Juhana Jämsén, Pauliina Nevalainen, Kirill Murashko and Anna Lähde
Lithium–sulfur batteries offer high theoretical energy density and low cost. However, challenges such as the polysulfide shuttle effect and poor conductivity of sulfur have hindered their commercial application. In this work, porous nitrogen-doped carbon materials were synthesized from Kraft lignin using a molten salt method combined with urea and K2CO3 for pore generation in a single synthesis step. The use of a KCl/NaCl salt mixture as the reaction medium allowed for control over product morphology and increased yield by retaining volatiles. The effects of varying lignin/urea/K2CO3 mass ratios on the characteristics of the produced materials were analyzed. The carbon-based host materials were then combined with sulfur through chemical deposition and melt diffusion. The properties of the host materials and composites were characterized using TGA, SEM, EDS, BET, XPS, and Raman analyses. Electrochemical tests were conducted to study the impact on the electrochemical properties of the lithium–sulfur battery cathode. The analysis revealed that the controlled porosity and functionalization of the host materials significantly influence the distribution and utilization of sulfur during electrochemical testing. By analyzing the effects of host material porosity and nitrogen doping, we improved the electrochemical properties of the cathode material. The best performing composite material exhibited a high initial discharge capacity 1407 mAh per g-S (83% of the theoretical capacity of sulfur) and retained 825 mAh g−1 capacity (average fade of 0.105% per cycle) and 98.7% coulombic efficiency after 200 cycles. In addition, the material displayed good performance at commercially viable mass loading.
锂硫电池理论能量密度高,成本低。然而,诸如多硫化物的穿梭效应和硫的导电性差等挑战阻碍了它们的商业应用。本文以硫酸盐木质素为原料,采用熔盐法与尿素和K2CO3结合,一步合成多孔氮掺杂碳材料。使用KCl/NaCl盐混合物作为反应介质可以控制产物形态,并通过保留挥发物来提高收率。分析了不同木质素/尿素/K2CO3质量比对生产材料性能的影响。然后通过化学沉积和熔体扩散将碳基主体材料与硫结合。采用热重分析(TGA)、扫描电镜(SEM)、能谱分析(EDS)、BET分析(BET)、XPS分析(XPS)和拉曼分析(Raman)表征了主体材料和复合材料的性能。通过电化学试验研究了对锂硫电池正极电化学性能的影响。分析表明,在电化学测试过程中,基质材料的孔隙率控制和功能化对硫的分布和利用有显著影响。通过分析基体孔隙率和氮掺杂对阴极材料性能的影响,改善了阴极材料的电化学性能。性能最好的复合材料表现出高的初始放电容量1407 mAh / g- s(83%的硫理论容量),在200次循环后保持825 mAh / g- 1容量(平均每循环衰减0.105%)和98.7%的库仑效率。此外,该材料在商业可行的质量载荷下表现出良好的性能。
{"title":"Molten salt assisted synthesis of a lignin derived porous carbon host for lithium–sulfur battery cathodes","authors":"Juhana Jämsén, Pauliina Nevalainen, Kirill Murashko and Anna Lähde","doi":"10.1039/D5YA00266D","DOIUrl":"https://doi.org/10.1039/D5YA00266D","url":null,"abstract":"<p >Lithium–sulfur batteries offer high theoretical energy density and low cost. However, challenges such as the polysulfide shuttle effect and poor conductivity of sulfur have hindered their commercial application. In this work, porous nitrogen-doped carbon materials were synthesized from Kraft lignin using a molten salt method combined with urea and K<small><sub>2</sub></small>CO<small><sub>3</sub></small> for pore generation in a single synthesis step. The use of a KCl/NaCl salt mixture as the reaction medium allowed for control over product morphology and increased yield by retaining volatiles. The effects of varying lignin/urea/K<small><sub>2</sub></small>CO<small><sub>3</sub></small> mass ratios on the characteristics of the produced materials were analyzed. The carbon-based host materials were then combined with sulfur through chemical deposition and melt diffusion. The properties of the host materials and composites were characterized using TGA, SEM, EDS, BET, XPS, and Raman analyses. Electrochemical tests were conducted to study the impact on the electrochemical properties of the lithium–sulfur battery cathode. The analysis revealed that the controlled porosity and functionalization of the host materials significantly influence the distribution and utilization of sulfur during electrochemical testing. By analyzing the effects of host material porosity and nitrogen doping, we improved the electrochemical properties of the cathode material. The best performing composite material exhibited a high initial discharge capacity 1407 mAh per g-S (83% of the theoretical capacity of sulfur) and retained 825 mAh g<small><sup>−1</sup></small> capacity (average fade of 0.105% per cycle) and 98.7% coulombic efficiency after 200 cycles. In addition, the material displayed good performance at commercially viable mass loading.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 1","pages":" 83-96"},"PeriodicalIF":4.3,"publicationDate":"2025-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/ya/d5ya00266d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146015981","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sukhvant Singh, Aditya Singh, Muhammad Azhar Iqbal and Samaneh Shahgaldi
