Pub Date : 2026-02-10DOI: 10.1016/j.cej.2026.173601
Leila Shahriari, Tyrus Antonson, Sang Eon Han, Sang M. Han, Maryam Hojati, Sungjin Kim
Carbon dioxide (CO2) mineralization offers a promising strategy to convert waste carbon into valuable carbonate feedstocks. Practical industrial implementation, however, requires precise reaction engineering to optimize efficiency while controlling particle morphology and polymorphism. We present a systematically designed reaction-engineering framework that elucidates the mechanistic controls governing catechol-mediated CO2 mineralization, inspired by biomineralization processes in marine environments, enabling tunable control over calcium carbonate (CaCO3) phase, morphology, and particle size. Within this framework, we integrate tannic acid (TA) and ultrasonic irradiation to enhance reaction kinetics and CO2 utilization. The combined use of TA and ultrasonication enhances the product yield by up to ∼300% compared with the control without polyphenol and ultrasonication. The improvement is attributed to the Ca-binding of TA, which accelerates nucleation and stabilizes the metastable vaterite phase, along with ultrasound-induced improvements in CO2 dissolution and mass transfer. Under these conditions, uniform spherical vaterite particles with diameters of 1–2 μm are produced as a result of intensified nucleation, enhanced CO2 dissolution, and the generation of smaller CO2 bubbles that serve as nucleation templates. These findings highlight a bioinspired organic-inorganic reaction engineering framework for scalable, efficient CO2 utilization toward sustainable manufacturing applications.
{"title":"Bioinspired reaction engineering of CO2 mineralization assisted by tannic acid and ultrasonication","authors":"Leila Shahriari, Tyrus Antonson, Sang Eon Han, Sang M. Han, Maryam Hojati, Sungjin Kim","doi":"10.1016/j.cej.2026.173601","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173601","url":null,"abstract":"Carbon dioxide (CO<ce:inf loc=\"post\">2</ce:inf>) mineralization offers a promising strategy to convert waste carbon into valuable carbonate feedstocks. Practical industrial implementation, however, requires precise reaction engineering to optimize efficiency while controlling particle morphology and polymorphism. We present a systematically designed reaction-engineering framework that elucidates the mechanistic controls governing catechol-mediated CO<ce:inf loc=\"post\">2</ce:inf> mineralization, inspired by biomineralization processes in marine environments, enabling tunable control over calcium carbonate (CaCO<ce:inf loc=\"post\">3</ce:inf>) phase, morphology, and particle size. Within this framework, we integrate tannic acid (TA) and ultrasonic irradiation to enhance reaction kinetics and CO<ce:inf loc=\"post\">2</ce:inf> utilization. The combined use of TA and ultrasonication enhances the product yield by up to ∼300% compared with the control without polyphenol and ultrasonication. The improvement is attributed to the Ca-binding of TA, which accelerates nucleation and stabilizes the metastable vaterite phase, along with ultrasound-induced improvements in CO<ce:inf loc=\"post\">2</ce:inf> dissolution and mass transfer. Under these conditions, uniform spherical vaterite particles with diameters of 1–2 μm are produced as a result of intensified nucleation, enhanced CO<ce:inf loc=\"post\">2</ce:inf> dissolution, and the generation of smaller CO<ce:inf loc=\"post\">2</ce:inf> bubbles that serve as nucleation templates. These findings highlight a bioinspired organic-inorganic reaction engineering framework for scalable, efficient CO<ce:inf loc=\"post\">2</ce:inf> utilization toward sustainable manufacturing applications.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"244 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146711","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Gouty arthritis (GA), caused by monosodium urate crystal deposition in the context of persistent hyperuricemia, remains difficult to treat due to the inability of conventional therapies to simultaneously control uric acid (UA) levels, oxidative stress, and inflammation. To overcome this, we develop a biomimetic nanozyme composed of AuPt bimetallic nanozymes cloaked with erythrocyte membrane (AuPt@EM). It integrates prolonged circulation with cascade enzyme activities to achieve systemic UA reduction, local crystal clearance, and modulation of the inflammatory hypoxic microenvironment. AuPt@EM exhibits superoxide dismutase-like and catalase-like activities, efficiently scavenging ROS and generating oxygen, thereby amplifying its uricase-like activity to sustainably reduce UA. This nanozyme reduces ROS, suppresses the PI3K/AKT/HIF-1α pathway, and promotes HIF-1α degradation, which reprograms macrophages from the pro-inflammatory M1 phenotype toward the anti-inflammatory M2 phenotype. In vivo, AuPt@EM facilitates crystal clearance, alleviates joint inflammation, and preserves cartilage integrity. Moreover, it restores systemic immune balance by elevating IL-10 while decreasing IL-1β and IL-6. This study establishes an integrated therapeutic paradigm that combines UA level control, crystal dissolution, and inflammatory hypoxic microenvironment modulation, offering a promising strategy for precise and effective intervention in hyperuricemia and gouty arthritis.
