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Robust CVD polymer encapsulation for thermally and chemically resistant fluorescent sensor nanoprobes 坚固的CVD聚合物封装,用于耐热和耐化学腐蚀的荧光传感器纳米探针
IF 4.7 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-02-06 DOI: 10.1016/j.ces.2026.123554
Merve Karabıyık, Gizem Cihanoğlu, Özgenç Ebil
Semiconductor quantum dots (QDs) are attractive fluorophores for sensor applications due to their narrow emission bandwidths and high photostability; however, their performance is often limited by insufficient chemical and thermal durability under operating conditions. In this study, a solvent-free encapsulation strategy based on initiated chemical vapor deposition (iCVD) is proposed to enhance the stability of QD-based sensor nanoprobes. Cross-linked poly (glycidyl methacrylate-co-ethylene glycol dimethacrylate) (ECOP) thin films were conformally deposited as encapsulation layers onto CdTe QD-functionalized poly(GMA) sensor surfaces. The encapsulated nanoprobes were evaluated under chemically aggressive environments (water, saltwater, toluene, and sulfuric acid) and elevated temperatures. Following exposure to aggressive solvents, both the polymer film thickness variation and QD fluorescence intensity change remained below 10 %, confirming the robustness of the cross-linked network. Also, thermal durability tests showed stable fluorescence performance after annealing at 250 °C, with structural and optical changes remaining within the accepted 10 % threshold. The results demonstrate that coatings deposited using iCVD exhibit conformal coverage and enhanced stability. This enables reliable protection of QD-based sensor nanoprobes without compromising optical performance. This study presents a promising method to extend the operational lifetime and environmental durability of QD-integrated sensor platforms by using chemically and thermally stable polymer encapsulation.
半导体量子点(QDs)由于其狭窄的发射带宽和光稳定性而成为传感器应用中有吸引力的荧光团;然而,在操作条件下,它们的性能往往受到化学和热耐久性不足的限制。本研究提出了一种基于引发化学气相沉积(iCVD)的无溶剂封装策略,以提高量子点传感器纳米探针的稳定性。将交联聚(甲基丙烯酸甘油酯-共乙二醇二甲基丙烯酸酯)(ECOP)薄膜作为包封层共形沉积在CdTe量子点功能化聚(GMA)传感器表面。在化学腐蚀性环境(水、盐水、甲苯和硫酸)和高温下对包封的纳米探针进行了评估。暴露于腐蚀性溶剂后,聚合物膜厚度变化和QD荧光强度变化均保持在10 %以下,证实了交联网络的鲁棒性。此外,热耐久性测试显示,在250 °C退火后,荧光性能稳定,结构和光学变化保持在可接受的10 %阈值内。结果表明,用iCVD沉积的涂层具有保形覆盖和增强的稳定性。这可以在不影响光学性能的情况下可靠地保护基于量子点的传感器纳米探针。本研究提出了一种有前途的方法,通过使用化学和热稳定的聚合物封装来延长量子点集成传感器平台的使用寿命和环境耐久性。
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引用次数: 0
Investigation of drying characteristics and evaluation strategy for wet coating in the manufacturing process of battery electrode 电池电极制造过程中湿涂层干燥特性及评价策略研究
IF 4.7 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-02-06 DOI: 10.1016/j.ces.2026.123541
Jiajun Wang, Yue Zeng, Hongqiang Ma, Huilun Kang, Jing Wu, Xuefeng Wu, Ruixiang Ding, Yujin Zhang, Weihua Cai
A multi-field coupling model of wet coating is proposed in the production process of battery electrode based on parallel and dynamic mesh methods. Its heat-mass transfer among wet coating, substrate and hot wind are considered in this model, and it is proved reliable because its errors are within ±15%. Through this model, the variations and distribution of drying characteristics of wet coating are studied with different design conditions. It can be found that the temperature, saturated vapor pressure, diffusion coefficient and moisture rate of wet coating are most significantly influenced by motion velocity. Liquid film thickness is most significantly influenced by thickness. Drying rate is subjected to the combined influences of mass transfer coefficient, saturated vapor pressure difference and initial moisture content, and its variation trend is different. The drying uniformity and moisture rate correlations of wet coating are proposed for comprehensive consideration of thickness, water saturation and motion velocity based on nonlinear regression method. And it can be found that they are proved reliable because the errors between simulation and calculation data are less than 14.55% and 10%, respectively. Finally, the evaluation strategy of drying characteristics is further obtained for wet coating.
