Ifeanyi Michael Smarte Anekwe and Yusuf Makarfi Isa
Catalyst deactivation remains a fundamental challenge in heterogeneous catalysis, compromising performance, efficiency, and sustainability across numerous industrial processes. This review critically examines the principal deactivation pathways including coking, poisoning, thermal degradation, and mechanical damage and evaluates the breadth of regeneration strategies developed to restore catalytic activity. Traditional methods such as oxidation, gasification, and hydrogenation are assessed alongside emerging approaches like supercritical fluid extraction (SFE), microwave-assisted regeneration (MAR), plasma-assisted regeneration (PAR) and atomic layer deposition (ALD) techniques. The environmental implications and operational trade-offs associated with each regeneration method were evaluated. By integrating recent scientific advancements with bibliometric analysis, this study identifies prevailing research trends and exposes key knowledge gaps in catalyst regeneration. Unlike prior reviews, this work offers a holistic perspective that spans multiple deactivation mechanisms and regeneration routes. Insights into process optimization and environmental impact reduction are presented to guide future innovation in sustainable catalytic system design. By contrasting current progress with unexplored potential, this study provides a basis for promoting innovation and management of sustainable catalysts. It serves as a strategic roadmap for enhancing catalyst longevity and performance in next-generation industrial applications.
{"title":"Unlocking catalytic longevity: a critical review of catalyst deactivation pathways and regeneration technologies","authors":"Ifeanyi Michael Smarte Anekwe and Yusuf Makarfi Isa","doi":"10.1039/D5YA00015G","DOIUrl":"https://doi.org/10.1039/D5YA00015G","url":null,"abstract":"<p >Catalyst deactivation remains a fundamental challenge in heterogeneous catalysis, compromising performance, efficiency, and sustainability across numerous industrial processes. This review critically examines the principal deactivation pathways including coking, poisoning, thermal degradation, and mechanical damage and evaluates the breadth of regeneration strategies developed to restore catalytic activity. Traditional methods such as oxidation, gasification, and hydrogenation are assessed alongside emerging approaches like supercritical fluid extraction (SFE), microwave-assisted regeneration (MAR), plasma-assisted regeneration (PAR) and atomic layer deposition (ALD) techniques. The environmental implications and operational trade-offs associated with each regeneration method were evaluated. By integrating recent scientific advancements with bibliometric analysis, this study identifies prevailing research trends and exposes key knowledge gaps in catalyst regeneration. Unlike prior reviews, this work offers a holistic perspective that spans multiple deactivation mechanisms and regeneration routes. Insights into process optimization and environmental impact reduction are presented to guide future innovation in sustainable catalytic system design. By contrasting current progress with unexplored potential, this study provides a basis for promoting innovation and management of sustainable catalysts. It serves as a strategic roadmap for enhancing catalyst longevity and performance in next-generation industrial applications.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 9","pages":" 1075-1113"},"PeriodicalIF":4.3,"publicationDate":"2025-08-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ya/d5ya00015g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145028047","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}
Arjun Patel, Michael L. Rasche, Sourav Mallick, Sunuk Kim, Mo Jiang, Mariappan Parans Paranthaman, Herman Lopez and Ram B. Gupta
Continuous production of good quality low-cobalt Ni-rich cathode is needed as it can offer high capacity suitable for electric vehicles. However, the low-cobalt NCM-based materials suffer from a high cation mixing and poor rate capability. Also, proper optimization of co-precipitation reaction parameters as well as the manufacturing platform are needed to obtain NCM-precursor particles with uniform particle size and morphology. In order to address all the issues, in this work, a slug-flow-based manufacturing platform is utilized for the continuous production of Fe3+ substituted Ni0.85Co(0.1−x)Mn0.05FexC2O4 (where x = 0, 0.02, 0.04) precursors. The slug-flow manufacturing produces precursor particles with high yield and uniformity. The effect of reactants concentration on the product yield and composition is analyzed through mathematical modelling. Finally, the electrochemical performance of the Ni-rich cathodes with various amounts of Co and Fe content is analyzed through rate capability, cycling stability, and impedance analysis. This work provides key insight into: (i) reactor design for continuous production; (ii) mathematical modelling of the precipitation reaction parameter; and (iii) a detail study of the effect of Co-substitution with Fe3+ in Ni-rich NCM on its physical properties as well as electrochemical performance. We find that an intermediate Fe content provides optimum cathode with desired properties.