{"title":"A biomimetic nanozyme enabling prolonged blood circulation for precise Theranostics in hyperuricemia and gouty arthritis","authors":"Lujie Yu, Qin Liu, Shutong Wu, Jian Zhang, Lin Chen, Huifang Hao, Mingxin Zhao, Chunmei Jiang, Weiwei Zhang, Ziliang Zheng, Ruiping Zhang","doi":"10.1016/j.cej.2026.173944","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173944","url":null,"abstract":"Gouty arthritis (GA), caused by monosodium urate crystal deposition in the context of persistent hyperuricemia, remains difficult to treat due to the inability of conventional therapies to simultaneously control uric acid (UA) levels, oxidative stress, and inflammation. To overcome this, we develop a biomimetic nanozyme composed of AuPt bimetallic nanozymes cloaked with erythrocyte membrane (AuPt@EM). It integrates prolonged circulation with cascade enzyme activities to achieve systemic UA reduction, local crystal clearance, and modulation of the inflammatory hypoxic microenvironment. AuPt@EM exhibits superoxide dismutase-like and catalase-like activities, efficiently scavenging ROS and generating oxygen, thereby amplifying its uricase-like activity to sustainably reduce UA. This nanozyme reduces ROS, suppresses the PI3K/AKT/HIF-1α pathway, and promotes HIF-1α degradation, which reprograms macrophages from the pro-inflammatory M1 phenotype toward the anti-inflammatory M2 phenotype. In vivo, AuPt@EM facilitates crystal clearance, alleviates joint inflammation, and preserves cartilage integrity. Moreover, it restores systemic immune balance by elevating IL-10 while decreasing IL-1β and IL-6. This study establishes an integrated therapeutic paradigm that combines UA level control, crystal dissolution, and inflammatory hypoxic microenvironment modulation, offering a promising strategy for precise and effective intervention in hyperuricemia and gouty arthritis.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"73 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146186","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-10DOI: 10.1016/j.cej.2026.173952
Feike Zhang, Jun Wang, Guixi Wang, Xiaoke Li, Weikun Ren, Jinghua Yang, Ruilong Liu, Shiyu Wang, Kang Ji, Shuyun Yao, Yingjie Ji, Jingyu Wu, Wanlong Bai, Zhiyu Yang, Yi-Ming Yan
Formate represents a promising liquid hydrogen carrier for advancing carbon neutrality goals while serving as a key intermediate in closed-loop carbon cycling systems. Despite their resistance to carbonaceous poisoning that plagues Pt catalysts, Pd-based electrocatalysts for formate oxidation reaction (FOR) suffer from performance degradation due to accumulating hydrogen intermediates (H*) that block active sites. Here, we report a MoS₂-supported Pd nanocatalyst (Pd/MoS₂/C) featuring bidirectional interfacial electronic interactions that fundamentally address H* poisoning through facilitated hydrogen spillover. This engineered interface establishes a two-way electronic communication: electron transfer from MoS₂ to Pd induces a downshift in the Pd d-band center, weakening Pd–H* bonds and promoting H* desorption, while simultaneously, Pd catalyzes a 2H-to-1 T phase transition in MoS₂, enhancing its electronic conductivity and hydrogen-hosting capability. The resulting catalyst achieves an exceptional mass activity of 7.92 A mgPd−1 for FOR—5.18-fold higher than commercial Pd/C. Through combined spectroscopic analyses and density functional theory calculations, we demonstrate that this bidirectional electronic coupling creates a self-sustaining hydrogen spillover pathway functioning as a hydrogen diode that continuously regenerates active Pd sites during catalysis. Our findings establish bidirectional interface engineering as a powerful approach for overcoming hydrogen-induced deactivation in Pd-based systems and highlight the critical role of phase-tunable 2D materials in designing high-performance electrocatalysts for sustainable energy conversion.
