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Establishing the custom 3D printing of thermally conductive elastomer composites with flexibility and resilience by coupling dual-filler networks 通过耦合双填料网络,建立具有柔性和弹性的导热弹性体复合材料的定制3D打印
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-10 DOI: 10.1016/j.cej.2026.174040
Junrui Tan, Guizhi Zhu, Mingwei Yang, Qiong Wu, Yong Li, Longfei Tan, Xianwei Meng
Material-extrusion-based 3D printing technology has shown advantages in promoting the on-demand fabrication of silicone-based flexible thermal interface materials (TIMs). However, the incompatibility between high-loading fillers and silicone matrix seriously deteriorates the ink printability and the comprehensive mechanical strength, leaving a great challenge in designing multi-functional silicone elastomers. In this work, a strategy of constructing dual-filler networks for 3D printable thermally conductive silicone elastomers was proposed. For silicone inks, the fumed silica nanoparticles with the branched structure realized the ink thixotropy. Meanwhile, fumed silica with small-scaled island structure guaranteed the self-supporting ability of printed filaments without sacrificing the ink extrudability. Multi-scaled AlN micro-spheres with silane modification were close-packed to construct continuous thermally conductive pathways. Dual-filler networks realized the ink printability and synergistically enhanced thermally conductive and mechanical properties. The 3D-printed products could also be shaped into various architectures to fit the heating objects. Meanwhile, it succeeded in realizing a superior thermal conductivity of up to 5.50 W m−1 K−1 even at −80 °C, a resilience of above 90% at 40% strain, and stable heat dissipation capacity over a wide temperature range of −80 to 200 °C. Therefore, our work could inspire the utilization of 3D printing in fabricating elastomers with functional architectures.
基于材料挤压的3D打印技术在促进硅基柔性热界面材料(TIMs)的按需制造方面显示出优势。然而,高负荷填料与有机硅基体的不相容性严重影响了油墨的可印刷性和综合机械强度,给多功能有机硅弹性体的设计带来了很大的挑战。在这项工作中,提出了一种构建双填充网络的策略,用于3D打印导热硅弹性体。对于有机硅油墨,气相二氧化硅纳米颗粒具有支链结构,实现了油墨的触变性。同时,具有小尺寸岛状结构的气相二氧化硅保证了印刷长丝的自支撑能力,同时又不牺牲油墨的可挤出性。硅烷修饰的多尺度AlN微球被紧密排列以构建连续的导热通道。双填料网络实现了油墨的可印刷性,并协同提高了导热性能和机械性能。3d打印产品还可以塑造成各种结构,以适应加热物体。同时,它成功地实现了优异的导热系数高达5.50 W m−1 K−1,即使在−80 °C下,40%应变下的回弹性也超过90%,并且在−80至200 °C的宽温度范围内具有稳定的散热能力。因此,我们的工作可以激发3D打印在制造具有功能结构的弹性体中的应用。
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引用次数: 0
Perovskite single-crystal photodetectors: Recent breakthroughs for superior device performance 钙钛矿单晶光电探测器:卓越器件性能的最新突破
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-10 DOI: 10.1016/j.cej.2026.173995
Abdul Kareem Kalathil Soopy, Shengzhong (Frank) Liu, Adel Najar
Metal-halide-based perovskite single crystals (SCs) now rival epitaxial III–V materials for high-performance photodetection, yet can be grown from solution in minutes on almost any substrate. Recent “crystal-by-design” protocols—inverse-temperature, anti-solvent, and laser-assisted cooling routes—routinely deliver millimeter-scale boules and laterally patterned micro/nanowires with defect densities below 1010 cm−3. Dimensional tuning, from bulk crystals to microstructures, thin films, and nanowires, has further enhanced device performance by facilitating tailored charge transport pathways. When integrated into photoconductor-type architectures, these SCs have demonstrated remarkable improvements in response speed, detectivity, and responsivity. Moreover, strategies such as surface passivation and thickness optimization have contributed to enhanced stability and more efficient carrier dynamics. Concurrently, the incorporation of functional materials—including graphene, WS₂, quantum dots, and carbon nanotubes—into interface engineering and heterojunction design has significantly improved charge separation efficiency and suppressed carrier recombination. These advances have already yielded flexible, pixelated imagers for X-ray and hyperspectral cameras, biocompatible sensors capable of single-photon-level fluorescence lifetime imaging, device architectures, and broadband photodetection capabilities. Continued convergence of scalable growth, surface science, and heterogeneous integration is poised to transition perovskite single-crystal photodetectors from laboratory curiosities to commercial platforms within the next few years.