The porous transport layer (PTL) is an integral component of the proton exchange membrane water electrolyzer (PEMWE), ensuring the supply of water, electrical conduction, and the removal of produced oxygen. The applied positive potential and acidic nature of the proton exchange membrane (PEM) in the PEMWE lead to an acidic environment, which promotes the formation of passivated TiOx on the surface of the Ti PTL. The limited conductivity of TiOx results in an increase in contact resistance and cell voltage. The precious metal coatings prevent TiOx formation, ensure low interfacial contact resistance (ICR), and provide long-term stability. In this work, a durable bilayer coated Ti PTL was prepared by applying a thin Pt sputtered coating onto Au-electroplated PTL. The bilayer coating of Au/Pt reduced the loading of precious metals to a low level (overall 0.14 mg cm−2) while exhibiting outstanding corrosion resistance and cell performance. The coated Pt layer with 0.06 mg cm−2 loading on Au coated Ti PTL exhibited a stability number 50 times higher than that of Ti PTL coated with Au alone. The balanced residual shear stress at the Au/Pt interface assisted to improve the charge transfer resistance against acid based corrosive environment. Employing the TiH/Au/Pt-0.06 coating on the Ti-PTL, a PEMWE cell performance of 1.716 V at 2.0 A cm−2 was achieved at 80 °C under ambient pressure.
多孔传输层(PTL)是质子交换膜水电解槽(PEMWE)的组成部分,保证水的供应、电的传导和产生氧的去除。质子交换膜(PEM)在质子交换膜(PEMWE)中所施加的正电位和酸性导致了酸性环境,这促进了钛PTL表面钝化TiOx的形成。TiOx的有限导电性导致接触电阻和电池电压的增加。贵金属涂层防止TiOx形成,确保低界面接触电阻(ICR),并提供长期稳定性。在本工作中,通过在镀金的PTL上镀上一层薄薄的Pt溅射涂层,制备了一种耐用的双层Ti PTL。Au/Pt双层涂层将贵金属的负载降低到较低的水平(总体0.14 mg cm - 2),同时表现出出色的耐腐蚀性和电池性能。负载0.06 mg cm−2的铂层在镀Au的Ti PTL上的稳定性比单独镀Au的Ti PTL高50倍。Au/Pt界面处的残余剪应力平衡有助于提高对酸基腐蚀环境的电荷传递能力。在Ti-PTL上采用TiH/Au/Pt-0.06涂层,在80°C的环境压力下,在2.0 a cm - 2下获得了1.716 V的PEMWE电池性能。
{"title":"Enhancing the durability of Au-coated Ti porous transport layers (PTLs) with a thin Pt top layer for PEM water electrolyzer applications","authors":"Sukhvant Singh, Aditya Singh, Muhammad Azhar Iqbal and Samaneh Shahgaldi","doi":"10.1039/D5YA00274E","DOIUrl":"https://doi.org/10.1039/D5YA00274E","url":null,"abstract":"<p >The porous transport layer (PTL) is an integral component of the proton exchange membrane water electrolyzer (PEMWE), ensuring the supply of water, electrical conduction, and the removal of produced oxygen. The applied positive potential and acidic nature of the proton exchange membrane (PEM) in the PEMWE lead to an acidic environment, which promotes the formation of passivated TiO<small><sub><em>x</em></sub></small> on the surface of the Ti PTL. The limited conductivity of TiO<small><sub><em>x</em></sub></small> results in an increase in contact resistance and cell voltage. The precious metal coatings prevent TiO<small><sub><em>x</em></sub></small> formation, ensure low interfacial contact resistance (ICR), and provide long-term stability. In this work, a durable bilayer coated Ti PTL was prepared by applying a thin Pt sputtered coating onto Au-electroplated PTL. The bilayer coating of Au/Pt reduced the loading of precious metals to a low level (overall 0.14 mg cm<small><sup>−2</sup></small>) while exhibiting outstanding corrosion resistance and cell performance. The coated Pt layer with 0.06 mg cm<small><sup>−2</sup></small> loading on Au coated Ti PTL exhibited a stability number 50 times higher than that of Ti PTL coated with Au alone. The balanced residual shear stress at the Au/Pt interface assisted to improve the charge transfer resistance against acid based corrosive environment. Employing the TiH/Au/Pt-0.06 coating on the Ti-PTL, a PEMWE cell performance of 1.716 V at 2.0 A cm<small><sup>−2</sup></small> was achieved at 80 °C under ambient pressure.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 1","pages":" 56-70"},"PeriodicalIF":4.3,"publicationDate":"2025-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/ya/d5ya00274e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146015978","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Souk Y. Kim, Noura Rayes, Armen R. Kemanian, Enrique D. Gomez and Nutifafa Y. Doumon
Correction for ‘Semitransparent organic and perovskite photovoltaics for agrivoltaic applications’ by Souk Y. Kim et al., Energy Adv., 2025, 4, 37–54, https://doi.org/10.1039/D4YA00492B.
