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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 4.3 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-05-15 Epub 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 CuO 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。
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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 4.3 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-05-15 Epub 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。
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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 4.3 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-05-15 Epub 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。
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引用次数: 0
Unraveling the molecular mechanism of solid–liquid phase equilibrium of DBD in different solvents 揭示了DBD在不同溶剂中固液平衡的分子机理
IF 4.3 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-05-15 Epub Date: 2026-01-31 DOI: 10.1016/j.ces.2026.123486
Ruijun Wang , Zhen Dong , Hui Wang , Yongbin Zou , Huaqi Zhang , Xue Hao , Yuan Gao , Zhiwen Ye , Hongxun Hao
1,2-Di(1′H-[1,5′-bitetrazol]-5-yl)diazene (DBD) is considered a promising high-energy, nitrogen-rich material. However, its practical utilization is limited by low solubility and insufficient understanding of its thermodynamic behavior. To address this, the solid–liquid equilibrium of DBD was examined in four pure solvents (water, acetonitrile, acetone, and 1,4-dioxane) and three binary solvent systems (with water as the anti-solvent) from 278.15 to 318.15 K using gravimetric method. The van’t Hoff, modified Apelblat, Yaws, GCM, and Jouyban-Acree models all yielded excellent correlations with the experimentally determined solubility data of DBD, among which the modified Apelblat model stood out with superior performance. A multi-technique approach was employed to unravel the molecular mechanisms. Hirshfeld surface analysis identified the preferential spatial contacts within the crystal structure, while molecular electrostatic potential (ESP) analysis exhibited the surface charge characteristics relevant to solute–solvent interactions. Combined DFT/IGMH/AIM analysis elucidated the dissolution mechanism: water solvent effectively disrupts solute–solute binding but demands high reorganization energy. Mixed solvents, on the other hand, optimize this energy balance, thereby creating a superior solubilizing environment. Molecular dynamics simulations revealed that the maximum solubility of DBD in binary water-organic solvent systems occurs at specific mixing ratios. This maximum is directly linked to the peak in solute–solvent interaction energy, as evidenced by its primary dependence on optimized hydrogen bonding and van der Waals interactions. This finding establishes a coherent framework linking macroscopic thermodynamics to microscopic molecular interactions, thereby affording fundamental insights for the practical optimization of DBD.
1,2-二(1 ' h-[1,5 ' -双四唑]-5-基)二氮烯(DBD)被认为是一种很有前途的高能量富氮物质。然而,由于其溶解度低和对其热力学行为了解不足,限制了其实际应用。为了解决这个问题,用重量法研究了DBD在278.15 ~ 318.15 K范围内的四种纯溶剂(水、乙腈、丙酮和1,4-二恶烷)和三种二元溶剂(水为反溶剂)体系中的固液平衡。van 't Hoff模型、改进的Apelblat模型、Yaws模型、GCM模型和Jouyban-Acree模型均与实验测定的DBD溶解度数据具有良好的相关性,其中改进的Apelblat模型表现优异。采用多技术方法来揭示分子机制。Hirshfeld表面分析确定了晶体结构内部的优先空间接触,而分子静电势(ESP)分析显示了与溶质-溶剂相互作用相关的表面电荷特征。DFT/IGMH/AIM联合分析阐明了溶解机理:水溶剂有效破坏溶质-溶质结合,但需要高重组能。另一方面,混合溶剂优化了这种能量平衡,从而创造了优越的溶解环境。分子动力学模拟表明,DBD在二元水-有机溶剂体系中的最大溶解度发生在特定的混合比下。这一最大值与溶质-溶剂相互作用能的峰值直接相关,其主要依赖于优化的氢键和范德华相互作用。这一发现建立了宏观热力学与微观分子相互作用的连贯框架,从而为DBD的实际优化提供了基础见解。