甲酸盐是一种很有前途的液氢载体，可以促进碳中和目标的实现，同时也是闭环碳循环系统的关键中间体。尽管铂催化剂具有抗碳中毒的能力，但甲酸酯氧化反应（for）的钯基电催化剂由于积累氢中间体（H*）阻塞活性位点而导致性能下降。在这里，我们报道了一种具有双向界面电子相互作用的MoS₂负载的Pd纳米催化剂（Pd/MoS₂/C），该催化剂通过促进氢溢出从根本上解决了氢中毒问题。该工程界面建立了双向电子通信：从MoS 2到Pd的电子转移引起Pd d带中心的下移，减弱Pd - H*键并促进H*解吸，同时，Pd催化MoS 2的2h -1 T相变，增强其电子导电性和载氢能力。所得催化剂的质量活性为7.92 A mgPd−1，比商用Pd/C高5.18倍。通过结合光谱分析和密度泛函理论计算，我们证明了这种双向电子耦合创造了一个自我维持的氢溢出途径，作为一个氢二极管，在催化过程中不断再生活性Pd位点。我们的研究结果确立了双向界面工程是克服pd基体系中氢诱导失活的有力方法，并强调了相可调二维材料在设计高性能电催化剂以实现可持续能量转换方面的关键作用。
{"title":"Bidirectionally interfacial electronic interactions in Pd/MoS₂ enable efficient formate oxidation through facilitated hydrogen spillover","authors":"Feike Zhang, Jun Wang, Guixi Wang, Xiaoke Li, Weikun Ren, Jinghua Yang, Ruilong Liu, Shiyu Wang, Kang Ji, Shuyun Yao, Yingjie Ji, Jingyu Wu, Wanlong Bai, Zhiyu Yang, Yi-Ming Yan","doi":"10.1016/j.cej.2026.173952","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173952","url":null,"abstract":"Formate represents a promising liquid hydrogen carrier for advancing carbon neutrality goals while serving as a key intermediate in closed-loop carbon cycling systems. Despite their resistance to carbonaceous poisoning that plagues Pt catalysts, Pd-based electrocatalysts for formate oxidation reaction (FOR) suffer from performance degradation due to accumulating hydrogen intermediates (H*) that block active sites. Here, we report a MoS₂-supported Pd nanocatalyst (Pd/MoS₂/C) featuring bidirectional interfacial electronic interactions that fundamentally address H* poisoning through facilitated hydrogen spillover. This engineered interface establishes a two-way electronic communication: electron transfer from MoS₂ to Pd induces a downshift in the Pd d-band center, weakening Pd–H* bonds and promoting H* desorption, while simultaneously, Pd catalyzes a 2H-to-1 T phase transition in MoS₂, enhancing its electronic conductivity and hydrogen-hosting capability. The resulting catalyst achieves an exceptional mass activity of 7.92 A mg<ce:inf loc=\"post\">Pd</ce:inf><ce:sup loc=\"post\">−1</ce:sup> for FOR—5.18-fold higher than commercial Pd/C. Through combined spectroscopic analyses and density functional theory calculations, we demonstrate that this bidirectional electronic coupling creates a self-sustaining hydrogen spillover pathway functioning as a hydrogen diode that continuously regenerates active Pd sites during catalysis. Our findings establish bidirectional interface engineering as a powerful approach for overcoming hydrogen-induced deactivation in Pd-based systems and highlight the critical role of phase-tunable 2D materials in designing high-performance electrocatalysts for sustainable energy conversion.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"89 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146709","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Phase change materials (PCMs) have demonstrated substantial potential in multiple energy storage applications. However, critical obstacles remain, including PCM leakage in liquid state, structural failure under external loads, and the lack of photo-/magnetothermal storage capability. Inspired by natural honeycomb structure, this work presents a one-step hydrothermal method of in situ growing Ni3S2 nanosheet arrays on nickel foam (Ni foam), subsequently encapsulating polyethylene glycol (PEG) to fabricate multifunctional PCM composites. Benefiting from the honeycomb-like architectures and the hydrogen bonding interactions between Ni3S2 nanosheets and PEG