基于并行网格法和动态网格法,建立了电池电极生产过程中湿涂膜的多场耦合模型。该模型考虑了湿涂层、基材和热风之间的热质传递,误差在±15%以内,证明了模型的可靠性。通过该模型,研究了不同设计条件下湿涂层干燥特性的变化和分布。结果表明,运动速度对湿涂层的温度、饱和蒸汽压、扩散系数和含水率的影响最为显著。液膜厚度受厚度的影响最为显著。干燥速率受传质系数、饱和蒸汽压差和初始含水率的综合影响,其变化趋势不同。基于非线性回归方法,综合考虑涂层厚度、含水饱和度和运动速度等因素,提出了湿涂层的干燥均匀性和含水率相关性。仿真与计算数据的误差分别小于14.55%和10%,证明了它们的可靠性。最后,进一步得出了湿涂膜干燥特性的评价策略。
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引用次数: 0
Constructing atomic-scale electric fields in nitrogen-doped FeS2 as intrinsic ion accelerators for sodium-ion batteries 氮掺杂FeS2作为钠离子电池本征离子加速器的原子尺度电场构建
IF 4.7 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-02-06 DOI: 10.1016/j.ces.2026.123522
Luchao Yue, Yifan Dou, Lin Jiang, Sidan Peng, Ran Zhang, Bin Li, Jiahui Zhao, Yu Feng, Lixin Zhang, Ruina Shi, Imran Shakir, Wei Song, Guisheng Qi, Xuping Sun
Transition metal sulfides are highly attractive anodes for large-scale sodium ion batteries owing to their high theoretical capacity. However, their practical application is severely bottlenecked by sluggish sodiation kinetics, a fundamental limitation rooted in their inherently poor electronic/ionic conductivity. Herein, we present a strategy to engineer atomic-scale electric fields within FeS2 via nitrogen (N) doping, aiming to fundamentally accelerate Na+ transport as intrinsic ion accelerators. Theoretical calculations indicate that N incorporation induces charge redistribution, creating localized built-in electric fields that facilitate Na+ adsorption and reduce Na+ diffusion barriers within FeS2. Consequently, the N-FeS2@NC with optimal N doping content exhibits a high sodium storage capacity of 545 mAh g−1 at 1.0 A g−1 over 100 cycles. Even at 10.0 A g−1, it maintains a capacity of 354 mAh g−1 with outstanding long-term cyclability (205 mAh g −1 after 4000 cycles). This work establishes engineering atomic-scale electric fields for intrinsically enhancing ion kinetics, offering a versatile and powerful pathway for designing next-generation, ultra-fast energy storage materials.
过渡金属硫化物具有较高的理论容量,是大型钠离子电池极具吸引力的阳极。然而,它们的实际应用受到缓慢的钠化动力学的严重瓶颈,这是其固有的电子/离子导电性差的根本限制。在此,我们提出了一种通过氮(N)掺杂在FeS2中设计原子尺度电场的策略,旨在从根本上加速Na+作为本征离子加速器的输运。理论计算表明,N的掺入诱导电荷重新分布,产生局域内嵌电场,促进Na+吸附并降低Na+在FeS2内的扩散障碍。因此,在1.0 ag−1下,具有最佳N掺杂含量的N-FeS2@NC在100次循环中具有545 mAh g−1的高钠存储容量。即使在10.0 A g−1下,它也能保持354 mAh g−1的容量,并具有出色的长期可循环性(4000次循环后可达到205 mAh g−1)。这项工作建立了工程原子尺度电场,从本质上增强了离子动力学,为设计下一代超快速储能材料提供了一个多功能和强大的途径。
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引用次数: 0
Towards a deeper understanding of the oxidation of isobutane to tert-butyl hydroperoxide in the liquid phase by an extended kinetic model. Initiation by di-tert-butyl peroxide 用扩展动力学模型对液相中异丁烷氧化生成过氧化叔丁基的过程有了更深入的了解。过氧化二叔丁基引发
IF 4.7 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-02-06 DOI: 10.1016/j.ces.2026.123523
Thomas Willms, Holger Kryk, Uwe Hampel
To date, the liquid phase oxidation of isobutane has not been comprehensively described in the literature, since the established kinetic models include either the effect of the initiator or the autocatalytic nature of the oxidation of isobutane, but not both. To overcome this deficiency, an extended kinetic model was developed and validated using experimental data from the literature. It enabled for the first time the distinction of three different processes: the oxidation of isobutane, the heterogeneous, unimolecular decomposition of tert-butyl hydroperoxide on the reactor wall and the homogeneous decomposition reactions of TBHP in solution. The rate constant of the heterogeneous unimolecular decomposition of TBHP on the wall surface of an untreated stainless-steel reactor, was found to be two to five times higher than that which was observed in a passivated steel reactor. However, similar values for the respective parameters describing the first-order decomposition of TBHP and the oxidation of isobutane were obtained in both reactors. In the non-passivated stainless-steel reactor, the second order decomposition of TBHP was absent. The results were compared with published data.