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引用次数: 0
Performance of Fe2O3/graphene hybrid nanofluids within an alternating oval tube: experimental investigation of the effects of pitch angle 交替椭圆管中Fe2O3/石墨烯混合纳米流体的性能:俯仰角影响的实验研究
IF 4.3 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-05-15 Epub Date: 2026-02-08 DOI: 10.1016/j.ces.2026.123537
Sasidhar Gurugubelli , Singuru Madhavarao , Yarrapragada K.S.S. Rao , Rapaka Jagadeesh , Ravikiran Balaga , Javed Syed
The effect of pitch angle on the design of an alternative oval tube heat exchanger is evaluated using Fe2O3/graphene hybrid nanofluid. The hybrid nanofluids were successfully synthesized, achieving optimal thermal conductivity at a 3:2 wt ratio. Experiments were conducted with different pitch angles (30°, 45°, 60°, and 90°) and nanoparticle concentrations ranging from 0.01% to 0.03%. The Nusselt number increased with the Reynolds number, by 12 to 20% at a 30° pitch compared to a 90° pitch, suggesting better heat transfer at lower pitch angles. Conversely, the friction factor and pressure drop exhibited a decrease with the Reynolds number, yet remained 8 to 15% elevated. It is observed that the highest concentration (0.03%) results in a 12% improvement in the heat transfer coefficient over 0.01%. Performance index ratios (PIR) decrease by approximately 25% as Reynolds numbers rise from 250 to 2000, with a 30° angle yielding a 12% higher PIR than 90°. The study suggests that a 30° pitch with a nanoparticle concentration of 0.02–0.03% at moderate Reynolds numbers (1000–1500) optimises heat transfer. Furthermore, a balanced design, favoring a 45° pitch angle and moderate nanofluid concentration, optimizes thermal performance while minimizing frictional losses, providing essential guidelines for effective industrial heat exchanger design.
利用Fe2O3/石墨烯混合纳米流体,研究了俯角对椭圆管换热器设计的影响。成功合成了混合纳米流体,在3:2的重量比下获得了最佳导热性。实验采用不同的俯仰角(30°、45°、60°和90°),纳米颗粒浓度为0.01%至0.03%。努塞尔数随着雷诺数的增加而增加,在30°俯仰角时比在90°俯仰角时增加了12 - 20%,这表明在较低的俯仰角下传热效果更好。相反,摩擦系数和压降随雷诺数的增加而减小,但仍保持8% ~ 15%的升高。观察到,最高浓度(0.03%)的传热系数比0.01%提高了12%。当雷诺数从250增加到2000时,性能指数比(PIR)下降了约25%,其中30°角比90°角的PIR高12%。研究表明,在中等雷诺数(1000-1500)下,30°螺距、纳米颗粒浓度为0.02-0.03%时,传热效果最佳。此外,一个平衡的设计,有利于45°的俯仰角和适度的纳米流体浓度,优化热性能,同时最大限度地减少摩擦损失,为有效的工业热交换器设计提供必要的指导。
{"title":"Performance of Fe2O3/graphene hybrid nanofluids within an alternating oval tube: experimental investigation of the effects of pitch angle","authors":"Sasidhar Gurugubelli ,&nbsp;Singuru Madhavarao ,&nbsp;Yarrapragada K.S.S. Rao ,&nbsp;Rapaka Jagadeesh ,&nbsp;Ravikiran Balaga ,&nbsp;Javed Syed","doi":"10.1016/j.ces.2026.123537","DOIUrl":"10.1016/j.ces.2026.123537","url":null,"abstract":"<div><div>The effect of pitch angle on the design of an alternative oval tube heat exchanger is evaluated using Fe<sub>2</sub>O<sub>3</sub>/graphene hybrid nanofluid. The hybrid nanofluids were successfully synthesized, achieving optimal thermal conductivity at a 3:2 wt ratio. Experiments were conducted with different pitch angles (30°, 45°, 60°, and 90°) and nanoparticle concentrations ranging from 0.01% to 0.03%. The Nusselt number increased with the Reynolds number, by 12 to 20% at a 30° pitch compared to a 90° pitch, suggesting better heat transfer at lower pitch angles. Conversely, the friction factor and pressure drop exhibited a decrease with the Reynolds number, yet remained 8 to 15% elevated. It is observed that the highest concentration (0.03%) results in a 12% improvement in