金属卤化物基钙钛矿单晶(SCs)现在可以与高性能光探测外延III-V材料相媲美,但可以在几乎任何衬底上从溶液中在几分钟内生长。最近的“晶体设计”方案-反温度,抗溶剂和激光辅助冷却路线-通常提供毫米级的孔和横向图案的微/纳米线,缺陷密度低于1010 cm−3。尺寸调谐,从块状晶体到微结构、薄膜和纳米线,通过促进定制电荷传输路径,进一步提高了器件性能。当集成到光导体型架构中时,这些sc在响应速度,探测性和响应性方面表现出显着的改善。此外,表面钝化和厚度优化等策略有助于增强稳定性和更有效的载流子动力学。同时,在界面工程和异质结设计中加入石墨烯、WS₂、量子点和碳纳米管等功能材料,显著提高了电荷分离效率,抑制了载流子复合。这些进步已经产生了用于x射线和高光谱相机的灵活的像素化成像仪,能够单光子级荧光寿命成像的生物兼容传感器,设备架构和宽带光探测能力。可扩展增长、表面科学和异质集成的持续融合,将在未来几年内将钙钛矿单晶光电探测器从实验室的好奇心转变为商业平台。
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引用次数: 0
Interfacial environment modulation by nanoneedle-shaped polyaniline for enhanced hydrogen isotope separation by water electrolysis 纳米针状聚苯胺对界面环境的调节促进水电解氢同位素分离
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-10 DOI: 10.1016/j.cej.2026.173948
Rui Li, Guoyu Li, Penghui Xiong, Yuhan Wu, Ruidong Liu, Hang Zhong, Yue Yao, Xin Xiang, Wenhua Luo, Jingsong Xu
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引用次数: 0
Simultaneous remediation and fertilization of saline-alkaline soil via the application of various phosphorus-rich hydrochars 利用各种富磷烃类对盐碱土的同步修复和施肥
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-10 DOI: 10.1016/j.cej.2026.174020
Ran Duan, Yuxin Yang, Xuchen Zhang, Junxia Wang, Jipeng Luo, Xiaoqiang Cui, Zhanjun Cheng, Guanyi Chen
Soil salinization and phosphorus (P) scarcity constrain agroecosystem sustainability. In this study, Acorus calamus hydrochar (ACH) and chicken manure hydrochar (CMH) were prepared via hydrothermal carbonization and applied to achieve the simultaneous remediation and fertilization of saline-alkaline soil. The total P was enriched in the hydrochars (3.78–9.19 and 16.23–22.39 mg/g for ACH and CMH) and labile P was transformed to stable orthophosphates. Both hydrochars reduced salinity and improved fertility with distinct functions. ACH excelled in salinity alleviation and enhanced the availability of soil P, while increasing available potassium by 26.5% to 117.23 mg/kg. CMH provided a long-term P source via mineral crystallization, increasing available P (up 72.6% to 6.99 mg/kg) and P measured by diffusive gradients in thin films (up 74.0% to 234.29 μg/L), while also enhancing available nitrogen by 29.1%. The microbial community analysis revealed ACH enriched Proteobacteria (54.65%) and saprotrophic fungi, which are associated with organic P cycling processes. In contrast, CMH promoted salt-tolerant Firmicutes (12.80%) and boosted phytase activities (up to 162%), facilitating P release. Therefore, the production and application of P-rich hydrochars could be a promising strategy for the amelioration of saline-alkaline soil, offering novel insights for P recycling and sustainable land management.