{"title":"Slug-flow-based continuous manufacturing of Fe-substituted Ni-rich NCM cathodes for lithium-ion batteries: synthesis and modeling","authors":"Arjun Patel, Michael L. Rasche, Sourav Mallick, Sunuk Kim, Mo Jiang, Mariappan Parans Paranthaman, Herman Lopez and Ram B. Gupta","doi":"10.1039/D5YA00032G","DOIUrl":"https://doi.org/10.1039/D5YA00032G","url":null,"abstract":"<p >Continuous production of good quality low-cobalt Ni-rich cathode is needed as it can offer high capacity suitable for electric vehicles. However, the low-cobalt NCM-based materials suffer from a high cation mixing and poor rate capability. Also, proper optimization of co-precipitation reaction parameters as well as the manufacturing platform are needed to obtain NCM-precursor particles with uniform particle size and morphology. In order to address all the issues, in this work, a slug-flow-based manufacturing platform is utilized for the continuous production of Fe<small><sup>3+</sup></small> substituted Ni<small><sub>0.85</sub></small>Co<small><sub>(0.1−<em>x</em>)</sub></small>Mn<small><sub>0.05</sub></small>Fe<small><sub><em>x</em></sub></small>C<small><sub>2</sub></small>O<small><sub>4</sub></small> (where <em>x</em> = 0, 0.02, 0.04) precursors. The slug-flow manufacturing produces precursor particles with high yield and uniformity. The effect of reactants concentration on the product yield and composition is analyzed through mathematical modelling. Finally, the electrochemical performance of the Ni-rich cathodes with various amounts of Co and Fe content is analyzed through rate capability, cycling stability, and impedance analysis. This work provides key insight into: (i) reactor design for continuous production; (ii) mathematical modelling of the precipitation reaction parameter; and (iii) a detail study of the effect of Co-substitution with Fe<small><sup>3+</sup></small> in Ni-rich NCM on its physical properties as well as electrochemical performance. We find that an intermediate Fe content provides optimum cathode with desired properties.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 10","pages":" 1267-1278"},"PeriodicalIF":4.3,"publicationDate":"2025-08-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ya/d5ya00032g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145248150","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}
Asma Kiran, Saleh S. Alarfaji, Muhammad Bilal Tahir and Muhammad Isa Khan
The identification of novel two-dimensional materials is often highly valued because of their extraordinary characteristics and prospective uses. This study presents a new bismuth selenide (Bi2Se3) monolayer based on density functional theory (DFT). Its bandgap, state density, and mobilities are determined and examined. This study investigates hydrogen storage in Bi2Se3 adorned with alkali metal (Li/Na and K) atoms. The optimal adsorption site for alkali metal (AM) atoms on the Bi2Se3 monolayer is located above an Se atom. The AM atoms are physically adsorbed on Bi2Se3, and the electronic charge shifts from these to the Bi2Se3 monolayer. In all scenarios examined, hydrogen molecules are physically adsorbed onto AM–Bi2Se3 complexes, suggesting that these systems could be employed for hydrogen storage. The K–Bi2Se3 monolayer shows the highest hydrogen storage capacity, with one potassium atom adsorbing up to 19 hydrogen molecules, while both Na–Bi2Se3 and Li–Bi2Se3 could adsorb 18 hydrogen molecules. It is estimated that the hydrogen-storage gravimetric capacities of AM–Bi2Se3 are within the US-DOE criteria, where the adatom coverage reaches about 6.71 wt% for K, 6.52 wt% for Na, and 6.66 wt% for Li.