Souk Y. Kim等人对“用于农业光伏应用的半透明有机和钙钛矿光伏”的修正,能源咨询,2025,4,37 - 54,https://doi.org/10.1039/D4YA00492B。
{"title":"Correction: Semitransparent organic and perovskite photovoltaics for agrivoltaic applications","authors":"Souk Y. Kim, Noura Rayes, Armen R. Kemanian, Enrique D. Gomez and Nutifafa Y. Doumon","doi":"10.1039/D5YA90042E","DOIUrl":"https://doi.org/10.1039/D5YA90042E","url":null,"abstract":"<p >Correction for ‘Semitransparent organic and perovskite photovoltaics for agrivoltaic applications’ by Souk Y. Kim <em>et al.</em>, <em>Energy Adv.</em>, 2025, <strong>4</strong>, 37–54, https://doi.org/10.1039/D4YA00492B.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 1","pages":" 130-130"},"PeriodicalIF":4.3,"publicationDate":"2025-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/ya/d5ya90042e?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146015976","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kathrin Schad, Nicolas Görnert, Christopher Markus Mehlich, Meichen Zhan and Kai Peter Birke
The rapid growth of lithium-ion battery (LiB) production calls for chemistries that combine high energy density with low environmental and economic impact. The GREENcell-concept addresses this challenge by pairing a fluorine (F)-free polyisobutylene (PIB) binder-based LiMn2O4 (LMO) cathode with an anode based on commercial aluminum (Al) alloy foil, whose theoretical capacity (993 mAh g−1) far exceeds that of graphite (372 mAh g−1). In this study cycling stability was improved through iterative optimization of the GREENcell-concept, targeting cathode formulation as well as Al foil composition, Al foil hardness, and Al surface passivation. Substituting polyvinylidene fluoride (PVDF)-based commercial LMO with a F-free PIB-based formulation reduced cathodic capacity fade by 17%, yet ∼20% of total losses in the full-cell set up remained cathode-related. To evaluate anode optimization strategies, full-cells incorporating the F-free LMO cathode were employed. Al alloy 8011 containing iron and silicon impurities outperformed high-purity Al 1050 reference foil, improving capacity retention by ∼10% through more uniform lithiation, while strain-hardened foils effectively suppressed plastic deformation compared with annealed counterparts. Surface passivation of the 8011 Al alloy foil provided further gains: a chrome(III)-based passivation improved capacity retention by 11%, and an Al silicate layer enabled the most durable cell performance, maintaining a stable capacity profile for 100 cycles after the initial losses were overcome, likely by promoting a robust solid–electrolyte interface (SEI) able to accommodate anode volume changes. Collectively, these strategies increased capacity retention after 100 cycles from 4% for uncoated annealed high-purity Al 1050 foil to 67% for the strain-hardened, Al silicate-passivated 8011 Al alloy foil, demonstrating GREENcell's promise as a scalable, low-cost, and environmentally benign LiB architecture, as demonstrated in laboratory coin cells.
