Pub Date : 2025-09-17DOI: 10.1016/j.joule.2025.102074
Xinyang Che , Lijun Liu , Wei He
Meeting net-zero targets is challenging, as terrestrial renewables face intermittency and regional constraints. Here, we assess space-based solar power, a near-constant source, using a high-resolution, Europe-wide capacity-expansion and dispatch model. We assess two advanced designs: (1) a near-baseload, low-TRL (technology readiness level) heliostat design and (2) a partially intermittent, higher-TRL planar design, using NASA’s 2050 forecast. We find that the heliostat design can cut total system costs by 7%–15%, offset up to 80% of wind and solar, and reduce battery usage by over 70%, although hydrogen remains vital for seasonal balancing. The planar design, by contrast, is uneconomical at its forecast costs. Sensitivity analyses reveal relative cost thresholds for both designs, at which space-based solar shifts from cost-prohibitive to complementary and ultimately to a dominant baseload source for net-zero transitions. These results provide robust techno-economic benchmarks, highlighting new net-zero pathways and guiding policymakers and industry toward large-scale, low-intermittency renewables.
{"title":"Assess space-based solar power for European-scale power system decarbonization","authors":"Xinyang Che , Lijun Liu , Wei He","doi":"10.1016/j.joule.2025.102074","DOIUrl":"10.1016/j.joule.2025.102074","url":null,"abstract":"<div><div>Meeting net-zero targets is challenging, as terrestrial renewables face intermittency and regional constraints. Here, we assess space-based solar power, a near-constant source, using a high-resolution, Europe-wide capacity-expansion and dispatch model. We assess two advanced designs: (1) a near-baseload, low-TRL (technology readiness level) heliostat design and (2) a partially intermittent, higher-TRL planar design, using NASA’s 2050 forecast. We find that the heliostat design can cut total system costs by 7%–15%, offset up to 80% of wind and solar, and reduce battery usage by over 70%, although hydrogen remains vital for seasonal balancing. The planar design, by contrast, is uneconomical at its forecast costs. Sensitivity analyses reveal relative cost thresholds for both designs, at which space-based solar shifts from cost-prohibitive to complementary and ultimately to a dominant baseload source for net-zero transitions. These results provide robust techno-economic benchmarks, highlighting new net-zero pathways and guiding policymakers and industry toward large-scale, low-intermittency renewables.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 9","pages":"Article 102074"},"PeriodicalIF":35.4,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144901300","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 : 2025-09-17DOI: 10.1016/j.joule.2025.102058
Chenyang Wei , Cheng Liu , Zeyu Zhang , Kai Sun , Chengkun Xing , Wenjuan Shi , Youyong Li , Jian-Feng Li , Bo Zhang
Enhancing current density is a crucial strategy for reducing costs and improving the efficiency of green hydrogen production through water electrolysis. However, mass diffusion and proton transport limitations under high-current densities remain serious obstacles. Here, we proposed a novel strategy to construct a three-dimensional mesoporous skeleton structure of IrO2 to address the limitations. By utilizing the dynamic loading of Ir nanoparticles during the La2O3 template reconstruction process, high-density embedding of ultra-small Ir nanoparticles in the template is achieved. During the electrochemical process, in situ oxidation of Ir nanoparticles combined with template leaching results in the formation of a three-dimensional, mesoporous IrO2 structure. The developed catalyst enables proton exchange membrane water electrolysis (PEMWE) to achieve stable operation for over 2,700 h at a current density of 5 A cm−2 with a voltage degradation rate of ∼0.38 μV h−1, which meets the 2030 EU Clean Hydrogen JU target and 2026 US Department of Energy (DOE) target.