the heat transfer coefficient over 0.01%. Performance index ratios (PIR) decrease by approximately 25% as Reynolds numbers rise from 250 to 2000, with a 30° angle yielding a 12% higher PIR than 90°. The study suggests that a 30° pitch with a nanoparticle concentration of 0.02–0.03% at moderate Reynolds numbers (1000–1500) optimises heat transfer. Furthermore, a balanced design, favoring a 45° pitch angle and moderate nanofluid concentration, optimizes thermal performance while minimizing frictional losses, providing essential guidelines for effective industrial heat exchanger design.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"326 ","pages":"Article 123537"},"PeriodicalIF":4.3,"publicationDate":"2026-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138480","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 4.3 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-05-15 Epub 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 ,&nbsp;Chaofan Qi ,&nbsp;Dingding Liu ,&nbsp;Guohua Jing ,&nbsp;Yongdan Li ,&nbsp;Huawang Zhao","doi":"10.1016/j.ces.2026.123547","DOIUrl":"10.1016/j.ces.2026.123547","url":null,"abstract":"<div><div>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.</div></div>","PeriodicalId":271,"journal":{"name":"Chemical Engineering Science","volume":"326 ","pages":"Article 123547"},"PeriodicalIF":4.3,"publicationDate":"2026-05-15","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
A passive and stable aerogel reactor based on Ag-loading cellulose Pickering emulsion 基于载银纤维素皮克林乳液的被动稳定气凝胶反应器
IF 4.3 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-05-15 Epub Date: 2026-02-06 DOI: 10.1016/j.ces.2026.123520
Jian Liu , Jianyi Song , Na Liu , Qiao Lan
A pump-free, stable and efficient aerogel reactor with abundant pores is designed using Ag-loading cellulose Pickering emulsions as a template for the continuous flow catalytic reduction of 4-nitrophenol. The fabrication of the aerogel reactor entails the two-step oxidation synthesis of aldehyde-functionalized cellulose nanocrystals (ACNC), the in-situ reduction of Ag nanoparticles (NPs) on them to form Ag@ACNC, the utilization of this material to stabilize a Pickering emulsion for preparing the hydrogel, and finally the freeze-drying of the hydrogel laying on a fabric strip. The emulsion-templated aerogel features abundant pores with loading Ag NPs on inner walls, enabling reactant to flow through the pores rapidly under driving by its gravity and the capillary action of the supporting fabric strip and react on the walls. The aerogel reactor achieves efficient three-dimensional flow catalysis without an external power source and exhibits excellent conversion and stability. The conversion all remains above 91.8% during the continuous flow catalysis reaction of 6 cycles (totaling 72 h), and the conversion still reaches 94.4% at 12 h after storage in air for 60 days. This emulsion-templated aerogel reactor demonstrates great potential for advancing recyclable catalytic systems, thereby paving the way for its wide applications.
以载银纤维素Pickering乳液为模板,设计了一种无泵、稳定、高效、孔隙丰富的气凝胶反应器,用于4-硝基苯酚的连续流催化还原。气凝胶反应器的制造需要两步氧化合成醛功能化纤维素纳米晶体(ACNC),在其上原位还原银纳米粒子(NPs)形成Ag@ACNC,利用该材料稳定制备水凝胶的Pickering乳液,最后将水凝胶放置在织物条上进行冷冻干燥。乳液模板气凝胶具有丰富的孔隙,在其内壁上加载了Ag NPs,在其重力和支撑织物条的毛细作用下,反应物可以快速流过孔隙,并在壁上发生反应。该气凝胶反应器无需外部电源即可实现高效的三维流动催化,并具有良好的转化率和稳定性。连续流动催化反应6个循环(共72 h),转化率均保持在91.8%以上,在空气中贮存60 天,12 h转化率仍达到94.4%。这种乳液模板气凝胶反应器在推进可回收催化系统方面显示出巨大的潜力,从而为其广泛应用铺平了道路。
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引用次数: 0