锂离子电池(LiB)生产的快速增长要求化学物质将高能量密度与低环境和经济影响结合起来。greencell概念解决了这一挑战,将无氟(F)聚异丁烯(PIB)粘合剂基LiMn2O4 (LMO)阴极与基于商业铝(Al)合金箔的阳极配对,其理论容量(993 mAh g - 1)远远超过石墨(372 mAh g - 1)。在本研究中,通过对greencell概念的迭代优化,以阴极配方、铝箔成分、铝箔硬度和铝表面钝化为目标,提高了循环稳定性。用不含f的pib基配方替代基于聚偏氟乙烯(PVDF)的商用LMO,使阴极容量衰减降低了17%,但在全电池装置中,总损耗的约20%仍与阴极有关。为了评估阳极优化策略,采用了含无氟LMO阴极的全电池。含有铁和硅杂质的铝合金8011优于高纯度的Al 1050参考箔,通过更均匀的锂化,提高了约10%的容量保留,而应变硬化箔与退火箔相比,有效地抑制了塑性变形。8011铝合金箔的表面钝化提供了进一步的增益:铬(III)基钝化使容量保持率提高了11%,硅酸铝层使电池性能最持久,在克服初始损耗后保持100次循环的稳定容量,可能是通过促进能够适应阳极体积变化的坚固的固体电解质界面(SEI)。总的来说,这些策略提高了100次循环后的容量保持率,从未涂层退火高纯度Al 1050箔的4%提高到应变硬化硅酸铝钝化8011铝合金箔的67%,证明了GREENcell作为可扩展、低成本和环保的LiB架构的承诺,正如实验室硬币电池所证明的那样。
{"title":"GREENcell – combination of a strain-hardened and passivated Al alloy foil anode with a F-free LiMn2O4 cathode","authors":"Kathrin Schad, Nicolas Görnert, Christopher Markus Mehlich, Meichen Zhan and Kai Peter Birke","doi":"10.1039/D5YA00287G","DOIUrl":"https://doi.org/10.1039/D5YA00287G","url":null,"abstract":"<p >The rapid growth of lithium-ion battery (LiB) production calls for chemistries that combine high energy density with low environmental and economic impact. The GREENcell-concept addresses this challenge by pairing a fluorine (F)-free polyisobutylene (PIB) binder-based LiMn<small><sub>2</sub></small>O<small><sub>4</sub></small> (LMO) cathode with an anode based on commercial aluminum (Al) alloy foil, whose theoretical capacity (993 mAh g<small><sup>−1</sup></small>) far exceeds that of graphite (372 mAh g<small><sup>−1</sup></small>). In this study cycling stability was improved through iterative optimization of the GREENcell-concept, targeting cathode formulation as well as Al foil composition, Al foil hardness, and Al surface passivation. Substituting polyvinylidene fluoride (PVDF)-based commercial LMO with a F-free PIB-based formulation reduced cathodic capacity fade by 17%, yet ∼20% of total losses in the full-cell set up remained cathode-related. To evaluate anode optimization strategies, full-cells incorporating the F-free LMO cathode were employed. Al alloy 8011 containing iron and silicon impurities outperformed high-purity Al 1050 reference foil, improving capacity retention by ∼10% through more uniform lithiation, while strain-hardened foils effectively suppressed plastic deformation compared with annealed counterparts. Surface passivation of the 8011 Al alloy foil provided further gains: a chrome(<small>III</small>)-based passivation improved capacity retention by 11%, and an Al silicate layer enabled the most durable cell performance, maintaining a stable capacity profile for 100 cycles after the initial losses were overcome, likely by promoting a robust solid–electrolyte interface (SEI) able to accommodate anode volume changes. Collectively, these strategies increased capacity retention after 100 cycles from 4% for uncoated annealed high-purity Al 1050 foil to 67% for the strain-hardened, Al silicate-passivated 8011 Al alloy foil, demonstrating GREENcell's promise as a scalable, low-cost, and environmentally benign LiB architecture, as demonstrated in laboratory coin cells.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 1","pages":" 97-109"},"PeriodicalIF":4.3,"publicationDate":"2025-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/ya/d5ya00287g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146015991","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Solid composite polymer electrolytes (CPEs) have emerged as a promising option due to their excellent ionic conductivity, mechanical flexibility, and compatibility with Li metal electrodes. In this study, polyethylene oxide (PEO) was selected as the base polymer, and a composite was formed with LLZTO and oxygen-vacancy LLZTO (OV-LLZTO) as an active ceramic filler. The surface defects in OV-LLZTO enhance its bonding with the PEO chains, leading to improved interfacial resistance, enhanced mechanical stability, prevention of PEO crystallization, mitigation of LLZTO nanoparticle agglomeration, and improved Li+ ion conductivity. The removal of oxygen atoms from the LLZTO crystal results in lattice contraction, which strengthens the interaction between the LLZTO and PEO polymer chains, thereby reducing interfacial resistance and improving lithium-ion conductivity. In solid-state battery performance, the ionic conductivity and transference number of the solid electrolyte are crucial, along with thermal, mechanical, and electrochemical stability. While pristine PEO electrolytes exhibit higher conductivity than composites, they have a lower transference number and inferior stability compared to the composite electrolytes. As the temperature increases, the transference number of the polymer electrolyte increases due to increased ion mobility; however, with aging it decreases due to the formation of a passivation layer. A solid-state full cell employing the PEO/OV-LLZTO electrolyte was used to demonstrate high-rate capability (10C rate) and excellent capacity retention at 60 °C with a cathode areal loading of ∼0.2 mAh cm−2, underscoring its potential for high-performance battery applications.