{"title":"First principles study of alkali metal-decorated bismuth selenide for hydrogen storage applications","authors":"Asma Kiran, Saleh S. Alarfaji, Muhammad Bilal Tahir and Muhammad Isa Khan","doi":"10.1039/D5YA00149H","DOIUrl":"https://doi.org/10.1039/D5YA00149H","url":null,"abstract":"<p >The identification of novel two-dimensional materials is often highly valued because of their extraordinary characteristics and prospective uses. This study presents a new bismuth selenide (Bi<small><sub>2</sub></small>Se<small><sub>3</sub></small>) monolayer based on density functional theory (DFT). Its bandgap, state density, and mobilities are determined and examined. This study investigates hydrogen storage in Bi<small><sub>2</sub></small>Se<small><sub>3</sub></small> adorned with alkali metal (Li/Na and K) atoms. The optimal adsorption site for alkali metal (AM) atoms on the Bi<small><sub>2</sub></small>Se<small><sub>3</sub></small> monolayer is located above an Se atom. The AM atoms are physically adsorbed on Bi<small><sub>2</sub></small>Se<small><sub>3</sub></small>, and the electronic charge shifts from these to the Bi<small><sub>2</sub></small>Se<small><sub>3</sub></small> monolayer. In all scenarios examined, hydrogen molecules are physically adsorbed onto AM–Bi<small><sub>2</sub></small>Se<small><sub>3</sub></small> complexes, suggesting that these systems could be employed for hydrogen storage. The K–Bi<small><sub>2</sub></small>Se<small><sub>3</sub></small> monolayer shows the highest hydrogen storage capacity, with one potassium atom adsorbing up to 19 hydrogen molecules, while both Na–Bi<small><sub>2</sub></small>Se<small><sub>3</sub></small> and Li–Bi<small><sub>2</sub></small>Se<small><sub>3</sub></small> could adsorb 18 hydrogen molecules. It is estimated that the hydrogen-storage gravimetric capacities of AM–Bi<small><sub>2</sub></small>Se<small><sub>3</sub></small> are within the US-DOE criteria, where the adatom coverage reaches about 6.71 wt% for K, 6.52 wt% for Na, and 6.66 wt% for Li.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 10","pages":" 1251-1266"},"PeriodicalIF":4.3,"publicationDate":"2025-08-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ya/d5ya00149h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145248149","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}
Recently, rechargeable aqueous aluminum ion batteries (RAAIBs) have been a promising candidate as the next-generation secondary battery in the rechargeable battery industry owing to its enhanced theoretical specific energy, low cost, and environmental friendliness. The manufacturing cost and price of battery components are very low because they can be prepared in ambient atmosphere and have a simple manufacturing process, which is advantageous compared to other battery types. Furthermore, the raw materials that comprise the battery's components are easily available and not expensive. However, currently its inferior cycle stability precludes real industrial application. In this article, the current progress in development of RAAIBs is briefly summarized based on the type of aluminum salt, including aluminum fluoride, chloride, sulfide, nitride, and others. Additionally, research areas necessary for improving the electrochemical performance of RAAIB will be discussed.
{"title":"Aqueous rechargeable aluminum battery – a mini review","authors":"Ryohei Mori","doi":"10.1039/D5YA00148J","DOIUrl":"https://doi.org/10.1039/D5YA00148J","url":null,"abstract":"<p >Recently, rechargeable aqueous aluminum ion batteries (RAAIBs) have been a promising candidate as the next-generation secondary battery in the rechargeable battery industry owing to its enhanced theoretical specific energy, low cost, and environmental friendliness. The manufacturing cost and price of battery components are very low because they can be prepared in ambient atmosphere and have a simple manufacturing process, which is advantageous compared to other battery types. Furthermore, the raw materials that comprise the battery's components are easily available and not expensive. However, currently its inferior cycle stability precludes real industrial application. In this article, the current progress in development of RAAIBs is briefly summarized based on the type of aluminum salt, including aluminum fluoride, chloride, sulfide, nitride, and others. Additionally, research areas necessary for improving the electrochemical performance of RAAIB will be discussed.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 11","pages":" 1321-1336"},"PeriodicalIF":4.3,"publicationDate":"2025-08-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ya/d5ya00148j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145449401","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}
With rising demand for lithium-ion batteries, efficient recycling is crucial. While conventional methods face cost and environmental challenges, electrochemical recovery offers a sustainable and energy-efficient alternative. In this study, we investigate the electrochemical recovery of lithium-ions from spent lithium iron phosphate batteries using carbon-coated lithium iron phosphate electrodes, with a focus on the influence of pH adjustment and competing ion effects. Our results demonstrate that NaOH-adjusted electrolytes provide the highest lithium-ion recovery efficiency, with an average removal capacity of 18 mgLi gLFP−1 over 50 cycles. However, prolonged cycling leads to capacity fading, particularly in the presence of competing cations such as Na+ and K+, which impact lithium selectivity and electrode stability. These findings underscore the importance of optimizing electrolyte conditions and electrode materials to enhance long-term performance. Future research should explore alternative pH control strategies and scalable process designs to facilitate industrial implementation. Advancing electrochemical lithium-ion recovery aligns with broader sustainability goals, offering a viable route toward circular battery recycling and reduced environmental impact.