提高电流密度是降低水电解绿色制氢成本和提高效率的关键策略。然而，在高电流密度下的质量扩散和质子输运限制仍然是严重的障碍。在此，我们提出了一种新的策略来构建三维介孔IrO2骨架结构，以解决这些限制。利用La2O3模板重构过程中Ir纳米颗粒的动态加载，实现了超小Ir纳米颗粒在La2O3模板中的高密度嵌入。在电化学过程中，Ir纳米颗粒的原位氧化结合模板浸出导致三维介孔IrO2结构的形成。该催化剂可使质子交换膜电解（PEMWE）在5 a cm−2的电流密度下稳定运行2700小时以上，电压降解率为0.38 μV h−1，满足2030年欧盟清洁氢JU目标和2026年美国能源部（DOE）目标。
{"title":"Dynamic template reconstruction induced mesoporous iridium catalysts for high-current-density PEMWE","authors":"Chenyang Wei , Cheng Liu , Zeyu Zhang , Kai Sun , Chengkun Xing , Wenjuan Shi , Youyong Li , Jian-Feng Li , Bo Zhang","doi":"10.1016/j.joule.2025.102058","DOIUrl":"10.1016/j.joule.2025.102058","url":null,"abstract":"<div><div>Enhancing current density is a crucial strategy for reducing costs and improving the efficiency of green hydrogen production through water electrolysis. However, mass diffusion and proton transport limitations under high-current densities remain serious obstacles. Here, we proposed a novel strategy to construct a three-dimensional mesoporous skeleton structure of IrO<sub>2</sub> to address the limitations. By utilizing the dynamic loading of Ir nanoparticles during the La<sub>2</sub>O<sub>3</sub> template reconstruction process, high-density embedding of ultra-small Ir nanoparticles in the template is achieved. During the electrochemical process, <em>in situ</em> oxidation of Ir nanoparticles combined with template leaching results in the formation of a three-dimensional, mesoporous IrO<sub>2</sub> structure. The developed catalyst enables proton exchange membrane water electrolysis (PEMWE) to achieve stable operation for over 2,700 h at a current density of 5 A cm<sup>−2</sup> with a voltage degradation rate of ∼0.38 μV h<sup>−1</sup>, which meets the 2030 EU Clean Hydrogen JU target and 2026 US Department of Energy (DOE) target.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 9","pages":"Article 102058"},"PeriodicalIF":35.4,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144756661","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 : 2025-09-17DOI: 10.1016/j.joule.2025.102091
Licheng Lou , Jinlin Wang , Yuan Li , Kang Yin , Xiao Xu , Bowen Zhang , Menghan Jiao , Shudan Chen , Tan Guo , Jingchen Wang , Yiming Li , Jiangjian Shi , Huijue Wu , Ruijuan Xiao , Hao Xin , Yanhong Luo , Dongmei Li , Qingbo Meng
The interface contact issue, surface defects, and energy level mismatches have significantly limited the optoelectronic performance of solution-processed transparent conductive window layers for use in thin-film solar cells. In this work, these challenges are systematically addressed by employing molecular engineering to regulate the multiple interfaces of ZnO nanoparticles (ZnO-nps)/silver nanowires (AgNWs) window layers in kesterite solar cells. The interface molecular engineering enhances the conformal deposition of ZnO-nps on rough Cu2ZnSn(S, Se)4 (CZTSSe)/CdS substrates, passivates hydroxyl defects in ZnO-nps, and optimizes energy level alignment at the ZnO-nps/AgNWs interface. These advancements enable us to achieve a certified total area efficiency of 14.3%, marking a significant milestone for all-solution-processed kesterite solar cells. Furthermore, the solution-processed window layer forms a robust and flexion-tolerant lateral conductive network, imparting excellent flexibility to the cells. This development provides a critical technical foundation to support the low-cost and simpler preparation of thin-film solar cells in future commercialization.