土壤盐渍化和磷缺乏制约了农业生态系统的可持续性。本研究采用水热炭化法制备菖蒲水炭(ACH)和鸡粪水炭(CMH),并将其应用于盐碱地的同时修复与施肥。总磷在烃类中富集(ACH和CMH分别为3.78 ~ 9.19和16.23 ~ 22.39 mg/g),不稳定的P转化为稳定的正磷酸盐。两种烃类化合物都具有不同的降低盐度和提高肥力的功能。乙酰氨基酚具有明显的缓盐和提高土壤磷有效性的作用,使土壤速效钾提高26.5%,达到117.23 mg/kg。CMH通过矿物结晶提供了长期磷源,提高了有效磷(增加72.6%至6.99 mg/kg)和通过薄膜扩散梯度测量的磷(增加74.0%至234.29 μg/L),同时提高了有效氮29.1%。微生物群落分析显示,与有机磷循环过程相关的Proteobacteria(54.65%)和腐养真菌富集ACH。相比之下,CMH提高了耐盐厚壁菌门(12.80%),提高了植酸酶活性(高达162%),促进了磷的释放。因此,富磷碳氢化合物的生产和应用可能是盐碱地改良的一种有前景的策略,为磷循环利用和土地可持续管理提供了新的见解。
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引用次数: 0
Engineering interfacial charge redistribution in Sb2Te3/MoS2 topological heterojunction for enhanced bifunctional electrocatalysis Sb2Te3/MoS2拓扑异质结中增强双功能电催化的工程界面电荷重分配
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-10 DOI: 10.1016/j.cej.2026.174016
Shoujun Ma, Shouyi Wang, Dingxuan Zhang, Xuan Fang, Ying Yang, Dan Fang, Haiyan Tao, Baitong Zhou, Jiayao Jiang, Junjie Pan, Dengkui Wang, Yong Wang, Hao Yan, Jinhua Li, Xiaohua Wang, Dongbo Wang
The development of efficient bifunctional electrocatalysts for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is critical for achieving sustainable hydrogen production through water splitting. A fundamental challenge lies in combining high catalytic activity with rapid charge transport, as conventional electrocatalysts must often strike a balance between these properties. For instance, transition metal dichalcogenides such as MoS2 provide abundant active sites, but suffer from limited conductivity, whereas topological insulators such as Sb2Te3 possess highly conductive surface states, yet lack sufficient catalytic activity. To address this limitation, we constructed a heterojunction by integrating MoS2 with Sb2Te3 on nickel–molybdenum foam (MoS2/Sb2Te3@NMF). The resulting hybrid catalyst exhibited exceptional bifunctional performance in an alkaline electrolyte, achieving ultralow overpotentials of 14 mV for HER and 16 mV for OER at 10 mA·cm−2, with Tafel slopes of 16 and 70 mV·dec−1, respectively, comparable with those of noble metal benchmarks. Mechanistic analysis revealed that the metallic topological surface states of Sb2Te3 promote a significant charge redistribution and the formation of a built-in electric field at the heterointerface, which collectively enhance the charge transfer and optimize the adsorption free energy of reaction intermediates. This work shows that the combination of topological insulators with transition metal dichalcogenides represents an ideal design strategy for high-performance bifunctional electrocatalysts, highlighting the broad potential of topological heterointerfaces in advancing electrocatalytic hydrogen production.
为析氢反应(HER)和析氧反应(OER)开发高效的双功能电催化剂是实现水裂解可持续制氢的关键。一个基本的挑战在于将高催化活性与快速电荷传输结合起来,因为传统的电催化剂通常必须在这些特性之间取得平衡。例如,过渡金属二硫族化合物如MoS2提供丰富的活性位点,但导电性有限,而拓扑绝缘体如Sb2Te3具有高导电性的表面状态,但缺乏足够的催化活性。为了解决这一限制,我们通过将MoS2与Sb2Te3集成在镍钼泡沫(MoS2/Sb2Te3@NMF)上构建了异质结。所制备的杂化催化剂在碱性电解质中表现出优异的双功能性能,在10 mA·cm−2下,HER和OER的过电位分别为14 mV和16 mV, Tafel斜率分别为16和70 mV·dec−1,与贵金属基准相当。机理分析表明,Sb2Te3的金属拓扑表面态促进了显著的电荷重分配,并在异质界面处形成了内置电场,共同增强了电荷转移,优化了反应中间体的吸附自由能。这项工作表明,拓扑绝缘体与过渡金属二硫族化合物的结合代表了高性能双功能电催化剂的理想设计策略,突出了拓扑异质界面在推进电催化制氢方面的广阔潜力。
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引用次数: 0
A high-dielectric additive for enhanced supercapacitor performance with N-doped carbon electrodes 一种用于增强n掺杂碳电极超级电容器性能的高介电添加剂
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-10 DOI: 10.1016/j.cej.2026.174038
Hongyu Liang, Hui Li, Shengda Tang, Jiahui Li, Zhaomin Zhu, Li Pan, Yongfeng Bu