{"title":"Competing ion effects and electrolyte optimization for electrochemical lithium extraction from spent lithium iron phosphate battery cathodes","authors":"Stefanie Arnold and Volker Presser","doi":"10.1039/D5YA00172B","DOIUrl":"https://doi.org/10.1039/D5YA00172B","url":null,"abstract":"<p >With rising demand for lithium-ion batteries, efficient recycling is crucial. While conventional methods face cost and environmental challenges, electrochemical recovery offers a sustainable and energy-efficient alternative. In this study, we investigate the electrochemical recovery of lithium-ions from spent lithium iron phosphate batteries using carbon-coated lithium iron phosphate electrodes, with a focus on the influence of pH adjustment and competing ion effects. Our results demonstrate that NaOH-adjusted electrolytes provide the highest lithium-ion recovery efficiency, with an average removal capacity of 18 mg<small><sub>Li</sub></small> g<small><sub>LFP</sub></small><small><sup>−1</sup></small> over 50 cycles. However, prolonged cycling leads to capacity fading, particularly in the presence of competing cations such as Na<small><sup>+</sup></small> and K<small><sup>+</sup></small>, which impact lithium selectivity and electrode stability. These findings underscore the importance of optimizing electrolyte conditions and electrode materials to enhance long-term performance. Future research should explore alternative pH control strategies and scalable process designs to facilitate industrial implementation. Advancing electrochemical lithium-ion recovery aligns with broader sustainability goals, offering a viable route toward circular battery recycling and reduced environmental impact.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 9","pages":" 1114-1129"},"PeriodicalIF":4.3,"publicationDate":"2025-08-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ya/d5ya00172b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145028048","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}
Ernst H. Hechter, Aderemi B. Haruna, Xiao-Yu Yang, Maxwell W. Terban, Héctor D. Abruña, Dean H. Barrett and Kenneth I. Ozoemena
High-entropy spinel oxide (Cu0.2Co0.2Fe0.2Mn0.2Ni0.2)3O4 nanoparticles were synthesized and confined in Vulcan carbon for use as a bifunctional OER/ORR catalyst in a rechargeable zinc–air battery (RZAB). A partially inverted spinel phase with a distorted O2− lattice was found, with metals randomly distributed in M2+ and M3+ states. Copper was the exception, being found only as Cu2+. Strong metal oxide–support interactions were noted, as well as ferromagnetism. The composite exhibited moderate intrinsic catalytic activity, with overpotentials and current densities comparable to those of commercial platinum on carbon catalysts even at low loadings: an example being Ej=10 of 1.53 V. Magnetic enhancement was noted and associated with the final OER and initial ORR electron transfers. The performance of the test RZAB was greatly improved when an external magnetic field was applied, with peak power increasing from 101 to 169 mW cm−2. We report the most significant magnetic enhancement in the RZAB power profile in the literature to date, as well as improved RZAB stability and areal energy, achieving 43.2 mWh cm−2 for over 140 h during 36 h charge–discharge cycles. This work offers insights into the mechanism of magnetic enhancement in the case of high-entropy materials, and illustrates the use of combined strategies to achieve stable, cost-efficient, and effective bifunctional OER/ORR electrocatalysis.
