Applied Catalysis A: General最新文献_第3页

Synergistic three-in-one photo-synthesis of benzimidazoles and H2O2 by porous N-rich g-C3N4/g-C3N5 isotype heterojunction 富n多孔g-C3N4/g-C3N5异质结协同作用下苯并咪唑与H2O2的三合一光合作用

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-11-20 DOI: 10.1016/j.apcata.2025.120713

Wenjie Tian , Xiongxiong Zeng , Wencong Liu , Lei Mao , Fen Guo , Yang Gui , Lan Yuan

Constructing a dual-functional photoredox system coupling fine-chemical synthesis with hydrogen peroxide (H₂O₂) production provides an intriguing and eco-friendly protocol for advancing sustainable practical applications. Herein, we present a facile one-pot strategy for fabricating a porous N-rich g-C₃N₄/g-C₃N₅ heterojunction (denoted as pN-N₄-N₅) using mixed melamine and 3-amino-1,2,4-triazine as the precursors with NH₄Cl as a penetrant for in-situ structure engineering. The resultant metal-free pN-N₄-N₅ exhibited a remarkable performance of H₂O₂ generation rate of 2.71 mmol g⁻¹ h⁻¹ with simultaneous production of industrially important 2-phenylbenzimidazole (2-BZ) under visible light and open air, along with a yield of 97 % and selectivity of > 99 %, outperforming most of the reported carbon nitride-based reaction systems for single-functional H₂O₂ or 2-BZ synthesis. Extensive characterizations and density functional theory (DFT) studies revealed that such a heterojunction with well-matched band structure, enlarged interlayer space and enriched amino groups on the catalyst surface enables the facilitated spatially oriented charge flow, efficient mass transfer and reactants activation, thus offering an efficient and sustainable platform to furnishing the three-in-one photoredox systems to produce bidirectional valuable products.

构建一个耦合精细化学合成与过氧化氢（H2O2）生产的双功能光氧化还原系统，为推进可持续的实际应用提供了一个有趣且环保的方案。在此，我们提出了一种简单的一锅策略，以混合三聚氰胺和3-氨基-1,2,4-三嗪为前驱体，以NH4Cl为渗透剂，制备多孔富n g-C3N4/g-C3N5异质结（简称pN-N4-N5），用于原位结构工程。得到的无金属pN-N4-N5的H2O2生成速率为2.71 mmol g−1 h−1，在可见光和空气条件下可同时生成工业上重要的2-苯基苯并咪唑（2-BZ），产率为97% %，选择性为 99 %，优于大多数基于氮化碳的单功能H2O2或2-BZ合成体系。广泛的表征和密度泛函数理论（DFT）研究表明，这种异质结具有良好匹配的带结构、扩大的层间空间和丰富的催化剂表面氨基，有利于电荷的空间定向流动、高效的传质和反应物的活化，从而为三合一光氧化还原体系生产双向有价产品提供了一个高效和可持续的平台。

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引用次数: 0

Controllable synthesis of SiO₂-supported cobalt nanocatalysts for selective hydrogenation of dinitriles to primary diamines 二腈选择性加氢制伯胺用二氧化硅负载钴纳米催化剂的可控合成

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-11-19 DOI: 10.1016/j.apcata.2025.120712

Yiheng Cui , Kailin Han , Tingting Ge, Yanxia Zheng, Haofei Huang, Cuncun Zuo, Ming Wang

Powdered Co/SiO₂ catalysts with varying cobalt loadings were prepared via the precipitation method for the selective hydrogenation of 3,3′-(cyclohexylazanediyl)dipropanenitrile (CDP) to produce N ¹ -(3-aminopropyl)-N ¹ -cyclohexylpropane-1,3-diamine (ACD). Compared to nickel-based catalysts, the cobalt-based catalysts exhibited moderate H₂ adsorption energy, which helps to suppress the cleavage of the C-N bond and thereby effectively inhibits the dealkylation reaction of amines, reducing the formation of the by-product N ¹ -cyclohexylpropane-1,3-diamine (CD). Characterization techniques including XRD, FT-IR, SEM, BET, and H₂-TPD confirmed that the catalyst with a 60 wt% cobalt loading possesses the optimal active crystalline phase, achieving 100 % CDP conversion and an 81 % yield of ACD. Furthermore, the introduction of ammonia water serves to neutralize surface acidity and establish a moderate interaction with the Co active sites, thereby reducing the energy barrier for H₂ dissociation. This modification significantly enhances both the hydrogenation activity and selectivity of the cobalt-based powder catalyst; however, excessive ammonia led to over-hydrogenation and increased CD formation. Through systematic optimization of solvent type, reaction temperature, pressure, and time, the optimal process conditions for CDP hydrogenation were determined, and a kinetic model of the reaction was established, providing theoretical and data support for industrial application.