Carbon-based supercapacitors represent one of the most widely utilized commercial capacitive energy storage devices. Organic electrolyte systems, particularly tetraethylammonium tetrafluoroborate/acetonitrile (TEABF4/AN), have maintained market dominance for decades due to their superior cost-effectiveness and performance characteristics. However, the potential of conventional carbon-tuning methods to enhance capacitance is now largely exhausted. Herein, we demonstrate that introducing a high dielectric constant organic salt (triethylmethylammonium tetrafluoroborate, TEMABF4) as an electrolyte additive can dramatically increase capacitance. At an optimal concentration of 2 wt% TEMABF4, the capacitance increases by 26% to exceed 200 F g−1, achieving an exceptional energy density of 50 Wh kg−1. This enhancement is due to the smaller radius and asymmetric structure of TEMA+ that compresses the double-layer thickness, surpassing traditional capacitance limits. The underlying mechanism is validated through in situ Raman spectroscopy and molecular dynamics simulations. This electrolyte additive paves the way for high-energy-density supercapacitors by transcending current capacitance limits.
碳基超级电容器是应用最广泛的商用电容储能装置之一。有机电解质系统,特别是四氟硼酸四乙基铵/乙腈(TEABF4/AN),由于其优越的成本效益和性能特点,几十年来一直保持着市场主导地位。然而,传统碳调谐方法提高电容的潜力现在基本上已经耗尽。在此,我们证明了引入高介电常数有机盐(三乙基甲基四氟硼酸铵,TEMABF4)作为电解质添加剂可以显着增加电容。当TEMABF4的最佳浓度为2 wt%时,电容增加26%,超过200 F g−1,实现了50 Wh kg−1的特殊能量密度。这种增强是由于TEMA+的半径更小,结构不对称,压缩了双层厚度,超越了传统的电容限制。通过原位拉曼光谱和分子动力学模拟验证了其潜在机制。这种电解质添加剂通过超越电流电容限制为高能量密度超级电容器铺平了道路。
{"title":"A high-dielectric additive for enhanced supercapacitor performance with N-doped carbon electrodes","authors":"Hongyu Liang, Hui Li, Shengda Tang, Jiahui Li, Zhaomin Zhu, Li Pan, Yongfeng Bu","doi":"10.1016/j.cej.2026.174038","DOIUrl":"https://doi.org/10.1016/j.cej.2026.174038","url":null,"abstract":"Carbon-based supercapacitors represent one of the most widely utilized commercial capacitive energy storage devices. Organic electrolyte systems, particularly tetraethylammonium tetrafluoroborate/acetonitrile (TEABF<ce:inf loc=\"post\">4</ce:inf>/AN), have maintained market dominance for decades due to their superior cost-effectiveness and performance characteristics. However, the potential of conventional carbon-tuning methods to enhance capacitance is now largely exhausted. Herein, we demonstrate that introducing a high dielectric constant organic salt (triethylmethylammonium tetrafluoroborate, TEMABF<ce:inf loc=\"post\">4</ce:inf>) as an electrolyte additive can dramatically increase capacitance. At an optimal concentration of 2 wt% TEMABF<ce:inf loc=\"post\">4</ce:inf>, the capacitance increases by 26% to exceed 200 F g<ce:sup loc=\"post\">−1</ce:sup>, achieving an exceptional energy density of 50 Wh kg<ce:sup loc=\"post\">−1</ce:sup>. This enhancement is due to the smaller radius and asymmetric structure of TEMA<ce:sup loc=\"post\">+</ce:sup> that compresses the double-layer thickness, surpassing traditional capacitance limits. The underlying mechanism is validated through in situ Raman spectroscopy and molecular dynamics simulations. This electrolyte additive paves the way for high-energy-density supercapacitors by transcending current capacitance limits.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"32 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153171","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}
引用次数: 0
Preparation of the core-shell grained Li4SiO4 pebble with an excellent CO2 adsorption capacity by solidification of suspension 采用悬浮液固化法制备具有优异CO2吸附性能的核-壳粒状Li4SiO4卵石