固体复合聚合物电解质(cpe)由于其优异的离子电导率、机械柔韧性和与锂金属电极的相容性而成为一种很有前途的选择。本研究选择聚乙烯氧化物(PEO)作为基体聚合物,以LLZTO和氧空位LLZTO (OV-LLZTO)作为活性陶瓷填料形成复合材料。OV-LLZTO的表面缺陷增强了其与PEO链的结合,从而提高了界面电阻,增强了机械稳定性,防止了PEO的结晶,减缓了LLZTO纳米颗粒的团聚,提高了Li+离子的电导率。从LLZTO晶体中去除氧原子导致晶格收缩,增强了LLZTO和PEO聚合物链之间的相互作用,从而降低了界面阻力,提高了锂离子的电导率。在固态电池性能中,固体电解质的离子电导率和转移数以及热、机械和电化学稳定性至关重要。虽然原始PEO电解质的电导率高于复合材料,但与复合材料电解质相比,它们的转移数较低,稳定性较差。随着温度的升高,由于离子迁移率的增加,聚合物电解质的转移数增加;然而,随着时效,由于钝化层的形成,它减少。采用PEO/OV-LLZTO电解质的固态全电池在60°C下具有高倍率(10C倍率)和优异的容量保持能力,阴极面积负载为~ 0.2 mAh cm - 2,强调了其高性能电池应用的潜力。
{"title":"Factors controlling the performance of lithium-metal solid-state batteries with polyethylene oxide-based composite polymer electrolytes","authors":"Bapi Bera, Douglas S. Aaron and Matthew M. Mench","doi":"10.1039/D5YA00278H","DOIUrl":"https://doi.org/10.1039/D5YA00278H","url":null,"abstract":"<p >Solid composite polymer electrolytes (CPEs) have emerged as a promising option due to their excellent ionic conductivity, mechanical flexibility, and compatibility with Li metal electrodes. In this study, polyethylene oxide (PEO) was selected as the base polymer, and a composite was formed with LLZTO and oxygen-vacancy LLZTO (OV-LLZTO) as an active ceramic filler. The surface defects in OV-LLZTO enhance its bonding with the PEO chains, leading to improved interfacial resistance, enhanced mechanical stability, prevention of PEO crystallization, mitigation of LLZTO nanoparticle agglomeration, and improved Li<small><sup>+</sup></small> ion conductivity. The removal of oxygen atoms from the LLZTO crystal results in lattice contraction, which strengthens the interaction between the LLZTO and PEO polymer chains, thereby reducing interfacial resistance and improving lithium-ion conductivity. In solid-state battery performance, the ionic conductivity and transference number of the solid electrolyte are crucial, along with thermal, mechanical, and electrochemical stability. While pristine PEO electrolytes exhibit higher conductivity than composites, they have a lower transference number and inferior stability compared to the composite electrolytes. As the temperature increases, the transference number of the polymer electrolyte increases due to increased ion mobility; however, with aging it decreases due to the formation of a passivation layer. A solid-state full cell employing the PEO/OV-LLZTO electrolyte was used to demonstrate high-rate capability (10C rate) and excellent capacity retention at 60 °C with a cathode areal loading of ∼0.2 mAh cm<small><sup>−2</sup></small>, underscoring its potential for high-performance battery applications.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 1","pages":" 119-129"},"PeriodicalIF":4.3,"publicationDate":"2025-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/ya/d5ya00278h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146015975","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
N. L. Grotkopp, M. Hokmabadi, M. Nebelsiek, M. Kurrat, P. Michalowski, A. Jean-Fulcrand and G. Garnweitner
PEO is the most investigated polymer for battery solid electrolytes, and continues to be considered state of the art to this day. It is often prepared by tape casting in a solvent-based process. However, solvent-free production of battery electrolytes has become a prominent topic in the recent years in science and industry. This is due to the elimination of one process step – the evaporation of a solvent – sparing production time, material, energy, solvent disposal and thus substantially reducing the production costs. Herein we propose the quick and simple solvent-free preparation of a PEO-LiTFSI electrolyte by kneading on a larger scale with reduced production times compared to conventional solvent based techniques. 50 g of electrolyte are produced at 60 °C within ∼15 min of kneading and another ∼5 min for calendering at 120 °C, whilst for the solvent-based solid electrolyte processing, ∼1.5 h followed by drying over night was required to prepare one solid electrolyte film. The processing and properties of the electrolyte are thoroughly discussed, comparing different conducting salts, polymer molecular weights and polymer–salt concentrations that are evaluated by EIS at different temperatures. An SEM and 4K light microscope-supported post mortem analysis was performed to provide insights on the surface processes of the electrodes that occur during galvanostatic cycling. Moreover, we report the first application of this solvent-free based PEO solid electrolyte in Li–S cells with different electrolyte thicknesses at 50 °C.