chains, the Ni@Ni3S2/PEG composite maintains excellent shape stability even after 8 h of intensive thermal cycling. Notably, the composite exhibits superior mechanical properties at both ambient temperature and above the melting point, with compressive strength enhanced by 430% to 780% compared to pristine PEG, alongside minimal leakage. Comprehensive analysis reveals that Ni3S2 nanosheets serve as heterogeneous nucleation sites, effectively reducing the crystallization activation energy of PEG from 160.3 kJ/mol to 125.6 kJ/mol. Simultaneously, the geometric confinement effect of Ni3S2 nanosheets guides the ordered arrangement of PEG chains and facilitates their rapid crystallization. Moreover, the composite successfully integrates magnetic-induced heating and photothermal conversion capabilities. Broadband light absorption (95.2%) is achieved by synergistically enhancing multiple scattering through a three-dimensional (3D) Ni foam porous structure integrated with Ni3S2 nanosheet arrays. A constructed solar-powered electricity generation device achieves a sustained current output of 168.35 mA. This work provides a facile design strategy for realizing synergistic enhancement of encapsulation performance, thermal storage density, and photothermal conversion in porous foam-based PCMs.
{"title":"Honeycomb-inspired Ni/Ni3S2 foam stabilizing phase change composites for multiple energy storage","authors":"Zi-jie Huang, Qin Wang, Zi-cheng Tang, Hao-hao Song, Jing-hui Yang, De-xiang Sun, Xiao-dong Qi, Yong Wang","doi":"10.1016/j.cej.2026.174023","DOIUrl":"https://doi.org/10.1016/j.cej.2026.174023","url":null,"abstract":"Phase change materials (PCMs) have demonstrated substantial potential in multiple energy storage applications. However, critical obstacles remain, including PCM leakage in liquid state, structural failure under external loads, and the lack of photo-/magnetothermal storage capability. Inspired by natural honeycomb structure, this work presents a one-step hydrothermal method of in situ growing Ni<ce:inf loc=\"post\">3</ce:inf>S<ce:inf loc=\"post\">2</ce:inf> nanosheet arrays on nickel foam (Ni foam), subsequently encapsulating polyethylene glycol (PEG) to fabricate multifunctional PCM composites. Benefiting from the honeycomb-like architectures and the hydrogen bonding interactions between Ni<ce:inf loc=\"post\">3</ce:inf>S<ce:inf loc=\"post\">2</ce:inf> nanosheets and PEG chains, the Ni@Ni<ce:inf loc=\"post\">3</ce:inf>S<ce:inf loc=\"post\">2</ce:inf>/PEG composite maintains excellent shape stability even after 8 h of intensive thermal cycling. Notably, the composite exhibits superior mechanical properties at both ambient temperature and above the melting point, with compressive strength enhanced by 430% to 780% compared to pristine PEG, alongside minimal leakage. Comprehensive analysis reveals that Ni<ce:inf loc=\"post\">3</ce:inf>S<ce:inf loc=\"post\">2</ce:inf> nanosheets serve as heterogeneous nucleation sites, effectively reducing the crystallization activation energy of PEG from 160.3 kJ/mol to 125.6 kJ/mol. Simultaneously, the geometric confinement effect of Ni<ce:inf loc=\"post\">3</ce:inf>S<ce:inf loc=\"post\">2</ce:inf> nanosheets guides the ordered arrangement of PEG chains and facilitates their rapid crystallization. Moreover, the composite successfully integrates magnetic-induced heating and photothermal conversion capabilities. Broadband light absorption (95.2%) is achieved by synergistically enhancing multiple