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-10 DOI: 10.1016/j.cej.2026.174037
Shuxian Wu, Jingli Shi, Hailiang Wang, Peng Yang, Aixia Guo, Penghe Xu, Chaoyang Jia, Lina Zheng, Feng Yu, Hongxia Lu, Hongliang Xu, Hailong Wang
Li4SiO4 has the expansive prospect for high-temperature CO₂ capture. However, the traditional Li4SiO4 powders or pebble adsorbents have a low adsorption efficiency and ordinary cycle stability. In the study, the core-shell grained Li4SiO4 adsorbent pebble was fabricated by using a novel solidification of suspension. The phase composition, microstructure, crushing load, and specific surface area were characterized. And the dynamic and cyclic adsorption/desorption properties were investigated. The core-shell grained Li4SiO4 pebbles displayed excellent dynamic adsorption capacity of 32.7 wt%, and high cyclic adsorption capacity of 29.8–32.4 wt% during 20 cycles. DFT calculations revealed that the presence of Li and O vacancies on the rough poriferous core significantly lowered the diffusion energy barrier to improve CO2 adsorption capacity. Besides, the dense shell prevented the structure from collapsing. In generally, the core-shell grained Li4SiO4 pebbles by solidification of suspension, as an efficient CO2 ceramic adsorbent, will have great application potential in the field of high-temperature CO2 adsorption.
Li4SiO4在高温捕集CO₂方面具有广阔的前景。然而,传统的Li4SiO4粉末或鹅卵石吸附剂的吸附效率较低,循环稳定性一般。在本研究中,采用新型悬浮液凝固法制备了核-壳粒型Li4SiO4吸附剂卵石。表征了材料的相组成、显微组织、破碎载荷和比表面积。并对其动态和循环吸附/解吸性能进行了研究。核壳粒状Li4SiO4鹅卵石在20次 循环中表现出优异的动态吸附容量为32.7 wt%,较高的循环吸附容量为29.8 ~ 32.4 wt%。DFT计算表明,粗孔岩心上Li和O空位的存在显著降低了扩散能垒,提高了CO2吸附能力。此外,致密的外壳防止了结构的倒塌。总体而言,经悬浮液固化而成的核壳粒状Li4SiO4鹅卵石作为一种高效的CO2陶瓷吸附剂,在高温CO2吸附领域将具有很大的应用潜力。
{"title":"Preparation of the core-shell grained Li4SiO4 pebble with an excellent CO2 adsorption capacity by solidification of suspension","authors":"Shuxian Wu, Jingli Shi, Hailiang Wang, Peng Yang, Aixia Guo, Penghe Xu, Chaoyang Jia, Lina Zheng, Feng Yu, Hongxia Lu, Hongliang Xu, Hailong Wang","doi":"10.1016/j.cej.2026.174037","DOIUrl":"https://doi.org/10.1016/j.cej.2026.174037","url":null,"abstract":"Li<ce:inf loc=\"post\">4</ce:inf>SiO<ce:inf loc=\"post\">4</ce:inf> has the expansive prospect for high-temperature CO₂ capture. However, the traditional Li<ce:inf loc=\"post\">4</ce:inf>SiO<ce:inf loc=\"post\">4</ce:inf> powders or pebble adsorbents have a low adsorption efficiency and ordinary cycle stability. In the study, the core-shell grained Li<ce:inf loc=\"post\">4</ce:inf>SiO<ce:inf loc=\"post\">4</ce:inf> adsorbent pebble was fabricated by using a novel solidification of suspension. The phase composition, microstructure, crushing load, and specific surface area were characterized. And the dynamic and cyclic adsorption/desorption properties were investigated. The core-shell grained Li<ce:inf loc=\"post\">4</ce:inf>SiO<ce:inf loc=\"post\">4</ce:inf> pebbles displayed excellent dynamic adsorption capacity of 32.7 wt%, and high cyclic adsorption capacity of 29.8–32.4 wt% during 20 cycles. DFT calculations revealed that the presence of Li and O vacancies on the rough poriferous core significantly lowered the diffusion energy barrier to improve CO<ce:inf loc=\"post\">2</ce:inf> adsorption capacity. Besides, the dense shell prevented the structure from collapsing. In generally, the core-shell grained Li<ce:inf loc=\"post\">4</ce:inf>SiO<ce:inf loc=\"post\">4</ce:inf> pebbles by solidification of suspension, as an efficient CO<ce:inf loc=\"post\">2</ce:inf> ceramic adsorbent, will have great application potential in the field of high-temperature CO<ce:inf loc=\"post\">2</ce:inf> adsorption.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"119 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153173","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}