Electro-initiated co-precipitation for synthesis of copper-based powder catalysts 电共沉淀法合成铜基粉末催化剂
IF 4.3 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-05-15 Epub Date: 2026-02-06 DOI: 10.1016/j.ces.2026.123549
Haoyuan Gu , Shengbin Dong , Pengfei Tian , Jiancheng Guo , Fu-Zhen Xuan , Minghui Zhu
Copper-based catalysts are extensively utilized in heterogeneous catalysis due to their cost-effectiveness and superior activity. However, their industrial production predominantly relies on conventional precipitation or impregnation methods, which inevitably generate substantial liquid and gaseous waste. Furthermore, these routes typically depend on nitrate precursors, where the production involves dissolving metals in strong acids, creating significant upstream environmental burdens. To address these issues, this work presents a facile and environmentally friendly electrochemical synthesis strategy. In this approach, a Cu mesh acts as the in-situ Cu2+ source, while OH– generated from the hydrogen evolution reaction serves as the precipitating agent. Furthermore, by adding sodium citrate to the electrolyte, we can control the morphology of the catalyst, and by replacing the metal cations in the nitrate electrolyte, we can control the composition of the catalyst. Notably, a copper-cerium mixed oxide synthesized with 0.1 M cerium nitrate and 0.01 M sodium citrate delivers exceptional performance in CO oxidation, achieving a T60 of 78 ℃ and a T90 of 92 ℃. This enhanced activity is attributed to a unique dispersed nanosheet morphology that promotes the formation of Cu-Ce solid solutions and oxygen vacancies. Consequently, this green synthesis protocol holds great promise for sustainable industrial catalyst manufacturing.
铜基催化剂因其经济高效、活性优异而广泛应用于多相催化。然而,它们的工业生产主要依赖于传统的沉淀或浸渍方法,这不可避免地产生大量的液体和气体废物。此外,这些途径通常依赖于硝酸盐前体,其生产涉及将金属溶解在强酸中,造成严重的上游环境负担。为了解决这些问题,本工作提出了一种简便、环保的电化学合成策略。在该方法中,Cu网作为原位Cu2+源,析氢反应产生的OH -作为沉淀剂。此外,通过在电解质中加入柠檬酸钠,我们可以控制催化剂的形态,通过替换硝酸盐电解质中的金属阳离子,我们可以控制催化剂的组成。值得注意的是,以0.1 M硝酸铈和0.01 M柠檬酸钠合成的铜铈混合氧化物具有优异的CO氧化性能,T60为78℃,T90为92℃。这种增强的活性归因于独特的分散纳米片形态,促进了Cu-Ce固溶体和氧空位的形成。因此,这种绿色合成协议为可持续的工业催化剂制造提供了巨大的希望。
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引用次数: 0
One-step nanoprecipitation of polymeric nanoparticles with tunable size, uniformity, shape and surface function 一步法制备具有可调尺寸、均匀性、形状和表面功能的聚合物纳米颗粒
IF 4.3 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-05-15 Epub Date: 2026-02-06 DOI: 10.1016/j.ces.2026.123557
Dongpeng Sun , Jingyi Chen , Canghai Luo , Yuan Zheng , Xinxiong Wang , Baoling Guo , David A. Weitz , Dong Chen
The full potentials of polymeric nanoparticles (NPs) in advanced applications strongly rely on the precise control of their physicochemical properties and some of them remain unexplored. Here, a facile strategy is presented to prepare polymeric NPs with tunable size, uniformity, shape and surface function in a single step by nanoprecipitation. Upon solvent exchange, the formation of NPs experiences three steps, including supersaturation, nucleation and growth. It is demonstrated that rapid mixing by microfluidics is a prerequisite to control the nanoprecipitation process and the precise control of NP size, uniformity, shape and surface function in a single step further broadens their applications. The insight on the underlying mechanism also shines light on the advancements of nanoprecipitation techniques. The review provides a systematic guideline for the rational design and one-step preparation of polymeric NPs with desired functions and optimal performances.