{"title":"Multi-interface engineering for all-solution-processed kesterite solar cells","authors":"Licheng Lou , Jinlin Wang , Yuan Li , Kang Yin , Xiao Xu , Bowen Zhang , Menghan Jiao , Shudan Chen , Tan Guo , Jingchen Wang , Yiming Li , Jiangjian Shi , Huijue Wu , Ruijuan Xiao , Hao Xin , Yanhong Luo , Dongmei Li , Qingbo Meng","doi":"10.1016/j.joule.2025.102091","DOIUrl":"10.1016/j.joule.2025.102091","url":null,"abstract":"<div><div>The interface contact issue, surface defects, and energy level mismatches have significantly limited the optoelectronic performance of solution-processed transparent conductive window layers for use in thin-film solar cells. In this work, these challenges are systematically addressed by employing molecular engineering to regulate the multiple interfaces of ZnO nanoparticles (ZnO-nps)/silver nanowires (AgNWs) window layers in kesterite solar cells. The interface molecular engineering enhances the conformal deposition of ZnO-nps on rough Cu<sub>2</sub>ZnSn(S, Se)<sub>4</sub> (CZTSSe)/CdS substrates, passivates hydroxyl defects in ZnO-nps, and optimizes energy level alignment at the ZnO-nps/AgNWs interface. These advancements enable us to achieve a certified total area efficiency of 14.3%, marking a significant milestone for all-solution-processed kesterite solar cells. Furthermore, the solution-processed window layer forms a robust and flexion-tolerant lateral conductive network, imparting excellent flexibility to the cells. This development provides a critical technical foundation to support the low-cost and simpler preparation of thin-film solar cells in future commercialization.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 9","pages":"Article 102091"},"PeriodicalIF":35.4,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144825983","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 : 2025-09-17DOI: 10.1016/j.joule.2025.102098
You Gao , Youpeng Wang , Penghui Yang , Biao Shi , Zhen Liu , Shuainan Liu , Sihan Li , Yali Liu , Xin Ge , Pengfei Liu , Yuan Luo , Cong Sun , Xiaona Du , Pengyang Wang , Ying Zhao , Jun Shao , Xiaodan Zhang
The non-uniformity of the perovskite layer is a critical bottleneck limiting performance improvements in large-area perovskite solar cells (PSCs). In the evaporation-solution hybrid method, the Marangoni effect occurs due to variations in local organic material concentration during the coating process, leading to material clustering and coffee-ring effects, which hinder device performance. Here, we discussed the air-blowing process during coating and identified shear flow as the key factor affecting film homogeneity. By modulating the shear flow intensity, the surface tension gradient induced by local concentration differences is adjusted, mitigating the Marangoni effect and resulting in uniform perovskite films. Consequently, perovskite/silicon tandem solar cells (PS-TSCs) achieved 27.36% efficiency (64.64 cm2 aperture area), whereas perovskite modules (PSMs) reached 21.83% efficiency (810 cm2 aperture area).
{"title":"Shear flow strategy for coating homogeneity of organic materials in perovskite solar cells and modules","authors":"You Gao , Youpeng Wang , Penghui Yang , Biao Shi , Zhen Liu , Shuainan Liu , Sihan Li , Yali Liu , Xin Ge , Pengfei Liu , Yuan Luo , Cong Sun , Xiaona Du , Pengyang Wang , Ying Zhao , Jun Shao , Xiaodan Zhang","doi":"10.1016/j.joule.2025.102098","DOIUrl":"10.1016/j.joule.2025.102098","url":null,"abstract":"<div><div>The non-uniformity of the perovskite layer is a critical bottleneck limiting performance improvements in large-area perovskite solar cells (PSCs). In the evaporation-solution hybrid method, the Marangoni effect occurs due to variations in local organic material concentration during the coating process, leading to material clustering and coffee-ring effects, which hinder device performance. Here, we discussed the air-blowing process during coating and identified shear flow as the key factor affecting film homogeneity. By modulating the shear flow intensity, the surface tension gradient induced by local concentration differences is adjusted, mitigating the Marangoni effect and resulting in uniform perovskite films. Consequently, perovskite/silicon tandem solar cells (PS-TSCs) achieved 27.36% efficiency (64.64 cm<sup>2</sup> aperture area), whereas perovskite modules (PSMs) reached 21.83% efficiency (810 cm<sup>2</sup> aperture area).</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 9","pages":"Article 102098"},"PeriodicalIF":35.4,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144901245","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 : 2025-09-17DOI: 10.1016/j.joule.2025.102096
Attila Kormányos , Adrienn Szirmai , Balázs Endrődi , Csaba Janáky
One of the greatest obstacles hampering the industrial application of CO2 electrolysis is the large cell voltage (often over 3 V), which is mainly rooted in the high redox potential and overpotential of the oxygen evolution reaction (OER) occurring at the anode. It is possible to mitigate this issue by replacing the OER with alternative processes, such as the electrochemical oxidation of small organic molecules. Although the number of examples of paired CO2 reduction reaction (CO2RR)/small organic molecule oxidation is rapidly increasing, their viability has only been tested at the laboratory scale, mainly in batch cells. In this perspective, taking the glycerol oxidation reaction (GOR) as an example, the main challenges concerning the quantification of GOR products, the use of crude glycerol as a feedstock, and the integration of GOR with CO2RR are summarized. Finally, the most important envisioned future steps for the implementation of paired CO2RR/GOR electrolysis at scale are outlined.