scattering through a three-dimensional (3D) Ni foam porous structure integrated with Ni<ce:inf loc=\"post\">3</ce:inf>S<ce:inf loc=\"post\">2</ce:inf> nanosheet arrays. A constructed solar-powered electricity generation device achieves a sustained current output of 168.35 mA. This work provides a facile design strategy for realizing synergistic enhancement of encapsulation performance, thermal storage density, and photothermal conversion in porous foam-based PCMs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"13 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153165","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-10DOI: 10.1016/j.cej.2026.174039
Qiushi Chen, Xuzhong Gong, Junhao Liu, Zhi Wang
Micron silicon has long suffered from poor ion transport capability despite the potential as a reliable anode material for next-generation lithium-ion batteries. In this work, we present a novel strategy that leverages the inherent Al impurities in waste photovoltaic cell wafers to fabricate LiAlO₂-coated micron silicon anode via electrothermal shock process. The LiAlO₂ layer can effectively mitigate silicon's volume expansion through mechanical constraint, while the intense thermal gradient generated during electrothermal shock induces abundant oxygen vacancies in the coating, thereby facilitating rapid lithium-ion transport. The asymmetric bonding at the Si/LiAlO₂ interface, together with the work function difference between the two materials, enhances lithium-ion transport across the interface. Partially pre-lithiated silicon during the synthesis of LiAlO2 and stable SEI formation achieve a high ICE of 91%. Long-term cycling tests demonstrate a stable capacity over 2300 mAh g−1 after 300 cycles at 0.5 A g−1, with a retention of 92%, and impressive rate capability with over 750 mAh g−1 maintained after 1000 cycles at 5 A g−1. Full cell with μm-Si@LAO anode and commercial NCM811 cathode deliver an energy density of over 480 Wh kg−1 at 0.5C. This work presents a promising strategy for developing high-performance micron silicon anodes with enhanced lithium-ion transport properties.
尽管作为下一代锂离子电池可靠的负极材料，微米硅长期以来一直受到离子传输能力差的困扰。在这项工作中，我们提出了一种新的策略，利用废弃光伏电池晶片中固有的Al杂质，通过电热冲击工艺制造LiAlO 2涂层的微米硅阳极。LiAlO₂层可以通过机械约束有效地减缓硅的体积膨胀，而电热冲击过程中产生的强烈热梯度会在涂层中产生丰富的氧空位，从而促进锂离子的快速传输。Si/LiAlO 2界面上的不对称键合以及两种材料之间的功函数差异增强了锂离子在界面上的输运。在LiAlO2合成过程中，部分预锂化硅和稳定的SEI形成实现了91%的高ICE。长期骑自行车测试演示一个稳定的容量超过2300 mAh g−1 300年后 周期在0.5 g−1,保留92%,令人印象深刻的速度能力超过750 mAh g−1 1000年后保持 周期在5 g−1。具有μm-Si@LAO阳极和商用NCM811阴极的全电池在0.5℃下提供超过480 Wh kg−1的能量密度。这项工作为开发具有增强锂离子输运性能的高性能微米硅阳极提供了一个有前途的策略。
{"title":"Surface-engineered micron silicon for lithium-ion battery anode with enhanced ion transport","authors":"Qiushi Chen, Xuzhong Gong, Junhao Liu, Zhi Wang","doi":"10.1016/j.cej.2026.174039","DOIUrl":"https://doi.org/10.1016/j.cej.2026.174039","url":null,"abstract":"Micron silicon has long suffered from poor ion transport capability despite the potential as a reliable anode material for next-generation lithium-ion batteries. In this work, we present a novel strategy that leverages the inherent Al impurities in waste photovoltaic cell wafers to fabricate LiAlO₂-coated micron silicon anode via electrothermal shock process. The LiAlO₂ layer can effectively mitigate silicon's volume expansion through mechanical constraint, while the intense thermal gradient generated during electrothermal shock induces abundant oxygen vacancies in the coating, thereby facilitating rapid lithium-ion transport. The