{"title":"Magnetic enhancement of high-entropy oxide electrocatalysts for high areal-energy rechargeable zinc air batteries†","authors":"Ernst H. Hechter, Aderemi B. Haruna, Xiao-Yu Yang, Maxwell W. Terban, Héctor D. Abruña, Dean H. Barrett and Kenneth I. Ozoemena","doi":"10.1039/D5YA00091B","DOIUrl":"https://doi.org/10.1039/D5YA00091B","url":null,"abstract":"<p >High-entropy spinel oxide (Cu<small><sub>0.2</sub></small>Co<small><sub>0.2</sub></small>Fe<small><sub>0.2</sub></small>Mn<small><sub>0.2</sub></small>Ni<small><sub>0.2</sub></small>)<small><sub>3</sub></small>O<small><sub>4</sub></small> nanoparticles were synthesized and confined in Vulcan carbon for use as a bifunctional OER/ORR catalyst in a rechargeable zinc–air battery (RZAB). A partially inverted spinel phase with a distorted O<small><sup>2−</sup></small> lattice was found, with metals randomly distributed in M<small><sup>2+</sup></small> and M<small><sup>3+</sup></small> states. Copper was the exception, being found only as Cu<small><sup>2+</sup></small>. Strong metal oxide–support interactions were noted, as well as ferromagnetism. The composite exhibited moderate intrinsic catalytic activity, with overpotentials and current densities comparable to those of commercial platinum on carbon catalysts even at low loadings: an example being <em>E</em><small><sub><em>j</em>=10</sub></small> of 1.53 V. Magnetic enhancement was noted and associated with the final OER and initial ORR electron transfers. The performance of the test RZAB was greatly improved when an external magnetic field was applied, with peak power increasing from 101 to 169 mW cm<small><sup>−2</sup></small>. We report the most significant magnetic enhancement in the RZAB power profile in the literature to date, as well as improved RZAB stability and areal energy, achieving 43.2 mWh cm<small><sup>−2</sup></small> for over 140 h during 36 h charge–discharge cycles. This work offers insights into the mechanism of magnetic enhancement in the case of high-entropy materials, and illustrates the use of combined strategies to achieve stable, cost-efficient, and effective bifunctional OER/ORR electrocatalysis.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 10","pages":" 1229-1240"},"PeriodicalIF":4.3,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ya/d5ya00091b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145248101","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}
Aqueous zinc-ion batteries (ZIBs) are an attractive storage solution for renewable energy storage system (ESS) applications. Despite the intrinsic safety, eco-friendliness, and low cost of aqueous ZIBs, their practical application is severely hindered by the unavailability of high-capacity and robust cathode materials. Vanadium-based cathodes with various structures, large layer spacing, and different oxidation states are considered to be suitable cathode candidates for ZIBs. In this work, we studied 2D layered VSe2 with high pseudocapacitive-mediated Zn-ion storage as a cathode for aqueous zinc-ion batteries. The VSe2 cathode reversibly hosted zinc ions with a capacity of 205 mAh g−1 at 0.2 A g−1, maintaining a capacity of 135 mAh g−1 at 8 A g−1 and a stability of 98% after 600 cycles at 1 A g−1, favoured by its 2D layered structure with defects and metallic conducting nature. The Zn-ion storage mechanism and kinetics in the cathode are examined using ex situ XRD, XPS, TEM, and GITT studies, and it is found that the favourable interlayer spacing with structural defects efficiently stored Zn-ions through a high contribution from capacitive-mediated storage. The favourable architecture enables fast Zn-ion diffusion and high capacity at a high current rate with good stability. The current work emphasizes the potential for the rational design of several transition-metal–dichalcogenide-based cathodes with strong pseudocapacitive storage for sustainable energy storage systems such as aqueous ZIBs.