{"title":"Pairing electrochemical CO2 reduction with glycerol oxidation: Bottlenecks today, opportunities tomorrow","authors":"Attila Kormányos , Adrienn Szirmai , Balázs Endrődi , Csaba Janáky","doi":"10.1016/j.joule.2025.102096","DOIUrl":"10.1016/j.joule.2025.102096","url":null,"abstract":"<div><div>One of the greatest obstacles hampering the industrial application of CO<sub>2</sub> electrolysis is the large cell voltage (often over 3 V), which is mainly rooted in the high redox potential and overpotential of the oxygen evolution reaction (OER) occurring at the anode. It is possible to mitigate this issue by replacing the OER with alternative processes, such as the electrochemical oxidation of small organic molecules. Although the number of examples of paired CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR)/small organic molecule oxidation is rapidly increasing, their viability has only been tested at the laboratory scale, mainly in batch cells. In this perspective, taking the glycerol oxidation reaction (GOR) as an example, the main challenges concerning the quantification of GOR products, the use of crude glycerol as a feedstock, and the integration of GOR with CO<sub>2</sub>RR are summarized. Finally, the most important envisioned future steps for the implementation of paired CO<sub>2</sub>RR/GOR electrolysis at scale are outlined.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 9","pages":"Article 102096"},"PeriodicalIF":35.4,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144901408","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 : 2025-09-17DOI: 10.1016/j.joule.2025.102101
Rémy Richard Jacquemond , Antoni Forner-Cuenca
In a recent issue of Chem, Carrington et al. introduced a low-cost operando diagnostic for aqueous organic redox flow batteries. Using pH and magnetic susceptibility measurements, they track state of charge and health of redox active organics in real time, revealing degradation pathways and air exposure effects without complex instrumentation.
{"title":"How are your molecules feeling? A facile method to monitor degradation pathways of organic molecules","authors":"Rémy Richard Jacquemond , Antoni Forner-Cuenca","doi":"10.1016/j.joule.2025.102101","DOIUrl":"10.1016/j.joule.2025.102101","url":null,"abstract":"<div><div>In a recent issue of <em>Chem</em>, Carrington et al. introduced a low-cost operando diagnostic for aqueous organic redox flow batteries. Using pH and magnetic susceptibility measurements, they track state of charge and health of redox active organics in real time, revealing degradation pathways and air exposure effects without complex instrumentation.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 9","pages":"Article 102101"},"PeriodicalIF":35.4,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145072080","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 : 2025-09-17DOI: 10.1016/j.joule.2025.102099
Shangwei Zhou , Wenjia Du , Bastian Mager , Paul R. Shearing , Thomas S. Miller , Rhodri Jervis
As demand grows for scalable and sustainable energy storage, fast and affordable diagnostics are urgently needed, especially for factory-level cell sorting and second-life assessments. Electrochemical impedance spectroscopy (EIS) is widely used but remains too slow, complex, and costly for large-scale use. This work introduces a multi-channel and multi-frequency electrical excitation response (MMER) technique that captures comparable impedance-related information at a fraction of the time and cost. MMER can diagnose entire battery modules in 1 s, regardless of cell count. It uses a binary multi-frequency excitation signal, implemented on simple hardware such as programmable logic devices. Unlike EIS, MMER avoids frequency-domain transformation and impedance fitting. Instead, it compares raw voltage responses under a shared excitation current to reveal performance variations. Experiments show MMER tracks cell health in line with EIS while reducing test time by over 99%. It supports real-time diagnostics even during high-rate cycling and extends to other electrochemical systems.