迄今为止,文献中尚未对异丁烷的液相氧化进行全面的描述,因为建立的动力学模型要么包括引发剂的作用,要么包括异丁烷氧化的自催化性质,而不是两者兼而有之。为了克服这一缺陷,开发了一个扩展的动力学模型,并使用文献中的实验数据进行了验证。它第一次区分了三种不同的过程:异丁烷的氧化、过氧化叔丁基在反应器壁上的非均相、单分子分解和三必和二必酸在溶液中的均相分解反应。在未经处理的不锈钢反应器壁面上,发现三氧化二硼的非均相单分子分解速率常数比在钝化钢反应器中观察到的速率常数高2至5倍。然而,在两个反应器中,描述三必和二必和三必和二必的一级分解和异丁烷氧化的相应参数的值相似。在未钝化的不锈钢反应器中,不存在TBHP的二级分解。研究结果与已发表的数据进行了比较。
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引用次数: 0
Low-concentration CO2 adsorption performance of MCM-41 molecular sieve doped with heterometals inherent in fly ash 掺粉煤灰异质金属的MCM-41分子筛低浓度CO2吸附性能研究
IF 4.7 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-02-05 DOI: 10.1016/j.ces.2026.123503
Kong Haowen, Wu Hong, Zhang Li, Wang Ping, Li Ruimeng
This study investigated the utilization of heterometals, such as Al, Fe, and Ti, inherent in fly ash in the synthesis of metal-doped MCM-41 molecular sieve for the efficient capture of low-concentration carbon dioxide (CO2). While active Si and Al components were extracted by an acid leaching-alkali fusion pretreatment process, the adsorbent was prepared using an in situ doping method, resulting in metal-doped MCM-41 with small grain sizes and ordered mesoporous channels. The distribution of metal heteroatoms was optimized by adjusting the synthesis pH. Al atoms were concentrated on the surface of the molecular sieve to form active sites, while Fe and Ti atoms were preferably incorporated into the bulk phase to regulate the pore structure. C10.5-M41, synthesized at pH 10.5, exhibited abundant surface acid-base sites and an increased pore size of 5.4 nm. In low-concentration CO2 adsorption tests, the material demonstrated adsorption capacities of 1.31 mmol/g at 25 °C and 1.06 mmol/g at 90 ℃. The adsorption capacity decreased by 38% at 90℃ with 8% water vapor. In addition, 90% of the adsorption capacity at 25 ℃ could be retained after ten regeneration cycles. Based on thermodynamic analysis, physical adsorption dominates at 25 ℃, while chemical adsorption is predominant at 90 ℃. The incorporation of metal ions into the framework increases the pore size of the adsorbent and reduces its internal transport resistance for CO2 gas. This study utilized heterometals inherent in fly ash as a resource and contributed to the design of high-capacity and thermally stable CO2 adsorbent materials.
本研究探讨了利用粉煤灰中固有的Al、Fe、Ti等异质金属合成掺杂金属的MCM-41分子筛,高效捕集低浓度二氧化碳(CO2)。采用酸浸-碱融合预处理工艺提取活性Si和Al组分,采用原位掺杂法制备吸附剂,制备出粒径小、介孔通道有序的金属掺杂MCM-41。通过调节合成ph来优化金属杂原子的分布,Al原子集中在分子筛表面形成活性位点,而Fe和Ti原子则优选掺入体相来调节孔结构。在pH 10.5下合成的C10.5-M41具有丰富的表面酸碱位点,孔径增大到5.4 nm。在低浓度CO2吸附试验中,材料在25 ℃时的吸附量为1.31 mmol/g,在90 ℃时的吸附量为1.06 mmol/g。当温度为90℃,水蒸气含量为8%时,吸附量下降38%。在25 ℃条件下,经过10次再生后,吸附量仍可保持90%。热力学分析表明,25 ℃时以物理吸附为主,90 ℃时以化学吸附为主。金属离子加入到框架中增加了吸附剂的孔径,降低了其对CO2气体的内部输送阻力。本研究利用粉煤灰中固有的异质金属作为资源,为设计高容量、热稳定的CO2吸附剂材料做出了贡献。
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引用次数: 0
Unique synergies of Ce and Nb doping on Cu-SSZ-13 resulting in excellent stability over a significantly wider temperature range Ce和Nb掺杂在Cu-SSZ-13上的独特协同作用使得Cu-SSZ-13在更宽的温度范围内具有优异的稳定性
IF 4.7 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-02-05 DOI: 10.1016/j.ces.2026.123531
Jingang Wang, Jianbo Zhang, Yuzhe Mu, Xuejiao Tang
Cu-SSZ-13 catalysts have emerged as the most promising on-board catalysts in denitrification with NH3-SCR due to the exceptional hydrothermal stability and catalytic activity. In the work, as-prepared Ce0.075-Nb1.5%/Cu-SSZ-13 catalyst exhibited a significantly most excellent catalytic activity with good stability in the wider temperature range of 300 ℃ to 650 ℃, due to the synergistic effect of Ce and Nb. The results of XPS and H2-TPR indicated that the interaction between Ce and Nb alters the chemical environment of the active site Cu, resulting in a more stable Cusingle bondO bond, which enhances the stability of the active Cu sites, which was verified by the analysis results of Materials Studio. The addition of Nb could lead to the increase of Ce3+/Ce4+ to improve the redox capacity of the catalyst. Moreover, the synergistic effect of Nb and Ce made few CuOx clusters formed and preserved a greater number of [Cu(OH)]+, which was impeded to migrate at high temperatures due to the steric hindrance formed by Nb and Ce, enhancing the catalytic activity at wider temperature range.