{"title":"Simple and scalable solvent-free PEO based electrolyte fabrication by kneading for all solid state lithium sulfur batteries","authors":"N. L. Grotkopp, M. Hokmabadi, M. Nebelsiek, M. Kurrat, P. Michalowski, A. Jean-Fulcrand and G. Garnweitner","doi":"10.1039/D5YA00294J","DOIUrl":"https://doi.org/10.1039/D5YA00294J","url":null,"abstract":"<p >PEO is the most investigated polymer for battery solid electrolytes, and continues to be considered state of the art to this day. It is often prepared by tape casting in a solvent-based process. However, solvent-free production of battery electrolytes has become a prominent topic in the recent years in science and industry. This is due to the elimination of one process step – the evaporation of a solvent – sparing production time, material, energy, solvent disposal and thus substantially reducing the production costs. Herein we propose the quick and simple solvent-free preparation of a PEO-LiTFSI electrolyte by kneading on a larger scale with reduced production times compared to conventional solvent based techniques. 50 g of electrolyte are produced at 60 °C within ∼15 min of kneading and another ∼5 min for calendering at 120 °C, whilst for the solvent-based solid electrolyte processing, ∼1.5 h followed by drying over night was required to prepare one solid electrolyte film. The processing and properties of the electrolyte are thoroughly discussed, comparing different conducting salts, polymer molecular weights and polymer–salt concentrations that are evaluated by EIS at different temperatures. An SEM and 4K light microscope-supported post mortem analysis was performed to provide insights on the surface processes of the electrodes that occur during galvanostatic cycling. Moreover, we report the first application of this solvent-free based PEO solid electrolyte in Li–S cells with different electrolyte thicknesses at 50 °C.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 2","pages":" 151-162"},"PeriodicalIF":4.3,"publicationDate":"2025-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/ya/d5ya00294j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146216700","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mohammad Reza Mohammadi, Masoumeh Khamehchi and Aida Mohammadi
Using a diffusion differential model, this paper presents models that have been developed to predict the photovoltaic characteristics of Zr-doped TiO2 dye-sensitized solar cells (DSSCs) by incorporating a CNT–TiO2 core–shell (CNT@TiO2) with mono- and double-layer photoanode configurations. The monolayer cells are composed of Zr-doped TiO2 nanoparticles with different molar concentrations of Zr, while the double-layer devices are composed of Zr-doped TiO2 nanoparticles with optimum Zr content (i.e., 0.025 mol%) as the under-layer and CNT@TiO2, with varying CNT weight content, as the over-layer. The model evaluates the impact of critical parameters, including Zr concentration, CNT@TiO2 content, operating temperature, and photoanode thickness, on the photovoltaic characteristics of the devices. The model predictions are validated, demonstrating their capability to accurately represent the photocurrent density–voltage behavior of the devices. Results indicate that the photocurrent density of monolayer DSSCs increases with increasing Zr content up to 0.025 mol% and then decreases with further increases in Zr molar percentage. Moreover, both photocurrent density and open-circuit voltage of the double-layer devices first increase with the introduction of CNT@TiO2 and then decrease, reaching the highest value at 0.025 wt%. It is found that high operating temperatures lead to a decrease in the open-circuit voltage for all photoanode thicknesses, while the photocurrent density first increases with an increase in operating temperature and then decreases with a further temperature increase, reaching a maximum at 30 °C. For monolayer DSSCs, photocurrent density increases with electrode thickness up to 15 µm, after which it declines. These findings present essential knowledge for optimizing the design and efficiency of DSSCs.