引用次数: 0
Tailoring electronic and interfacial synergy in Cu-FeGa/Al2O3 for direct CO2 hydrogenation to ethanol Cu-FeGa/Al2O3中的电子和界面协同作用直接将CO2加氢成乙醇
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-10 DOI: 10.1016/j.cej.2026.173969
Shiquan Huang, Ling Fang, Siling Luo, Hao Deng, Tomas Ramirez Reina, Guangting Zou, Qing Liu, Rongbin Zhang, Maohong Fan, Jinshu Tian, Gang Feng, Runping Ye
Chemical CO2 recycling via direct CO2 hydrogenation to ethanol represents a forward-looking route to curb greenhouse gases emissions while simultaneously alleviating the pressure from fossil fuel extraction and consumption. However, this is a complex chemical process whose successful implementation requires a careful trade-off among its key reaction steps: CO2 activation, selective CC coupling, and hydrogenation termination. Achieving optimal ethanol synthesis requires a balance of surface intermediates and promoting CC coupling, as indicated by thermodynamic and kinetic constraints. Herein, we have developed an efficient FeGa-doped Cu/Al2O3 catalyst prepared by the sol-gel method, achieving a space-time yield of 1.48 mmol·gcat−1·h−1 for ethanol. The Al2O3 support could disperse Cu active sites and generate oxygen vacancies for CO2 activation. Furthermore, Fe doping and Ga modification synergistically enhance both CC coupling capability and the non-dissociative CO activation ability of the Cu/Al2O3 catalyst, ultimately boosting CO2 conversion to ethanol. In-situ DRIFTS spectra reveal a potential catalytic mechanism for ethanol formation: CHx species couple with non-dissociated CO at the Cu-FeGaOx interface, followed by hydrogenation to ethanol. Overall, this work proposes a dual-promoter strategy that incorporates both Fe and Ga in a multi-competent Cu-based formulation, offering a novel approach to designing tunable catalysts for low-carbon ethanol synthesis.
通过直接将二氧化碳加氢转化为乙醇来回收化学二氧化碳,这是一条具有前瞻性的途径,既能抑制温室气体排放,又能减轻化石燃料开采和消耗带来的压力。然而,这是一个复杂的化学过程,其成功实施需要在其关键反应步骤之间进行谨慎的权衡:CO2活化,选择性CC偶联和氢化终止。如热力学和动力学约束所示,实现最佳的乙醇合成需要表面中间体的平衡和促进CC耦合。本文采用溶胶-凝胶法制备了fega掺杂Cu/Al2O3催化剂,对乙醇的时空产率为1.48 mmol·gcat−1·h−1。Al2O3载体可以分散Cu的活性位点,并产生氧空位进行CO2活化。此外,Fe掺杂和Ga修饰协同增强了Cu/Al2O3催化剂的CC偶联能力和非解离CO活化能力,最终促进了CO2转化为乙醇。原位漂移光谱揭示了乙醇形成的潜在催化机制:CHx与未解离的CO在Cu-FeGaOx界面偶联,然后加氢成乙醇。总的来说,这项工作提出了一种双启动子策略,将Fe和Ga结合在多活性cu基配方中,为设计低碳乙醇合成的可调催化剂提供了一种新方法。
{"title":"Tailoring electronic and interfacial synergy in Cu-FeGa/Al2O3 for direct CO2 hydrogenation to ethanol","authors":"Shiquan Huang, Ling Fang, Siling Luo, Hao Deng, Tomas Ramirez Reina, Guangting Zou, Qing Liu, Rongbin Zhang, Maohong Fan, Jinshu Tian, Gang Feng, Runping Ye","doi":"10.1016/j.cej.2026.173969","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173969","url":null,"abstract":"Chemical CO<ce:inf loc=\"post\">2</ce:inf> recycling via direct CO<ce:inf loc=\"post\">2</ce:inf> hydrogenation to ethanol represents a forward-looking route to curb greenhouse gases emissions while simultaneously alleviating the pressure from fossil fuel extraction and consumption. However, this is a complex chemical process whose successful implementation requires a careful trade-off among its key reaction steps: CO<ce:inf loc=\"post\">2</ce:inf> activation, selective C<ce:glyph name=\"sbnd\"></ce:glyph>C coupling, and hydrogenation termination. Achieving optimal ethanol