{"title":"Batch diagnosis of batteries within one second","authors":"Shangwei Zhou , Wenjia Du , Bastian Mager , Paul R. Shearing , Thomas S. Miller , Rhodri Jervis","doi":"10.1016/j.joule.2025.102099","DOIUrl":"10.1016/j.joule.2025.102099","url":null,"abstract":"<div><div>As demand grows for scalable and sustainable energy storage, fast and affordable diagnostics are urgently needed, especially for factory-level cell sorting and second-life assessments. Electrochemical impedance spectroscopy (EIS) is widely used but remains too slow, complex, and costly for large-scale use. This work introduces a multi-channel and multi-frequency electrical excitation response (MMER) technique that captures comparable impedance-related information at a fraction of the time and cost. MMER can diagnose entire battery modules in 1 s, regardless of cell count. It uses a binary multi-frequency excitation signal, implemented on simple hardware such as programmable logic devices. Unlike EIS, MMER avoids frequency-domain transformation and impedance fitting. Instead, it compares raw voltage responses under a shared excitation current to reveal performance variations. Experiments show MMER tracks cell health in line with EIS while reducing test time by over 99%. It supports real-time diagnostics even during high-rate cycling and extends to other electrochemical systems.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 9","pages":"Article 102099"},"PeriodicalIF":35.4,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144901177","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 : 2025-09-17DOI: 10.1016/j.joule.2025.102057
Feihong Du , Shihao Yang , Tian Yao , Donglin Han , Qiang Li , Shanyu Zheng , Ruhong Luo , Cenling Huang , Yifan Zhao , Yezhan Lin , Zhenhua Ma , Haotian Chen , Chenyu Guo , Haixin Qiu , Tiannan Yang , Xin Chen , Xiaoshi Qian
The advancement of high-performance electrocaloric (EC) cooling devices necessitates materials that exhibit robust EC effects under practical electric fields and that are suitable for industrial-scale production. Relaxor ferroelectric polymer nanocomposites represent a promising avenue. However, achieving high EC responses in current nanocomposites typically requires filler contents exceeding 5 vol %, resulting in material nonuniformity that limits practical applications. Here, we introduce a novel approach using nanocomposites with infinitesimally low loading of fillers that exploits interface effects to amplify dipolar responses, thereby significantly reducing the necessary filler content. We demonstrated that incorporating only 0.02 vol % CsPbBr3 perovskite quantum dots into P(VDF-TrFE-CFE) doubled the EC effect, with a filler content an order of magnitude lower than those previously reported. Our findings provide a clear structural understanding of how dilute nanocomposites enhance the dipolar response in polymeric materials and extend this promising concept for improved dipolar response-related properties to ferroelectric materials.