asymmetric bonding at the Si/LiAlO₂ interface, together with the work function difference between the two materials, enhances lithium-ion transport across the interface. Partially pre-lithiated silicon during the synthesis of LiAlO<ce:inf loc=\"post\">2</ce:inf> and stable SEI formation achieve a high ICE of 91%. Long-term cycling tests demonstrate a stable capacity over 2300 mAh g<ce:sup loc=\"post\">−1</ce:sup> after 300 cycles at 0.5 A g<ce:sup loc=\"post\">−1</ce:sup>, with a retention of 92%, and impressive rate capability with over 750 mAh g<ce:sup loc=\"post\">−1</ce:sup> maintained after 1000 cycles at 5 A g<ce:sup loc=\"post\">−1</ce:sup>. Full cell with μm-Si@LAO anode and commercial NCM811 cathode deliver an energy density of over 480 Wh kg<ce:sup loc=\"post\">−1</ce:sup> at 0.5C. This work presents a promising strategy for developing high-performance micron silicon anodes with enhanced lithium-ion transport properties.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"5 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153176","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-10DOI: 10.1016/j.cej.2026.174007
Fan Cheng, Xuefeng Zhang, Jialiang An, Xuecong Wang, Chuang Wang, Zhao Fang
Nonaqueous electrolytes represent a promising alternative to circumvent the inherent limitations of aqueous systems for zinc ion batteries (ZIBs), particularly under high-temperature environment, including dendrite growth, hydrogen evolution, and restricted voltage window. Herein, we strategically select a cyclic sulfone solvent characterized by its strong electron-donating ability and high dielectric constant to enhance salt dissociation and establish a weakly coordinated Zn2+ solvation environment. This rational electrolyte design promotes the formation of a double-gradient solid-electrolyte interphase rich in inorganic species, which in turn enables homogeneous Zn2+ plating/stripping, suppresses zinc dendrite formation, and extends the electrochemical stability window. As a result, Zn||Zn symmetrical cells achieve long-term cycling stability over 8000 h, while ZnǀǀCu asymmetric cells deliver an outstanding average Coulombic efficiency of 99.81% at 0.5 mA cm−2. When paired with a Mn2+-preintercalated vanadium oxide (MVO) cathode, the full cell exhibits remarkable cycling performance over 4000 cycles at 1.0 A g−1 and maintains stable operation across a wide temperature range from 25 °C to 80 °C. This work offers a promising path for developing nonaqueous electrolytes for high-performance ZIBs.
对于锌离子电池（zbs）来说，非水电解质是一种很有前途的替代方案，可以克服水系统固有的局限性，特别是在高温环境下，包括枝晶生长、析氢和受限的电压窗。为此，我们策略性地选择一种具有强给电子能力和高介电常数的环砜溶剂来促进盐解离，建立弱配位的Zn2+溶剂化环境。这种合理的电解质设计促进了富含无机物质的双梯度固-电解质界面的形成，从而实现了Zn2+的均匀镀/剥离，抑制了锌枝晶的形成，延长了电化学稳定窗口。因此，锌||锌对称电池在8000 h以上实现了长期循环稳定性，而ZnǀǀCu不对称电池在0.5 mA cm−2下提供了99.81%的平均库仑效率。当与Mn2+-预插层氧化钒（MVO）阴极配对时，整个电池在1.0 a g−1下表现出超过4000次 循环的卓越性能，并在25 °C至80 °C的宽温度范围内保持稳定运行。这项工作为开发高性能ZIBs的非水电解质提供了一条有前途的途径。
{"title":"Anion-enriched solvation chemistry toward long-life and high-temperature tolerant zinc batteries","authors":"Fan Cheng, Xuefeng Zhang, Jialiang An, Xuecong Wang, Chuang Wang, Zhao Fang","doi":"10.1016/j.cej.2026.174007","DOIUrl":"https://doi.org/10.1016/j.cej.2026.174007","url":null,"abstract":"Nonaqueous electrolytes represent a promising alternative to circumvent the inherent limitations of aqueous systems for zinc ion batteries (ZIBs), particularly under high-temperature environment, including dendrite growth, hydrogen evolution, and