Cu-SSZ-13催化剂因其优异的水热稳定性和催化活性而成为最有前途的车载NH3-SCR脱硝催化剂。在本研究中,由于Ce和Nb的协同作用,制备的Ce0.075-Nb1.5%/Cu-SSZ-13催化剂在300 ~ 650℃的较宽温度范围内表现出最优异的催化活性和良好的稳定性。XPS和H2-TPR结果表明,Ce和Nb之间的相互作用改变了活性位点Cu的化学环境,导致CuO键更加稳定,从而增强了活性位点Cu的稳定性,这一点得到了Materials Studio分析结果的验证。Nb的加入会导致Ce3+/Ce4+的增加,从而提高催化剂的氧化还原能力。此外,Nb和Ce的协同作用使得形成的CuOx簇较少,保留了大量的[Cu(OH)]+,由于Nb和Ce形成的位阻阻碍了[Cu(OH)]+在高温下的迁移,提高了在更宽温度范围内的催化活性。
{"title":"Unique synergies of Ce and Nb doping on Cu-SSZ-13 resulting in excellent stability over a significantly wider temperature range","authors":"Jingang Wang, Jianbo Zhang, Yuzhe Mu, Xuejiao Tang","doi":"10.1016/j.ces.2026.123531","DOIUrl":"https://doi.org/10.1016/j.ces.2026.123531","url":null,"abstract":"Cu-SSZ-13 catalysts have emerged as the most promising on-board catalysts in denitrification with NH<sub>3</sub>-SCR due to the exceptional hydrothermal stability and catalytic activity. In the work, as-prepared Ce<sub>0.075</sub>-Nb<sub>1.5%</sub>/Cu-SSZ-13 catalyst exhibited a significantly most excellent catalytic activity with good stability in the wider temperature range of 300 ℃ to 650 ℃, due to the synergistic effect of Ce and Nb. The results of XPS and H<sub>2</sub>-TPR indicated that the interaction between Ce and Nb alters the chemical environment of the active site Cu, resulting in a more stable Cu<img alt=\"single bond\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/sbnd.gif\" style=\"vertical-align:middle\"/>O bond, which enhances the stability of the active Cu sites, which was verified by the analysis results of Materials Studio. The addition of Nb could lead to the increase of Ce<sup>3+</sup>/Ce<sup>4+</sup> to improve the redox capacity of the catalyst. Moreover, the synergistic effect of Nb and Ce made few CuO<sub>x</sub> clusters formed and preserved a greater number of [Cu(OH)]<sup>+</sup>, which was impeded to migrate at high temperatures due to the steric hindrance formed by Nb and Ce, enhancing the catalytic activity at wider temperature range.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"42 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2026-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116033","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
D-alanine-bridged phosphotungstic acid/UiO-66 hybrids as efficient catalysts for oxidative desulfurization of fuels d -丙氨酸桥接磷钨酸/UiO-66杂化物作为燃料氧化脱硫的高效催化剂
IF 4.7 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-02-05 DOI: 10.1016/j.ces.2026.123545
Mengying Lin, Hanyue Lou, Zhaoyang Qi, Jie Chen, Changshen Ye, Ting Qiu
The development of highly active catalysts is crucial for oxidative desulfurization (ODS) to meet the growing demand for sulfur-free fuels. In this study, a defect-rich composite catalyst UiO-DAlaPW was successfully synthesized via mechanochemical grinding, wherein phosphotungstic acid (HPW) was encapsulated within a defect-engineered UiO-66 framework, utilizing D-alanine (DAla) as a bridging molecule. The synthesized catalyst, UiO-DAlaPW, significantly enhances the utilization efficiency of hydrogen peroxide (H2O2). In the model oil ODS system, the material exhibited exceptional catalytic performance: achieving deep desulfurization at room temperature within merely 5 min under conditions of extremely low acetonitrile cosolvent usage and a low oxidant/sulfur (O/S) ratio, accompanied by remarkably high H2O2 utilization efficiency. Moreover, the catalyst maintained high desulfurization efficiency even in the absence of acetonitrile. Characterization by XRD, FT-IR, TGA, and XPS confirmed the successful encapsulation of HPW within the UiO-66 framework. Mechanistic studies revealed a significant synergistic effect between UiO-66 and HPW. The effective cooperation of the two active sites, namely Zr in UiO-66 and PW, significantly enhances the catalytic performance, contributing to superior oxidative desulfurization activity.