聚合物纳米粒子(NPs)在高级应用中的全部潜力强烈依赖于对其物理化学性质的精确控制,其中一些尚未开发。本文提出了一种简单的方法,通过纳米沉淀法一步制备具有可调尺寸、均匀性、形状和表面功能的聚合物纳米粒子。经过溶剂交换,NPs的形成经历了过饱和、成核和生长三个步骤。研究表明,微流体的快速混合是控制纳米沉淀过程的先决条件,而在一步中精确控制NP的大小、均匀性、形状和表面功能进一步拓宽了微流体的应用范围。对潜在机制的洞察也照亮了纳米沉淀技术的进步。本文综述为合理设计和一步制备具有理想功能和最佳性能的高分子NPs提供了系统的指导。
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引用次数: 0
Intensification of one-step mixing for the preparation of Al2O3-H2O nanofluids using free triple-impinging jets 利用自由三冲击射流强化一步混合制备Al2O3-H2O纳米流体
IF 4.3 2区 工程技术 Q2 ENGINEERING, CHEMICAL Pub Date : 2026-05-15 Epub Date: 2026-02-07 DOI: 10.1016/j.ces.2026.123539
Jun Zhang , Peng-fei Liang , You-zhi Liu
A novel one-step mixing using free triple-impinging jets (FTIJs) was employed to prepare Al2O3–H2O nanofluids. The effects of key operating parameters, namely, horizontal nozzle distance (w = 10 mm & 20 mm), perpendicular nozzle distance (h = 10 mm & 20 mm), H2O/SDBS jet velocity u (1.6 m/s ∼ 4.8 m/s), Al2O3 mass flow rate Q1 (1.2 g/h ∼ 3 g/h), and SDBS mass fraction ω (0.4% ∼ 1.2%) on the stability, size, and morphology of Al2O3–H2O nanofluids were systematically investigated through experimental studies. For comparative analysis, free opposed impinging jets (FOIJs) was implemented, in which two liquid jets from two horizontally aligned nozzle and collide in a wall-free environment, enabling a two-step mixing of Al2O3–H2O nanofluids preparation. The results indicate that increasing u and Q1 leads to reduced sedimentation height, transmissivity and average diameter, along with an increased absolute value of zeta potential, so that the stability and size uniformity are improved, with the minimum average diameter reaching 48 nm. In contrast, increasing the nozzle distance resulted in adverse trends in both stability and nanofluids size. Optimal performance was observed at ω = 0.6%, where Al2O3–H2O nanofluids exhibited superior stability and smaller sizes. Compared to the one-step mixing in FTIJs, the two-step mixing in FOIJs is inferior stability and thermal conductivity performance. These findings demonstrate that FTIJs effectively intensifies the one-step mixing for Al2O3–H2O nanofluids preparation, providing a theoretical basis for advanced nanofluids fabrication, as well as expanding existing preparation methodologies and broadening the application potential of free impinging jets.
采用自由三冲击射流一步混合制备了Al2O3-H2O纳米流体。关键操作参数的影响,即水平喷嘴距离(w =  10毫米,20 毫米),垂直喷嘴距离(h =  10 mm, 20 毫米),水/深发展喷射速度u(1.6 m / s ∼  4.8 m / s),氧化铝质量流率Q1 (1.2 g / h  ∼ 3 g / h),和深发展质量分数ω(0.4%∼1.2%)稳定性,纳米流体大小和形态的Al2O3-H2O纳米流体系统进行了实验研究。为了进行对比分析,采用了自由对置碰撞射流(FOIJs),即来自两个水平对齐喷嘴的两束液体射流在无壁环境中碰撞,实现了Al2O3-H2O纳米流体制备的两步混合。结果表明:增大u和Q1,沉降高度、透过率和平均粒径降低,zeta电位绝对值增大,稳定性和粒径均匀性提高,最小平均粒径可达48 nm;相反,增加喷嘴距离会导致稳定性和纳米流体尺寸的不利趋势。当ω = 0.6%时,Al2O3-H2O纳米流体表现出更好的稳定性和更小的尺寸。与ftij的一步混合相比,foij的两步混合稳定性和导热性能较差。这些发现表明,FTIJs有效地强化了Al2O3-H2O纳米流体制备的一步混合,为先进的纳米流体制备提供了理论基础,并扩展了现有的制备方法,拓宽了自由撞击射流的应用潜力。
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Chemical Engineering Science
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