水锌离子电池(zib)是一种有吸引力的可再生能源存储系统(ESS)应用的存储解决方案。尽管水基ZIBs具有固有的安全性、环保性和低成本,但由于缺乏高容量和坚固的阴极材料,它们的实际应用受到严重阻碍。具有多种结构、大层间距和不同氧化态的钒基阴极被认为是zbs的合适阴极候选材料。在这项工作中,我们研究了具有高假电容介导的锌离子存储的二维层状VSe2作为水锌离子电池的阴极。在0.2 a g−1电流下,VSe2阴极可逆负载的锌离子容量为205 mAh g−1,在8 a g−1电流下可保持135 mAh g−1的容量,在1 a g−1电流下循环600次后稳定性为98%,这有利于其具有缺陷和金属导电性质的二维层状结构。利用x射线衍射(XRD)、XPS、透射电镜(TEM)和红外光谱(git)研究了锌离子在阴极中的储存机理和动力学,发现具有结构缺陷的层间空间通过电容介导的高贡献有效地储存了锌离子。良好的结构使锌离子在高电流速率下快速扩散和高容量具有良好的稳定性。目前的工作强调了合理设计几种基于过渡金属-二硫族化合物的阴极的潜力,这些阴极具有强假电容存储,可用于可持续的能量存储系统,如水性ZIBs。
{"title":"2D layered VSe2 with high pseudocapacitive Zn-ion storage as a cathode for high-power zinc-ion batteries","authors":"Saddam Hussain, Mayanmi Zimik, Meghali Devi, Md Kasif and Ranjith Thangavel","doi":"10.1039/D5YA00130G","DOIUrl":"https://doi.org/10.1039/D5YA00130G","url":null,"abstract":"<p >Aqueous zinc-ion batteries (ZIBs) are an attractive storage solution for renewable energy storage system (ESS) applications. Despite the intrinsic safety, eco-friendliness, and low cost of aqueous ZIBs, their practical application is severely hindered by the unavailability of high-capacity and robust cathode materials. Vanadium-based cathodes with various structures, large layer spacing, and different oxidation states are considered to be suitable cathode candidates for ZIBs. In this work, we studied 2D layered VSe<small><sub>2</sub></small> with high pseudocapacitive-mediated Zn-ion storage as a cathode for aqueous zinc-ion batteries. The VSe<small><sub>2</sub></small> cathode reversibly hosted zinc ions with a capacity of 205 mAh g<small><sup>−1</sup></small> at 0.2 A g<small><sup>−1</sup></small>, maintaining a capacity of 135 mAh g<small><sup>−1</sup></small> at 8 A g<small><sup>−1</sup></small> and a stability of 98% after 600 cycles at 1 A g<small><sup>−1</sup></small>, favoured by its 2D layered structure with defects and metallic conducting nature. The Zn-ion storage mechanism and kinetics in the cathode are examined using <em>ex situ</em> XRD, XPS, TEM, and GITT studies, and it is found that the favourable interlayer spacing with structural defects efficiently stored Zn-ions through a high contribution from capacitive-mediated storage. The favourable architecture enables fast Zn-ion diffusion and high capacity at a high current rate with good stability. The current work emphasizes the potential for the rational design of several transition-metal–dichalcogenide-based cathodes with strong pseudocapacitive storage for sustainable energy storage systems such as aqueous ZIBs.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 9","pages":" 1154-1166"},"PeriodicalIF":4.3,"publicationDate":"2025-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ya/d5ya00130g?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145028051","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}
Hybrid electrolytes are comprised of a salt-containing polymer and an ion-conducting ceramic. The general appeal of these electrolytes is that they combine the desirable properties of each component. Namely, the flexibility, processability and interface compatibility of the polymer and the mechanical strength and high ionic conductivity of the ceramic. In this work, hybrid electrolytes comprised of poly(ethylene oxide) (PEO) and Li1.5Al0.5Ge1.5(PO4)3 (LAGP) were prepared using two different methods: solvent casting in acetonitrile and melt processing using a micro compounder. The presence of added solvents has been shown to impact the properties and stability of polymer electrolytes, but the effect of residual solvents on hybrid electrolytes has not been extensively investigated. Hybrid electrolytes prepared by solvent-free melt processing were compared to those prepared by solution casting, with and without vacuum drying, to determine the impact of solvent exposure on the properties of the electrolyte. Preparation via melt processing improved the dispersion of the ceramic phase in the polymer matrix which resulted in lower tortuosity and higher ionic conductivity. The absence of acetonitrile and low water content in the melt-processed sample improved stability during long-term cycling in Li–Li symmetric cells.