开发高活性催化剂是氧化脱硫(ODS)技术满足日益增长的无硫燃料需求的关键。在本研究中,通过机械化学研磨成功合成了一种富含缺陷的复合催化剂UiO-DAlaPW,其中磷钨酸(HPW)被封装在缺陷工程的UiO-66框架中,利用d -丙氨酸(DAla)作为桥接分子。合成的UiO-DAlaPW催化剂显著提高了过氧化氢(H2O2)的利用效率。在模型油ODS系统中,该材料表现出优异的催化性能:在极低的乙腈助溶剂用量和低的氧化剂/硫(O/S)比的条件下,在室温下仅5 min即可实现深度脱硫,并具有非常高的H2O2利用率。此外,即使在没有乙腈的情况下,催化剂也能保持较高的脱硫效率。通过XRD, FT-IR, TGA和XPS的表征证实了HPW在UiO-66框架内的成功封装。机制研究表明UiO-66与HPW之间存在显著的协同效应。UiO-66和PW中Zr两个活性位点的有效配合,显著提高了催化性能,具有优异的氧化脱硫活性。
{"title":"D-alanine-bridged phosphotungstic acid/UiO-66 hybrids as efficient catalysts for oxidative desulfurization of fuels","authors":"Mengying Lin, Hanyue Lou, Zhaoyang Qi, Jie Chen, Changshen Ye, Ting Qiu","doi":"10.1016/j.ces.2026.123545","DOIUrl":"https://doi.org/10.1016/j.ces.2026.123545","url":null,"abstract":"The development of highly active catalysts is crucial for oxidative desulfurization (ODS) to meet the growing demand for sulfur-free fuels. In this study, a defect-rich composite catalyst UiO-DAlaPW was successfully synthesized via mechanochemical grinding, wherein phosphotungstic acid (HPW) was encapsulated within a defect-engineered UiO-66 framework, utilizing D-alanine (DAla) as a bridging molecule. The synthesized catalyst, UiO-DAlaPW, significantly enhances the utilization efficiency of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>). In the model oil ODS system, the material exhibited exceptional catalytic performance: achieving deep desulfurization at room temperature within merely 5 min under conditions of extremely low acetonitrile cosolvent usage and a low oxidant/sulfur (O/S) ratio, accompanied by remarkably high H<sub>2</sub>O<sub>2</sub> utilization efficiency. Moreover, the catalyst maintained high desulfurization efficiency even in the absence of acetonitrile. Characterization by XRD, FT-IR, TGA, and XPS confirmed the successful encapsulation of HPW within the UiO-66 framework. Mechanistic studies revealed a significant synergistic effect between UiO-66 and HPW. The effective cooperation of the two active sites, namely Zr in UiO-66 and PW, significantly enhances the catalytic performance, contributing to superior oxidative desulfurization activity.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"70 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2026-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122517","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Dual functional Li4[Fe(CN)6] modified PVDF-HFP membrane: An effective gel polymer solid electrolyte for solid-state lithium batteries 双功能Li4[Fe(CN)6]改性PVDF-HFP膜:固态锂电池的有效凝胶聚合物固体电解质
IF 4.7 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-02-05 DOI: 10.1016/j.ces.2026.123455
Jing Wang, Xiangbo Feng, Yuzhen Zhao, Du Lv, Hao Ma, Manni Li, Yao Liu, Guoqing Guan, Jian Miao
Solid electrolyte is an effective way to address the safety concerns associated with liquid electrolytes based-rechargeable Li-ion batteries (LIBs), making the improvement of their electrochemical performance particularly significant. In this work, a poly(vinylidene fluoride-hexafluoro propylene) (PVDF-HFP) membrane was successfully modified with lithium hexacyanoferrate(II) (Li4[Fe(CN)6]), the resulting bonding interactions enabled the formation of a gel polymer electrolyte (GPE) with high ionic conductivity, making it highly suitable for applications in SSLBs applications. Impressively, the obtained GPE with a three-dimensional (3D) porous network exhibited a wide electrochemical window of ∼5.0 V, a high lithium transference number of 0.42, and an enhanced ionic conductivity of 2.63 × 10-4 S·cm−1. These improvements can be attributed to the dual functional Li4[Fe(CN)6], which not only serves as a lithium ion source but also effectively reduces the crystallization of PVDF-HFP. Additionally, the assembled SSLB with this GPE exhibited excellent cycling stability, achieving a high initial capacity of 119.1 mAh·g−1 and a high initial Coulombic efficiency of 97.24% at 1C. This PVDF-HFP-Li4[Fe(CN)6] GPE is therefore expected to be an effective electrolyte for next-generation SSLBs with high cycling stability.