restricted voltage window. Herein, we strategically select a cyclic sulfone solvent characterized by its strong electron-donating ability and high dielectric constant to enhance salt dissociation and establish a weakly coordinated Zn<sup>2+</sup> solvation environment. This rational electrolyte design promotes the formation of a double-gradient solid-electrolyte interphase rich in inorganic species, which in turn enables homogeneous Zn<sup>2+</sup> plating/stripping, suppresses zinc dendrite formation, and extends the electrochemical stability window. As a result, Zn||Zn symmetrical cells achieve long-term cycling stability over 8000 h, while ZnǀǀCu asymmetric cells deliver an outstanding average Coulombic efficiency of 99.81% at 0.5 mA cm<sup>−2</sup>. When paired with a Mn<sup>2+</sup>-preintercalated vanadium oxide (MVO) cathode, the full cell exhibits remarkable cycling performance over 4000 cycles at 1.0 A g<sup>−1</sup> and maintains stable operation across a wide temperature range from 25 °C to 80 °C. This work offers a promising path for developing nonaqueous electrolytes for high-performance ZIBs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"5 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146145940","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-02-10DOI: 10.1016/j.cej.2026.174008
Subin Kim, Gwan Hyeon Park, Sangyeon Won, Jaehyun Heo, Taehun Kim, Sehun Choi, Jaehyeong Yu, Minguk Kwak, Jae Hyeong Park, Yunseo Lee, Won Bae Kim
Efficient lithium sulfide (Li2S) precipitation is crucial for high-performance lithium‑sulfur batteries (LSBs), especially under high-rate operation conditions. In this study, we introduce a cation-mixed high entropy spinel oxide (CM-HEO) as an effective catalyst to overcome the sluggish Li2S precipitation kinetics. The band gap narrowing, the coexistence of transition metal-oxygen (TM-O) bonds with varying degrees of covalency and emergence TM-O bonds with increased polarity were observed, together leading to the “cocktail effect”, which enhances its catalytic activity. Electrochemical tests in comparison with a physical mixture of low entropy oxides (PM-LEO) validated that this modulated electronic structure successfully promoted Li2S precipitation. The CM-HEO exhibited enhanced Li2S precipitation kinetics delivering a specific capacity of 512 mAh g−1 at 5C while the PM-LEO cathode only reached about 150 mAh g−1 due to its incomplete sulfur redox reaction. Furthermore, the CM-HEO cathode demonstrated excellent cycle stability over 1000 cycles with an average decay rate of 0.037% per cycle at 2C and delivered a remarkably high areal capacity of 3.93 mAh cm−2 during 50 cycles even under low electrolyte/sulfur ratio (E/S ratio) with high sulfur loading conditions. These results suggest that sulfur redox kinetics can be significantly enhanced by introducing well-engineered cation-mixed high entropy spinel oxides as cathode catalysts in the next generation LSBs.
高效的硫化锂（Li2S）沉淀对于高性能锂硫电池（LSBs）至关重要，特别是在高倍率运行条件下。在这项研究中，我们引入了一种阳离子混合高熵尖晶石氧化物（CM-HEO）作为克服Li2S沉淀动力学缓慢的有效催化剂。带隙缩小，不同共价程度的过渡金属-氧（TM-O）键和极性增加的涌现TM-O键共存，形成“鸡尾酒效应”，增强了其催化活性。与物理混合的低熵氧化物（PM-LEO）相比，电化学测试验证了这种调制的电子结构成功地促进了Li2S的沉淀。CM-HEO表现出增强的Li2S沉淀动力学，在5C时的比容量为512 mAh g−1，而PM-LEO阴极由于硫氧化还原反应不完全，仅达到约150 mAh g−1。此外，cm - heo阴极在1000次 循环中表现出优异的循环稳定性，在2C下每个循环的平均衰减率为0.037%，即使在低电解质/硫比（E/S比）和高硫负载条件下，在50次 循环中也能提供3.93 mAh cm - 2的显着高面积容量。这些结果表明，在下一代lsb中引入精心设计的阳离子混合高熵尖晶石氧化物作为阴极催化剂，可以显著增强硫的氧化还原动力学。
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