{"title":"The impact of solvent exposure during preparation on the performance of poly(ethylene) oxide–Li1.5Al0.5Ge1.5(PO4)3 hybrid electrolytes","authors":"Gabrielle Foran, Cédric Barcha, Caroline St-Antoine, Arnaud Prébé and Mickael Dollé","doi":"10.1039/D5YA00082C","DOIUrl":"https://doi.org/10.1039/D5YA00082C","url":null,"abstract":"<p >Hybrid electrolytes are comprised of a salt-containing polymer and an ion-conducting ceramic. The general appeal of these electrolytes is that they combine the desirable properties of each component. Namely, the flexibility, processability and interface compatibility of the polymer and the mechanical strength and high ionic conductivity of the ceramic. In this work, hybrid electrolytes comprised of poly(ethylene oxide) (PEO) and Li<small><sub>1.5</sub></small>Al<small><sub>0.5</sub></small>Ge<small><sub>1.5</sub></small>(PO<small><sub>4</sub></small>)<small><sub>3</sub></small> (LAGP) were prepared using two different methods: solvent casting in acetonitrile and melt processing using a micro compounder. The presence of added solvents has been shown to impact the properties and stability of polymer electrolytes, but the effect of residual solvents on hybrid electrolytes has not been extensively investigated. Hybrid electrolytes prepared by solvent-free melt processing were compared to those prepared by solution casting, with and without vacuum drying, to determine the impact of solvent exposure on the properties of the electrolyte. Preparation <em>via</em> melt processing improved the dispersion of the ceramic phase in the polymer matrix which resulted in lower tortuosity and higher ionic conductivity. The absence of acetonitrile and low water content in the melt-processed sample improved stability during long-term cycling in Li–Li symmetric cells.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 9","pages":" 1135-1153"},"PeriodicalIF":4.3,"publicationDate":"2025-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ya/d5ya00082c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145028050","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}
Varsha Joseph, Nara Kim, Sae Young Lee, Reverant Crispin, Tae Hyun Park and Ziyauddin Khan
Zinc metal batteries suffer from dendrite formation, hydrogen evolution, and interfacial instability. While water-in-salt electrolytes (WiSEs) suppress side reactions and hydrogels enhance interfacial stability, WiSE systems are costly and viscous, and conventional hydrogels contain excess water, promoting hydrogen evolution. To overcome these limitations, we developed a polyethylene glycol-based water-in-salt hydrogel (WiSH) electrolyte, incorporating tunable concentrations of zinc triflate (Zn(OTf)2) from 1 to 4 mol kg−1. The optimized 4 mol kg−1 formulation enabled dendrite free and corrosion-free zinc plating/stripping in symmetric Zn‖Zn cells for over 2000 hours at 1 mA cm−2 (1 mAh cm−2 area capacity), demonstrating exceptional long-term stability. The WiSH electrolyte exhibited improved mechanical strength and toughness with increasing salt concentration, attributed to stronger ionic crosslinking within the hydrogel matrix. Rheological and spectroscopic analyses confirmed the formation of a robust, densely crosslinked polymer network critical for stable and uniform Zn electrodeposition. Furthermore, a Zn–lignin full cell using the WiSH electrolyte achieved an energy density of 25 Wh kg−1 and 506 W kg−1 of specific power, highlighting its potential for energy storage systems. These results establish WiSH as a promising electrolyte platform for next-generation zinc batteries.
锌金属电池受到枝晶形成、析氢和界面不稳定的影响。虽然盐中水电解质(WiSE)可以抑制副反应,水凝胶可以增强界面稳定性,但WiSE系统价格昂贵且粘稠,而且传统的水凝胶含有多余的水,会促进氢的析出。为了克服这些限制,我们开发了一种基于聚乙二醇的盐中水凝胶(WiSH)电解质,加入了可调浓度的三酸锌(Zn(OTf)2),从1到4 mol kg−1。优化的4mol kg−1配方使对称Zn‖锌电池在1ma cm−2 (1mah cm−2面积容量)下无枝晶和无腐蚀的镀锌/剥离超过2000小时,表现出卓越的长期稳定性。随着盐浓度的增加,WiSH电解质表现出更好的机械强度和韧性,这归因于水凝胶基质内更强的离子交联。流变学和光谱分析证实了坚固、密集交联的聚合物网络的形成,这对稳定和均匀的锌电沉积至关重要。此外,使用WiSH电解质的锌木质素全电池实现了25 Wh kg - 1的能量密度和506 W kg - 1的比功率,突出了其储能系统的潜力。这些结果奠定了WiSH作为下一代锌电池电解质平台的前景。