固体电解质是解决液态电解质可充电锂离子电池(LIBs)安全问题的有效途径,使得其电化学性能的改善尤为重要。在这项工作中,用六氰高铁酸锂(II) (Li4[Fe(CN)6])成功地修饰了聚偏氟乙烯-六氟丙烯(PVDF-HFP)膜,所产生的键相互作用使凝胶聚合物电解质(GPE)的形成具有高离子电导率,使其非常适合sslb应用。令人印象深刻的是,获得的具有三维(3D)多孔网络的GPE具有~ 5.0 V的宽电化学窗口,0.42的高锂转移数和2.63 × 10-4 S·cm−1的离子电导率增强。这些改进可归因于双官能团Li4[Fe(CN)6],它不仅作为锂离子源,而且有效地减少了PVDF-HFP的结晶。此外,用该GPE组装的SSLB具有优异的循环稳定性,在1C下达到119.1 mAh·g−1的高初始容量和97.24%的高初始库仑效率。因此,这种PVDF-HFP-Li4[Fe(CN)6] GPE有望成为具有高循环稳定性的下一代sslb的有效电解质。
{"title":"Dual functional Li4[Fe(CN)6] modified PVDF-HFP membrane: An effective gel polymer solid electrolyte for solid-state lithium batteries","authors":"Jing Wang, Xiangbo Feng, Yuzhen Zhao, Du Lv, Hao Ma, Manni Li, Yao Liu, Guoqing Guan, Jian Miao","doi":"10.1016/j.ces.2026.123455","DOIUrl":"https://doi.org/10.1016/j.ces.2026.123455","url":null,"abstract":"Solid electrolyte is an effective way to address the safety concerns associated with liquid electrolytes based-rechargeable Li-ion batteries (LIBs), making the improvement of their electrochemical performance particularly significant. In this work, a poly(vinylidene fluoride-hexafluoro propylene) (PVDF-HFP) membrane was successfully modified with lithium hexacyanoferrate(II) (Li<sub>4</sub>[Fe(CN)<sub>6</sub>]), the resulting bonding interactions enabled the formation of a gel polymer electrolyte (GPE) with high ionic conductivity, making it highly suitable for applications in SSLBs applications. Impressively, the obtained GPE with a three-dimensional (3D) porous network exhibited a wide electrochemical window of ∼5.0 V, a high lithium transference number of 0.42, and an enhanced ionic conductivity of 2.63 × 10<sup>-4</sup> S·cm<sup>−1</sup>. These improvements can be attributed to the dual functional Li<sub>4</sub>[Fe(CN)<sub>6</sub>], which not only serves as a lithium ion source but also effectively reduces the crystallization of PVDF-HFP. Additionally, the assembled SSLB with this GPE exhibited excellent cycling stability, achieving a high initial capacity of 119.1 mAh·g<sup>−1</sup> and a high initial Coulombic efficiency of 97.24% at 1C. This PVDF-HFP-Li<sub>4</sub>[Fe(CN)<sub>6</sub>] GPE is therefore expected to be an effective electrolyte for next-generation SSLBs with high cycling stability.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"63 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2026-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146135363","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Pd/SSZ-39 low-temperature hydrocarbon traps: probing adsorption mechanisms and hydrothermal aging impacts Pd/SSZ-39低温油气圈闭:探测吸附机理及热液老化影响
IF 4.7 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-02-05 DOI: 10.1016/j.ces.2026.123547
Jinhuang Cai, Chaofan Qi, Dingding Liu, Guohua Jing, Yongdan Li, Huawang Zhao