{"title":"Infinitesimal amount of perovskite quantum dots enhances electrocaloric cooling performances in diluted nanocomposites","authors":"Feihong Du , Shihao Yang , Tian Yao , Donglin Han , Qiang Li , Shanyu Zheng , Ruhong Luo , Cenling Huang , Yifan Zhao , Yezhan Lin , Zhenhua Ma , Haotian Chen , Chenyu Guo , Haixin Qiu , Tiannan Yang , Xin Chen , Xiaoshi Qian","doi":"10.1016/j.joule.2025.102057","DOIUrl":"10.1016/j.joule.2025.102057","url":null,"abstract":"<div><div>The advancement of high-performance electrocaloric (EC) cooling devices necessitates materials that exhibit robust EC effects under practical electric fields and that are suitable for industrial-scale production. Relaxor ferroelectric polymer nanocomposites represent a promising avenue. However, achieving high EC responses in current nanocomposites typically requires filler contents exceeding 5 vol %, resulting in material nonuniformity that limits practical applications. Here, we introduce a novel approach using nanocomposites with infinitesimally low loading of fillers that exploits interface effects to amplify dipolar responses, thereby significantly reducing the necessary filler content. We demonstrated that incorporating only 0.02 vol % CsPbBr<sub>3</sub> perovskite quantum dots into P(VDF-TrFE-CFE) doubled the EC effect, with a filler content an order of magnitude lower than those previously reported. Our findings provide a clear structural understanding of how dilute nanocomposites enhance the dipolar response in polymeric materials and extend this promising concept for improved dipolar response-related properties to ferroelectric materials.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 9","pages":"Article 102057"},"PeriodicalIF":35.4,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144756674","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 : 2025-09-17DOI: 10.1016/j.joule.2025.102089
Xu Gao , Biao Li , Anatolii V. Morozov , Leiting Zhang , Erik Elkaïm , Gwenaëlle Rousse , Artem M. Abakumov , Jean-Marie Tarascon
Lithium-rich manganese-based oxides are promising cathode materials for high-energy lithium-ion batteries but suffer from capacity deterioration due to oxygen release, irreversible structural changes, and detrimental secondary reactions—all of which are known to be exacerbated at elevated temperatures, leading to inferior high-temperature cycling performance. Here, we report the discovery of an unconventional temperature-dependent behavior in an O2-type cathode, which exhibits significantly improved cycling stability at an elevated temperature (55°C) compared with room temperature (RT), delivering high capacities of up to 300 mAh g−1. Combined structural and electrochemical analyses reveal that an in situ-formed ramsdellite-like surface layer, with tunnels oriented parallel to the crystallite surface, effectively protects the O-redox activity within the layered core but impedes the Li+ diffusion into and out of the particle at RT. However, Li+ diffusion through this protective surface layer is kinetically unlocked at elevated temperatures, resulting in improved capacity and cycling stability.
富锂锰基氧化物是高能锂离子电池很有前途的正极材料，但由于氧气释放、不可逆的结构变化和有害的二次反应，导致容量下降，所有这些都在高温下加剧，导致高温循环性能下降。在这里，我们报告了在O2型Li0.75[Li0.25Mn0.75]O2Li0.75[Li0.25Mn0.75]O2阴极中发现的一种非常规的温度依赖行为，与室温（RT）相比，该阴极在高温（55°C）下表现出显著改善的循环稳定性，提供高达300 mAh g−1的高容量。结合结构和电化学分析表明，原位形成的ramsdellite-like表面层具有平行于晶体表面的隧道，有效地保护了层状核心内的o -氧化还原活性，但阻碍了Li+在高温下进出颗粒的扩散。然而，在高温下，Li+通过这一保护表面层的扩散被动力学解锁，从而提高了容量和循环稳定性。
{"title":"Unconventional high-temperature cycling stability of O2-type Li0.75[Li0.25Mn0.75]O2 cathode","authors":"Xu Gao , Biao Li , Anatolii V. Morozov , Leiting Zhang , Erik Elkaïm , Gwenaëlle Rousse , Artem M. Abakumov , Jean-Marie Tarascon","doi":"10.1016/j.joule.2025.102089","DOIUrl":"10.1016/j.joule.2025.102089","url":null,"abstract":"<div><div>Lithium-rich manganese-based oxides are promising cathode materials for high-energy lithium-ion batteries but suffer from capacity deterioration due to oxygen release, irreversible structural changes, and detrimental secondary reactions—all of which are known to be exacerbated at elevated temperatures, leading to inferior high-temperature cycling performance. Here, we report the discovery of an unconventional