{"title":"Modeling the photovoltaic characteristics of Zr-doped TiO2 dye-sensitized solar cells by incorporating CNT@TiO2","authors":"Mohammad Reza Mohammadi, Masoumeh Khamehchi and Aida Mohammadi","doi":"10.1039/D5YA00347D","DOIUrl":"https://doi.org/10.1039/D5YA00347D","url":null,"abstract":"<p >Using a diffusion differential model, this paper presents models that have been developed to predict the photovoltaic characteristics of Zr-doped TiO<small><sub>2</sub></small> dye-sensitized solar cells (DSSCs) by incorporating a CNT–TiO<small><sub>2</sub></small> core–shell (CNT@TiO<small><sub>2</sub></small>) with mono- and double-layer photoanode configurations. The monolayer cells are composed of Zr-doped TiO<small><sub>2</sub></small> nanoparticles with different molar concentrations of Zr, while the double-layer devices are composed of Zr-doped TiO<small><sub>2</sub></small> nanoparticles with optimum Zr content (<em>i.e.</em>, 0.025 mol%) as the under-layer and CNT@TiO<small><sub>2</sub></small>, with varying CNT weight content, as the over-layer. The model evaluates the impact of critical parameters, including Zr concentration, CNT@TiO<small><sub>2</sub></small> content, operating temperature, and photoanode thickness, on the photovoltaic characteristics of the devices. The model predictions are validated, demonstrating their capability to accurately represent the photocurrent density–voltage behavior of the devices. Results indicate that the photocurrent density of monolayer DSSCs increases with increasing Zr content up to 0.025 mol% and then decreases with further increases in Zr molar percentage. Moreover, both photocurrent density and open-circuit voltage of the double-layer devices first increase with the introduction of CNT@TiO<small><sub>2</sub></small> and then decrease, reaching the highest value at 0.025 wt%. It is found that high operating temperatures lead to a decrease in the open-circuit voltage for all photoanode thicknesses, while the photocurrent density first increases with an increase in operating temperature and then decreases with a further temperature increase, reaching a maximum at 30 °C. For monolayer DSSCs, photocurrent density increases with electrode thickness up to 15 µm, after which it declines. These findings present essential knowledge for optimizing the design and efficiency of DSSCs.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 1","pages":" 110-118"},"PeriodicalIF":4.3,"publicationDate":"2025-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/ya/d5ya00347d?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146015974","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mismatched complex oxide thin films and heterostructures based on perovskites have key applications in technologies such as solid oxide fuel cells, batteries, and solar cells because of emerging properties at the interface. Although lattice mismatch and resulting misfit dislocations are one of the fundamental reasons for the emergence of new properties at the interface, their precise role is not well understood. In light of this, we have used first principles calculations to study BaZrO3(110)/SrTiO3(100) heterostructures for thin film electrolyte applications and predict the interfacial stability as a function of termination layer chemistry. Atomic scale structure and electronic structure of oxygen vacancies at doped interfaces was further studied to comprehend their stability and location preference at the interface. Strong dependence of oxygen vacancy formation on termination layer chemistry is observed. Among the four possible interfaces, oxygen vacancies exhibit a thermodynamic preference to form at the TiO2–ZrO2 interface. Results herein shed light on the fundamental aspects of mismatched perovskite oxide interfaces and their influence on thermodynamic stability of oxygen vacancy defects, which influences ionic transport and is imperative to design next-generation thin film oxide electrolytes.
{"title":"Interface layer chemistry dependent oxygen defect formation in BaZrO3(110)/SrTiO3(100) heterostructures","authors":"Jason Rakowsky and Pratik P. Dholabhai","doi":"10.1039/D5YA00220F","DOIUrl":"https://doi.org/10.1039/D5YA00220F","url":null,"abstract":"<p >Mismatched complex oxide thin films and heterostructures based on perovskites have key applications in technologies such as solid oxide fuel cells, batteries, and solar cells because of emerging properties at the interface. Although lattice mismatch and resulting misfit dislocations are one of the fundamental reasons for the emergence of new properties at the interface, their precise role is not well understood. In light of this, we have used first principles calculations to study BaZrO<small><sub>3</sub></small>(110)/SrTiO<small><sub>3</sub></small>(100) heterostructures for thin film electrolyte applications and predict the interfacial stability as a function of termination layer chemistry. Atomic scale structure and electronic structure of oxygen vacancies at doped interfaces was further studied to comprehend their stability and location preference at the interface. Strong dependence of oxygen vacancy formation on termination layer chemistry is observed. Among the four possible interfaces, oxygen vacancies exhibit a thermodynamic preference to form at the TiO<small><sub>2</sub></small>–ZrO<small><sub>2</sub></small> interface. Results herein shed light on the fundamental aspects of mismatched perovskite oxide interfaces and their influence on thermodynamic stability of oxygen vacancy defects, which influences ionic transport and is imperative to design next-generation thin film oxide electrolytes.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 1","pages":" 43-55"},"PeriodicalIF":4.3,"publicationDate":"2025-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/ya/d5ya00220f?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146015977","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Parisa Akhtari Zavareh, Aditya Naveen Matam and Krishna Shah
Heterogeneous aging of lithium-ion (Li-ion) battery cells within a battery pack is a major challenge that limits the pack's overall performance, safety, and life. Variations in cell degradation rates lead to nonuniform charge/discharge behavior among cells in a pack, accelerated aging in some cells turning them into “weak links”, and reducing energy throughput at the pack level. While previous studies have investigated uneven aging driven by differences in capacity or resistance, limited attention has been given to the root causes of these variations, particularly those arising from manufacturing-induced differences in the electrode microstructure. This study addresses this gap by investigating the effects of variations in the mean active material particle size across cells, a key design parameter of a porous electrode, on the aging behavior of these cells when connected in series and parallel. Using an electrochemical battery model, the aging behavior of individual cells and the pack as a whole is investigated for three electrical configurations (i.e., 1S4P, 4S1P, and 2S2P) at select C-rates and voltage windows. Results indicate that cells with smaller mean particle size degrade faster despite having a thinner SEI layer at the end of life, and even a minor variation of 1 µm in the mean active material particle size across cells can lead to significant uneven capacity fade across cells and accelerated aging of the pack, particularly at low C-rates. These findings highlight the critical impact that variability in the microstructure has on pack-level aging and provide insights into effective cell and pack manufacturing.