{"title":"Water-in-salt hydrogel electrolyte for dendrite-free Zn deposition","authors":"Varsha Joseph, Nara Kim, Sae Young Lee, Reverant Crispin, Tae Hyun Park and Ziyauddin Khan","doi":"10.1039/D5YA00169B","DOIUrl":"https://doi.org/10.1039/D5YA00169B","url":null,"abstract":"<p >Zinc metal batteries suffer from dendrite formation, hydrogen evolution, and interfacial instability. While water-in-salt electrolytes (WiSEs) suppress side reactions and hydrogels enhance interfacial stability, WiSE systems are costly and viscous, and conventional hydrogels contain excess water, promoting hydrogen evolution. To overcome these limitations, we developed a polyethylene glycol-based water-in-salt hydrogel (WiSH) electrolyte, incorporating tunable concentrations of zinc triflate (Zn(OTf)<small><sub>2</sub></small>) from 1 to 4 mol kg<small><sup>−1</sup></small>. The optimized 4 mol kg<small><sup>−1</sup></small> formulation enabled dendrite free and corrosion-free zinc plating/stripping in symmetric Zn‖Zn cells for over 2000 hours at 1 mA cm<small><sup>−2</sup></small> (1 mAh cm<small><sup>−2</sup></small> area capacity), demonstrating exceptional long-term stability. The WiSH electrolyte exhibited improved mechanical strength and toughness with increasing salt concentration, attributed to stronger ionic crosslinking within the hydrogel matrix. Rheological and spectroscopic analyses confirmed the formation of a robust, densely crosslinked polymer network critical for stable and uniform Zn electrodeposition. Furthermore, a Zn–lignin full cell using the WiSH electrolyte achieved an energy density of 25 Wh kg<small><sup>−1</sup></small> and 506 W kg<small><sup>−1</sup></small> of specific power, highlighting its potential for energy storage systems. These results establish WiSH as a promising electrolyte platform for next-generation zinc batteries.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 9","pages":" 1167-1178"},"PeriodicalIF":4.3,"publicationDate":"2025-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ya/d5ya00169b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145028052","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}
Masakazu Yamagiwa, Naoya Fujiwara, Yusuke Kofuji and Ryota Kitagawa
The movement of water in zero-gap CO2 electrolysis cells from the anode side to the cathode side may potentially hamper CO2 transport to the reduction catalyst, ultimately resulting in reduced CO production. To help prevent this, it is desirable to understand where and how water accumulates. Dynamic water transport in zero-gap CO2 electrolysis cells was visualized by both visible light and X-ray operando imaging. The water breakthrough to the cathode gas channel was visualized by visible light camera observation, while the water seepage through the membrane-electrode assembly was visualized by X-ray radiography. Each frame from the X-ray radiography video was converted to a spatial map of the liquid saturation, and the consecutive frames were used to calculate the liquid flux from the anode to the cathode. This quantitative analysis provides insight into the locations of water accumulation, which tended to occur under the ribs. The flux data showed that, when the water accumulated in the cathode to a certain extent, breakthrough to the cathode flow channel became significant, and water migration from the cathode parts under the ribs to that facing the flow channel also proceeded.
{"title":"Operando analysis of water transport in zero-gap CO2 electrolysis cells†","authors":"Masakazu Yamagiwa, Naoya Fujiwara, Yusuke Kofuji and Ryota Kitagawa","doi":"10.1039/D5YA00111K","DOIUrl":"https://doi.org/10.1039/D5YA00111K","url":null,"abstract":"<p >The movement of water in zero-gap CO<small><sub>2</sub></small> electrolysis cells from the anode side to the cathode side may potentially hamper CO<small><sub>2</sub></small> transport to the reduction catalyst, ultimately resulting in reduced CO production. To help prevent this, it is desirable to understand where and how water accumulates. Dynamic water transport in zero-gap CO<small><sub>2</sub></small> electrolysis cells was visualized by both visible light and X-ray <em>operando</em> imaging. The water breakthrough to the cathode gas channel was visualized by visible light camera observation, while the water seepage through the membrane-electrode assembly was visualized by X-ray radiography. Each frame from the X-ray radiography video was converted to a spatial map of the liquid saturation, and the consecutive frames were used to calculate the liquid flux from the anode to the cathode. This quantitative analysis provides insight into the locations of water accumulation, which tended to occur under the ribs. The flux data showed that, when the water accumulated in the cathode to a certain extent, breakthrough to the cathode flow channel became significant, and water migration from the cathode parts under the ribs to that facing the flow channel also proceeded.</p>","PeriodicalId":72913,"journal":{"name":"Energy advances","volume":" 9","pages":" 1130-1134"},"PeriodicalIF":4.3,"publicationDate":"2025-07-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/ya/d5ya00111k?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145028049","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}