采用沉淀法制备了不同钴载量的Co/ sio2粉末催化剂，对3,3′-（环己基二基）二丙腈（CDP）进行选择性加氢反应，得到N ¹ -（3-氨基丙基）-N ¹ -环己基丙烷-1,3-二胺（ACD）。与镍基催化剂相比，钴基催化剂具有中等的H2吸附能，这有助于抑制C-N键的断裂，从而有效抑制胺的脱烷基反应，减少副产物N ¹ -环己基丙烷-1,3-二胺（CD）的生成。表征技术包括XRD， FT-IR， SEM， BET和H₂-TPD证实，钴负载为60 wt%的催化剂具有最佳的活性晶相，实现了100% %的CDP转化率和81% %的ACD收率。此外，氨水的引入有助于中和表面酸性，并与Co活性位点建立适度的相互作用，从而降低H₂解离的能量屏障。该改性显著提高了钴基粉末催化剂的加氢活性和选择性；然而，过量的氨导致过氢化和CD形成增加。通过对溶剂类型、反应温度、压力、时间等进行系统优化，确定了CDP加氢的最佳工艺条件，并建立了反应动力学模型，为工业应用提供了理论和数据支持。

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引用次数: 0

Carboxyl-induced surface modification of Cu-based catalysts for acetylene semi-hydrogenation 乙炔半加氢cu基催化剂的羧基表面改性研究

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-11-17 DOI: 10.1016/j.apcata.2025.120710

Ao Li , Zilong Zhang , Ruoting Liu , Yuxue Yue , Bolin Wang

The synergy of O-functional groups in the semi-hydrogenation of acetylene is indispensable for reasonably modulating the product distributions and improving the catalyst design. However, distinguishing the interaction between various O-functional groups and quantifying and tuning each functionality is still difficult. In this study, the developed Cu/AC-solvent catalysts promote directional carboxyl groups enrichment by systematically regulating the solvent polarity, ranging from water (H₂O) to tetrahydrofuran (THF). The optimized Cu/AC-THF catalyst demonstrates superior performance over a broad operational range (413–503 K), with a remarkable 6.49-fold improvement compared to Cu/AC-H₂O catalyst. Comprehensive characterization techniques and theoretical calculations show that Cu sites are anchored by carboxyl groups and modified into electron-deficient states through electron transfer. It improved the adsorption of the acetylene and facilitated trapping them on Cu sites, thus boosting performance. This study highlights the influence of carboxyl groups on Cu-based catalysts, providing a universal paradigm for designing Cu-based catalysts in acetylene semi-hydrogenation.

在乙炔半加氢反应中，o官能团的协同作用对于合理调节产物分布和改进催化剂设计是必不可少的。然而，区分各种o官能团之间的相互作用以及量化和调优每个功能仍然很困难。在本研究中，开发的Cu/ ac溶剂催化剂通过系统调节溶剂极性，从水（H2O）到四氢呋喃（THF），促进了羧基的定向富集。优化后的Cu/AC-THF催化剂在较宽的工作范围内（413-503 K）表现出优异的性能，与Cu/AC-H2O催化剂相比，性能提高了6.49倍。综合表征技术和理论计算表明，Cu位点被羧基锚定，并通过电子转移修饰成缺电子态。它改善了对乙炔的吸附，并有助于将其捕获在Cu位点上，从而提高了性能。该研究突出了羧基对cu基催化剂的影响，为设计乙炔半加氢cu基催化剂提供了一个通用的范例。

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引用次数: 0

Esterification of valeric acid and glycerol via various acidic zeolites 不同酸性沸石催化戊酸和甘油酯化反应

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-11-17 DOI: 10.1016/j.apcata.2025.120708

Rawipa Intakul , Phuoc Hoang Ho , Derek Creaser , Oleg Pajalic , Louise Olsson

Biomass-derived green esters can be produced from the esterification of valeric acid and glycerol. In this work, various zeolites (ZSM-5, Y, and BEA) were examined, specifically targeting divalerin and trivalerin esters. A direct link between pore size and esterification performance was not evident. This outcome can be attributed to the combined influence of various characteristics such as acidity, hydrophobicity and mesoporous structure. Among the zeolite types tested, HZSM-5, HY, and HBEA with SiO₂/Al₂O₃ ratios of 87, 88.6, and 45.2, respectively, showed the best performance. The Y-zeolite with a SiO₂/Al₂O₃ atomic ratio of 88.6 produced the lowest amount of by-products. This sample had a combination of low acidity (indicating high hydrophobicity), the highest mesoporous area and a relatively high mesoporous volume. These balanced properties rendered Y zeolite with active acid sites that were easily accessible, and facilitated effective pore diffusion properties for both the reactants and products during the esterification of glycerol and valeric acid. This zeolite achieved complete glycerol conversion and a 52.9 % yield of divalerin and a 25 % of trivalerin at 130 °C after 6 h, using 1 wt% catalyst, a 5:1 acid-to-glycerol mole ratio, and continuous water removal. Additionally, the reusability of the zeolite was demonstrated, as the Y zeolite could be recycled four times with only a minimal decrease in glycerol conversion. Complete regeneration of the zeolite was also achieved through re-calcination. This study demonstrates that acidic commercial zeolites are a promising option for esterification processes due to their good catalytic performance, long-term stability and easy regeneration.