{"title":"Heterogeneous aging in a multi-cell lithium-ion battery system driven by manufacturing-induced variability in electrode microstructure: a physics-based simulation study","authors":"Parisa Akhtari Zavareh, Aditya Naveen Matam and Krishna Shah","doi":"10.1039/D5YA00182J","DOIUrl":"https://doi.org/10.1039/D5YA00182J","url":null,"abstract":"<p >Heterogeneous aging of lithium-ion (Li-ion) battery cells within a battery pack is a major challenge that limits the pack's overall performance, safety, and life. Variations in cell degradation rates lead to nonuniform charge/discharge behavior among cells in a pack, accelerated aging in some cells turning them into “weak links”, and reducing energy throughput at the pack level. While previous studies have investigated uneven aging driven by differences in capacity or resistance, limited attention has been given to the root causes of these variations, particularly those arising from manufacturing-induced differences in the electrode microstructure. This study addresses this gap by investigating the effects of variations in the mean active material particle size across cells, a key design parameter of a porous electrode, on the aging behavior of these cells when connected in series and parallel. Using an electrochemical battery model, the aging behavior of individual cells and the pack as a whole is investigated for three electrical configurations (<em>i.e.</em>, 1S4P, 4S1P, and 2S2P) at select C-rates and voltage windows. Results indicate that cells with smaller mean particle size degrade faster despite having a thinner SEI layer at the end of life, and even a minor variation of 1 µm in the mean active material particle size across cells can lead to significant uneven capacity fade across cells and accelerated aging of the pack, particularly at low C-rates. These findings highlight the critical impact that variability in the microstructure has on pack-level aging and provide insights into effective cell and pack manufacturing.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 2","pages":" 202-223"},"PeriodicalIF":4.3,"publicationDate":"2025-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2026/ya/d5ya00182j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146216715","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Fe–N–C catalysts have emerged as the most promising class of non-precious metal electrocatalysts for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs), offering favourable activity, structure tunability, and cost-effectiveness. However, challenges remain in achieving the performance and durability required for practical applications. This review systematically summarizes recent progress in Fe–N–C catalyst development, with a focus on synthetic strategies aimed at increasing the active site density, optimizing Fe–Nx coordination environments and potential engineering solutions to the membrane electrode assembly (MEA) based on Fe–N–C, particular attention is given to the pyrolysis atmosphere control, post-synthesis treatment, and optimizing the microstructure and catalytic performance. Furthermore, this review explores emerging approaches to integrate Fe–N–C catalysts into membrane electrode assemblies (MEAs), including ionomer–catalyst interaction tuning and electrode architecture optimization, with the goal of bridging the gap from laboratory activity to real-world fuel cell operation.
{"title":"Advancing Fe–N–C catalysts: synthesis strategies and performance enhancements for fuel cell applications","authors":"Bochen Li and Rhodri Jervis","doi":"10.1039/D5YA00256G","DOIUrl":"https://doi.org/10.1039/D5YA00256G","url":null,"abstract":"<p >Fe–N–C catalysts have emerged as the most promising class of non-precious metal electrocatalysts for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs), offering favourable activity, structure tunability, and cost-effectiveness. However, challenges remain in achieving the performance and durability required for practical applications. This review systematically summarizes recent progress in Fe–N–C catalyst development, with a focus on synthetic strategies aimed at increasing the active site density, optimizing Fe–N<small><sub><em>x</em></sub></small> coordination environments and potential engineering solutions to the membrane electrode assembly (MEA) based on Fe–N–C, particular attention is given to the pyrolysis atmosphere control, post-synthesis treatment, and optimizing the microstructure and catalytic performance. Furthermore, this review explores emerging approaches to integrate Fe–N–C catalysts into membrane electrode assemblies (MEAs), including ionomer–catalyst interaction tuning and electrode architecture optimization, with the goal of bridging the gap from laboratory activity to real-world fuel cell operation.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 12","pages":" 1412-1425"},"PeriodicalIF":4.3,"publicationDate":"2025-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ya/d5ya00256g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145665857","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}