Hydrocarbons (HCs) emission during the cold-start period of internal combustion engine vehicles accounts for the majority of total HCs emission. In this work, we developed a Pd/SSZ-39 catalyst with exceptional low-temperature C3H6 (representative of light HCs) trapping performance, achieving the C3H6 storage capacity of 0.87 mmol/g (C3H6/Pd2+=12). The C3H6 adsorption tests revealed that aged Pd/SSZ-39 samples retained 47% and 28% of its original C3H6 trapping capacity after treatment at 800 °C and 900 °C for 20 h, respectively, while its C3H6 oxidation efficiency remained largely unaffected. Characterization studies indicate that Pd2+ ions serve as primary adsorption sites, initially capturing C3H6 molecules as Pd2+(C3H6)x, which then undergo cracking and polymerization at neighboring Brønsted acid sites. The reduction in both Pd2+ ions and Brønsted acid sites directly correlates with the diminished C3H6 adsorption capacity. During the desorption phase, Pd2+(C3H6)x species decompose between 200–300 °C, while polymerized hydrocarbons undergo oxidation at 300–400 °C, yielding distinct C3H6 and CO2/CO release peaks. These findings highlight the Pd/SSZ-39 as a robust low-temperature hydrocarbon trap, even under extreme hydrothermal aging conditions.
内燃机汽车冷启动阶段的碳氢化合物(hc)排放量占总排放量的大部分。在这项工作中,我们开发了一种具有优异低温C3H6(轻hc的代表)捕获性能的Pd/SSZ-39催化剂,实现了C3H6的存储容量为0.87 mmol/g (C3H6/Pd2+=12)。老化Pd/SSZ-39样品在800 °C和900 °C下处理20 h后,C3H6吸附量分别保持47%和28%,而C3H6氧化效率基本未受影响。表征研究表明,Pd2+离子作为主要吸附位点,最初以Pd2+(C3H6)x的形式捕获C3H6分子,然后在邻近的br / nsted酸位点发生裂解和聚合。Pd2+离子和Brønsted酸位的减少与C3H6吸附能力的降低直接相关。在解吸阶段,Pd2+(C3H6)x在200-300 °C之间分解,而聚合烃在300-400 °C发生氧化,产生明显的C3H6和CO2/CO释放峰。这些发现强调了Pd/SSZ-39是一个强大的低温油气圈闭,即使在极端热液老化条件下也是如此。
{"title":"Pd/SSZ-39 low-temperature hydrocarbon traps: probing adsorption mechanisms and hydrothermal aging impacts","authors":"Jinhuang Cai, Chaofan Qi, Dingding Liu, Guohua Jing, Yongdan Li, Huawang Zhao","doi":"10.1016/j.ces.2026.123547","DOIUrl":"https://doi.org/10.1016/j.ces.2026.123547","url":null,"abstract":"Hydrocarbons (HCs) emission during the cold-start period of internal combustion engine vehicles accounts for the majority of total HCs emission. In this work, we developed a Pd/SSZ-39 catalyst with exceptional low-temperature C<sub>3</sub>H<sub>6</sub> (representative of light HCs) trapping performance, achieving the C<sub>3</sub>H<sub>6</sub> storage capacity of 0.87 mmol/g (C<sub>3</sub>H<sub>6</sub>/Pd<sup>2+</sup>=12). The C<sub>3</sub>H<sub>6</sub> adsorption tests revealed that aged Pd/SSZ-39 samples retained 47% and 28% of its original C<sub>3</sub>H<sub>6</sub> trapping capacity after treatment at 800 °C and 900 °C for 20 h, respectively, while its C<sub>3</sub>H<sub>6</sub> oxidation efficiency remained largely unaffected. Characterization studies indicate that Pd<sup>2+</sup> ions serve as primary adsorption sites, initially capturing C<sub>3</sub>H<sub>6</sub> molecules as Pd<sup>2+</sup>(C<sub>3</sub>H<sub>6</sub>)<sub>x</sub>, which then undergo cracking and polymerization at neighboring Brønsted acid sites. The reduction in both Pd<sup>2+</sup> ions and Brønsted acid sites directly correlates with the diminished C<sub>3</sub>H<sub>6</sub> adsorption capacity. During the desorption phase, Pd<sup>2+</sup>(C<sub>3</sub>H<sub>6</sub>)<sub>x</sub> species decompose between 200–300 °C, while polymerized hydrocarbons undergo oxidation at 300–400 °C, yielding distinct C<sub>3</sub>H<sub>6</sub> and CO<sub>2</sub>/CO release peaks. These findings highlight the Pd/SSZ-39 as a robust low-temperature hydrocarbon trap, even under extreme hydrothermal aging conditions.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"47 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2026-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146121907","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Effect of wide-range operating pressure on O2 production by CO2 conversion in a gliding arc reactor 大范围操作压力对滑动弧反应器CO2转化产氧的影响