由戊酸和甘油的酯化反应可生产生物质衍生的绿酯。在这项工作中，研究了各种沸石（ZSM-5， Y和BEA），专门针对二缬草素和三缬草素酯。孔径大小与酯化性能之间的直接联系并不明显。这一结果可归因于酸度、疏水性和介孔结构等多种特性的综合影响。其中，SiO2/Al2O3比分别为87、88.6和45.2的HZSM-5、HY和HBEA分子筛性能最好。SiO2/Al2O3原子比为88.6的y型分子筛副产物量最少。该样品具有低酸度（表明高疏水性），最高介孔面积和相对较高的介孔体积的组合。这些平衡的性质使得Y沸石具有易于接近的活性酸位点，并且在甘油和戊酸酯化过程中促进了反应物和产物的有效孔隙扩散特性。该分子筛使用1 wt%的催化剂，酸与甘油摩尔比为5:1，连续脱水，在130°C下，6 h后，甘油完全转化，二缬草素的收率为52.9% %，三缬草素的收率为25% %。此外，沸石的可重复使用性也得到了证明，因为Y型沸石可以循环使用四次，而甘油转化率只有很小的降低。通过再煅烧也实现了沸石的完全再生。该研究表明，酸性工业沸石具有良好的催化性能、长期稳定性和易于再生等优点，是酯化反应的理想选择。

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引用次数: 0

Kinetic modeling of the combined HCHO/SCR reaction on V2O5/WO3/TiO2 catalyst in lean exhaust gas of stationary gas engines 固定式燃气发动机稀废气中V2O5/WO3/TiO2催化剂上HCHO/SCR联合反应动力学建模

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-11-17 DOI: 10.1016/j.apcata.2025.120709

Christoph Hahn, Sven Kureti

For the simultaneous removal of NO_x and HCHO from lean exhaust gas of stationary gas engines, V₂O₅/WO₃/TiO₂ (VWT) catalysts are used. The VWT catalysts oxidize HCHO and convert NO_x according to the selective catalytic reduction (SCR). However, the combined HCHO/SCR conversion leads to the production of HCN, which can subsequently decompose along the VWT catalyst.

In this context, a global kinetic model of the combined HCHO/SCR conversion was developed using a VWT monolith with a V₂O₅ load of 2 %. The model was based on a systematic series of kinetic studies performed in a gradient free loop reactor as well as a plug flow reactor The kinetic model represented a network of 8 reactions consisting of the NH₃ adsorption and desorption, SCR reaction, NH₃ oxidation, HCHO oxidation, HCN formation as well as hydrolysis and oxidation of HCN. The kinetics of the respective reactions was described by Arrhenius-based rate expressions including 19 kinetic parameters. The kinetic parameters were primarily obtained from numerical fitting calculations. The model and the implemented kinetic parameters were finally validated by predicting kinetic experiments.

Moreover, the model was used to simulate the fractions of NO_x, NH₃, HCHO and HCN along the VWT monolith. Using these axial profiles operation temperatures and design of the monolith were evaluated to limit the emissions of a stationary lean-burn gas engine.

为了同时从固定式燃气发动机的稀薄废气中去除NOx和HCHO，使用V₂O₅/WO₃/TiO₂（VWT）催化剂。VWT催化剂通过选择性催化还原（selective catalytic reduction， SCR）作用氧化HCHO并转化NOx。然而，HCHO/SCR联合转化会产生HCN， HCN随后会沿着VWT催化剂分解。在这种情况下，使用VWT单体，V2O5负载为2 %，建立了HCHO/SCR联合转化的全局动力学模型。该模型基于在梯度自由循环反应器和塞流反应器中进行的一系列系统动力学研究，动力学模型代表了8个反应网络，包括NH3吸附和解吸，SCR反应，NH3氧化，HCHO氧化，HCN形成以及HCN的水解和氧化。各反应的动力学用包含19个动力学参数的Arrhenius-based速率表达式来描述。动力学参数主要通过数值拟合计算得到。最后通过预测动力学实验对模型和实现的动力学参数进行了验证。此外，利用该模型模拟了NOx、NH3、HCHO和HCN沿VWT整体的组分。使用这些轴向剖面，评估了运行温度和整体设计，以限制固定稀燃燃气发动机的排放。