temperature-dependent behavior in an O2-type <span><math><mrow><msub><mtext>Li</mtext><mn>0.75</mn></msub><mrow><mo>[</mo><mrow><msub><mtext>Li</mtext><mn>0.25</mn></msub><msub><mtext>Mn</mtext><mn>0.75</mn></msub></mrow><mo>]</mo></mrow><msub><mi>O</mi><mn>2</mn></msub></mrow></math></span> cathode, which exhibits significantly improved cycling stability at an elevated temperature (55°C) compared with room temperature (RT), delivering high capacities of up to 300 mAh g<sup>−1</sup>. Combined structural and electrochemical analyses reveal that an <em>in situ</em>-formed ramsdellite-like surface layer, with tunnels oriented parallel to the crystallite surface, effectively protects the O-redox activity within the layered core but impedes the Li<sup>+</sup> diffusion into and out of the particle at RT. However, Li<sup>+</sup> diffusion through this protective surface layer is kinetically unlocked at elevated temperatures, resulting in improved capacity and cycling stability.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 9","pages":"Article 102089"},"PeriodicalIF":35.4,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144797397","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 : 2025-09-17DOI: 10.1016/j.joule.2025.102090
Eric K. Zimmerer , Wentao Liang , Rachana Somaskandan , Elizabeth DeToma , Connor Fawcett , Andrea M. Bruck , Lu Ma , Steven N. Ehrlich , Qing Zhao , Joshua W. Gallaway
Battery technologies beyond Li-ion are likely needed for extensive integration of grid-scale storage. The rechargeable Zn-MnO2 chemistry has the potential for high sustainability, high safety, and low cost, using Earth-abundant basis materials. In an alkaline electrolyte, the MnO2 cathode can cycle reversibly if modified by including a Bi-containing additive, although the cycling mechanism remains mostly unknown. This work presents an account of the intermediate species involved in the electrochemical transformation from layered δ-MnO2 to Mn(OH)2 and back. During charge, a disordered intermediate with a structure resembling layered β-MnOOH exists stably for an extended period, corresponding to a regime known to have unexpected electrochemical activity of Bi. During discharge, β-MnOOH exists only briefly and is never the majority material, revealing that the cycling mechanism is asymmetric. These findings represent a significant advance in mechanistic knowledge and can enable engineering to develop the system for commercial use.
{"title":"Dynamics of disordered intermediates during the two-electron alkaline MnO2 conversion reaction for grid-scale batteries","authors":"Eric K. Zimmerer , Wentao Liang , Rachana Somaskandan , Elizabeth DeToma , Connor Fawcett , Andrea M. Bruck , Lu Ma , Steven N. Ehrlich , Qing Zhao , Joshua W. Gallaway","doi":"10.1016/j.joule.2025.102090","DOIUrl":"10.1016/j.joule.2025.102090","url":null,"abstract":"<div><div>Battery technologies beyond Li-ion are likely needed for extensive integration of grid-scale storage. The rechargeable Zn-MnO<sub>2</sub> chemistry has the potential for high sustainability, high safety, and low cost, using Earth-abundant basis materials. In an alkaline electrolyte, the MnO<sub>2</sub> cathode can cycle reversibly if modified by including a Bi-containing additive, although the cycling mechanism remains mostly unknown. This work presents an account of the intermediate species involved in the electrochemical transformation from layered <em>δ</em>-MnO<sub>2</sub> to Mn(OH)<sub>2</sub> and back. During charge, a disordered intermediate with a structure resembling layered <em>β</em>-MnOOH exists stably for an extended period, corresponding to a regime known to have unexpected electrochemical activity of Bi. During discharge, <em>β</em>-MnOOH exists only briefly and is never the majority material, revealing that the cycling mechanism is asymmetric. These findings represent a significant advance in mechanistic knowledge and can enable engineering to develop the system for commercial use.</div></div>","PeriodicalId":343,"journal":{"name":"Joule","volume":"9 9","pages":"Article 102090"},"PeriodicalIF":35.4,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144797554","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}
扫码关注我们
求助内容：
应助结果提醒方式：
京公网安备 11010802042870号