fluoro-2-methoxybenzonitrile is used to maximize the difference in the nucleation driving force between top and bottom sides of perovskite, resulting in upward unidirectional perovskite crystallization. The high-dimensional defects of transverse grain boundaries, buried voids and amorphous regions are all eliminated, contributing to a power conversion efficiency of 26.4% (certified 26.0%). In addition, the encapsulated devices exhibited superior stability following ISOS-D-3 and ISOS-L-2 protocols, respectively.
{"title":"Eliminating high-dimensional defects by upward unidirectional crystallization for efficient and stable inverted perovskite solar cells","authors":"Zhenzhen Qin, Mengjiong Chen, Ziyang Zhang, Yanbo Wang, Liyuan Han","doi":"10.1039/d4ee05968a","DOIUrl":"https://doi.org/10.1039/d4ee05968a","url":null,"abstract":"High-quality crystallization is the most effective way to eliminate high-dimensional defects. However, it remains a critical challenge for the perovskites grown on self-assembled monolayers. Here, a double-side treatment strategy is proposed and a tailor-made 4-fluoro-2-methoxybenzonitrile is used to maximize the difference in the nucleation driving force between top and bottom sides of perovskite, resulting in upward unidirectional perovskite crystallization. The high-dimensional defects of transverse grain boundaries, buried voids and amorphous regions are all eliminated, contributing to a power conversion efficiency of 26.4% (certified 26.0%). In addition, the encapsulated devices exhibited superior stability following ISOS-D-3 and ISOS-L-2 protocols, respectively.","PeriodicalId":72,"journal":{"name":"Energy & Environmental Science","volume":"74 1","pages":""},"PeriodicalIF":32.5,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055642","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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