synthesis requires a balance of surface intermediates and promoting C<ce:glyph name=\"sbnd\"></ce:glyph>C coupling, as indicated by thermodynamic and kinetic constraints. Herein, we have developed an efficient FeGa-doped Cu/Al<ce:inf loc=\"post\">2</ce:inf>O<ce:inf loc=\"post\">3</ce:inf> catalyst prepared by the sol-gel method, achieving a space-time yield of 1.48 mmol·g<ce:inf loc=\"post\">cat</ce:inf><ce:sup loc=\"post\">−1</ce:sup>·h<ce:sup loc=\"post\">−1</ce:sup> for ethanol. The Al<ce:inf loc=\"post\">2</ce:inf>O<ce:inf loc=\"post\">3</ce:inf> support could disperse Cu active sites and generate oxygen vacancies for CO<ce:inf loc=\"post\">2</ce:inf> activation. Furthermore, Fe doping and Ga modification synergistically enhance both C<ce:glyph name=\"sbnd\"></ce:glyph>C coupling capability and the non-dissociative CO activation ability of the Cu/Al<ce:inf loc=\"post\">2</ce:inf>O<ce:inf loc=\"post\">3</ce:inf> catalyst, ultimately boosting CO<ce:inf loc=\"post\">2</ce:inf> conversion to ethanol. In-situ DRIFTS spectra reveal a potential catalytic mechanism for ethanol formation: CH<ce:inf loc=\"post\">x</ce:inf><ce:sup loc=\"post\">⁎</ce:sup> species couple with non-dissociated CO<ce:sup loc=\"post\">⁎</ce:sup> at the Cu-FeGaO<ce:inf loc=\"post\">x</ce:inf> interface, followed by hydrogenation to ethanol. Overall, this work proposes a dual-promoter strategy that incorporates both Fe and Ga in a multi-competent Cu-based formulation, offering a novel approach to designing tunable catalysts for low-carbon ethanol synthesis.","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":"146153181","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}
引用次数: 0
Fluorinated dynamic imine-based porous materials with excellent hydrophobicity and closed-loop recycling 具有优异疏水性和闭环回收的氟化动态亚胺基多孔材料
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-10 DOI: 10.1016/j.cej.2026.173959
Wei Hong, Ping Yu, Haiyue Wang, Changyi You, Hongfei He, Hongying Qiu, Ruiqiang Ding, Guanxiang Ma, Bin Yu
{"title":"Fluorinated dynamic imine-based porous materials with excellent hydrophobicity and closed-loop recycling","authors":"Wei Hong, Ping Yu, Haiyue Wang, Changyi You, Hongfei He, Hongying Qiu, Ruiqiang Ding, Guanxiang Ma, Bin Yu","doi":"10.1016/j.cej.2026.173959","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173959","url":null,"abstract":"","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"99 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153188","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}
引用次数: 0
Synergistic integration of oil-mediated adhesion and post-crosslinking imprinting technology for surface imprinted polymers to precision separation of 2′-deoxyadenosine 表面印迹聚合物的油介导黏附和后交联印迹技术协同集成以精确分离2 ' -脱氧腺苷
IF 15.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Pub Date : 2026-02-10 DOI: 10.1016/j.cej.2026.173960
Zhuangxin Wei, Tao Wang, Pan Wang, Jianming Pan
{"title":"Synergistic integration of oil-mediated adhesion and post-crosslinking imprinting technology for surface imprinted polymers to precision separation of 2′-deoxyadenosine","authors":"Zhuangxin Wei, Tao Wang, Pan Wang, Jianming Pan","doi":"10.1016/j.cej.2026.173960","DOIUrl":"https://doi.org/10.1016/j.cej.2026.173960","url":null,"abstract":"","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"16 1","pages":""},"PeriodicalIF":15.1,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146153193","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}
引用次数: 0
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