IF 4.7 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-02-05 DOI: 10.1016/j.ces.2026.123532
Dingchen Li, Yang Liu, Xiangen Zhao, Jingjie Ye, Chuanlong Ma, Chuan Li, Enhao Wei, Menghan Xiao, Yaping Du
Efficient O2 recovery from CO2 is a critical technology for closed-loop life support systems in aerospace, submarine environments, and future extraterrestrial exploration. Gliding arc (GA) plasma-assisted CO2 conversion offers high chemical activity and low implementation cost. Here, we developed a GA reactor operating from 7 to 760 Torr to study the effect of pressure and matching power on O2 yield by CO2 conversion. The results show that O2 yield first rises then falls with the operating pressure, and its optimal pressure shifts higher as power increases. Synchronized electrical signals, direct optical images and spatial distribution of atomic oxygen of discharge-patterns (glow → transition → GA) is used to analyze the reasons for changes in O2 yield with pressure. Notably, the reactor achieved an oxygen production rate of 6 g/hr at 400 Torr and 210 W, comparable to state-of-the-art solid oxide electrolysis systems (e.g., MOXIE). These findings provide essential physical insights for optimizing plasma-based O2 generation in variable-pressure environments, ranging from high-altitude flight to in-situ resource utilization.
从CO2中高效回收O2是航空航天、海底环境和未来地外探索中闭环生命支持系统的关键技术。滑翔弧(GA)等离子体辅助CO2转化具有高化学活性和低实施成本的优点。在此,我们开发了一个运行在7 - 760 Torr的GA反应器,以研究压力和匹配功率对CO2转化O2产率的影响。结果表明:O2产率随操作压力的增大先升后降,其最优压力随功率的增大而增大;利用同步电信号、直接光学图像和放电模式(发光 → 跃迁 → GA)原子氧的空间分布,分析了O2产率随压力变化的原因。值得注意的是,反应器在400 Torr和210 W下的产氧速率为6 g/hr,可与最先进的固体氧化物电解系统(例如MOXIE)相媲美。这些发现为在变压环境下优化基于血浆的氧气生成提供了重要的物理见解,范围从高空飞行到原位资源利用。
{"title":"Effect of wide-range operating pressure on O2 production by CO2 conversion in a gliding arc reactor","authors":"Dingchen Li, Yang Liu, Xiangen Zhao, Jingjie Ye, Chuanlong Ma, Chuan Li, Enhao Wei, Menghan Xiao, Yaping Du","doi":"10.1016/j.ces.2026.123532","DOIUrl":"https://doi.org/10.1016/j.ces.2026.123532","url":null,"abstract":"Efficient O<sub>2</sub> recovery from CO<sub>2</sub> is a critical technology for closed-loop life support systems in aerospace, submarine environments, and future extraterrestrial exploration. Gliding arc (GA) plasma-assisted CO<sub>2</sub> conversion offers high chemical activity and low implementation cost. Here, we developed a GA reactor operating from 7 to 760 Torr to study the effect of pressure and matching power on O<sub>2</sub> yield by CO<sub>2</sub> conversion. The results show that O<sub>2</sub> yield first rises then falls with the operating pressure, and its optimal pressure shifts higher as power increases. Synchronized electrical signals, direct optical images and spatial distribution of atomic oxygen of discharge-patterns (glow → transition → GA) is used to analyze the reasons for changes in O<sub>2</sub> yield with pressure. Notably, the reactor achieved an oxygen production rate of 6 g/hr at 400 Torr and 210 W, comparable to state-of-the-art solid oxide electrolysis systems (e.g., MOXIE). These findings provide essential physical insights for optimizing plasma-based O<sub>2</sub> generation in variable-pressure environments, ranging from high-altitude flight to in-situ resource utilization.","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"1 1","pages":""},"PeriodicalIF":4.7,"publicationDate":"2026-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116034","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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Chemical Engineering Science
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