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引用次数: 0

Influence of pretreatment conditions and support type on CO oxidation activity of Au–Ni catalysts: Insights from operando DRIFTS 预处理条件和载体类型对Au-Ni催化剂CO氧化活性的影响：来自operando DRIFTS的见解

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-11-17 DOI: 10.1016/j.apcata.2025.120711

Alexis Hellmer , Rubén Mendoza-Cruz , Benjamín Portales-Martínez , Rodolfo Zanella

In this report, operando DRIFTS–MS analyses were applied to determine the influence of thermal pretreatment on the oxidation states and catalytic performance of Au–Ni catalysts supported on TiO₂ or γ-Al₂O₃ during the catalytic CO oxidation reaction over a temperature range of –100 °C to 200 °C, monitoring the real-time evolution of surface-adsorbed intermediates. Operando DRIFTS–MS, XPS, TPR, and STEM–HAADF revealed that support material critically influences catalyst behavior: TiO₂-supported catalysts exhibit enhanced CO conversion compared to those on Al₂O₃. Notably, pre-reduced catalysts on TiO₂ showed an important synergistic effect, primarily through the formation of reactive Au^δ- species resulting from the partial reduction of Au⁰ sites. In contrast, pre-oxidized catalysts maintained a higher fraction of oxidized Au species, correlating with moderate activity. Operando DRIFTS–MS data showed that the incorporation of Ni into the bimetallic nanoparticles prevents the formation of adsorbed bicarbonate species or promotes their conversion into more reactive carbonate and carboxylate species, coinciding with the formation of Au^δ- sites and leading to increased CO₂ production. Al₂O₃-supported catalysts exhibit persistent spectator intermediates, such as formate species, which likely block active sites and slow CO₂ production. These insights underscore the significant roles of metal–support interactions, thermal pretreatment conditions, and bimetallic synergistic effects in catalyst design, providing a rational basis for developing more effective Au–Ni catalysts for low-temperature CO oxidation.

本文采用operando drift - ms分析方法，在-100℃至200℃的温度范围内，测定了热预处理对负载在TiO2或γ-Al2O3上的Au-Ni催化剂在催化CO氧化反应中的氧化态和催化性能的影响，并实时监测了表面吸附中间体的演变。Operando drift - ms、XPS、TPR和STEM-HAADF表明，载体材料对催化剂的行为有重要影响：与Al2O3载体相比，tio2载体催化剂表现出更高的CO转化率。值得注意的是，预还原催化剂在TiO2上表现出重要的协同作用，主要是通过部分还原Au0位点形成活性Auδ-来实现的。相比之下，预氧化催化剂保持了较高比例的氧化金，与中等活性相关。Operando漂移- ms数据表明，在双金属纳米颗粒中掺入Ni可以阻止被吸附的碳酸氢盐的形成或促进其转化为活性更强的碳酸盐和羧酸盐，与Auδ-位点的形成相一致，导致二氧化碳产量增加。al2o3负载的催化剂表现出持久的旁观者中间体，如甲酸盐，可能会阻塞活性位点，减缓二氧化碳的产生。这些发现强调了金属-载体相互作用、热预处理条件和双金属协同效应在催化剂设计中的重要作用，为开发更有效的Au-Ni低温CO氧化催化剂提供了合理的基础。

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引用次数: 0

Experimental and DFT studies on the preparation of boron-doped Pd/Al2O3 foam ceramic-based catalysts for mirabelon intermediates 制备掺硼Pd/Al2O3泡沫陶瓷基mirabelon中间体催化剂的实验和DFT研究

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-11-15 DOI: 10.1016/j.apcata.2025.120704

Fangxu Shi , Fuxin Liang , Yulin Wei , Junyan Wu , Sai Huang , Honglei Wang , Zhi Wang , Guopu Shi

The hydrogenation-catalyzed synthesis of mirabellone, a drug for the treatment of overactive bladder (OAB), faces the challenge of catalytic efficiency and selectivity regulation of its core intermediate. In this study, we propose an innovative strategy for constructing a Pd/B-Al₂O₃ composite catalytic system on a foam ceramic substrate using the impregnation method, and systematically investigate the modulation mechanism of different boron doping ratios on the catalyst's performance. Experimental and density functional theory studies demonstrate that the incorporation of boron synergistically enhances surface adsorption of reaction intermediates, facilitates the efficient reduction of PdO, and precisely modulates the distribution of acidic sites, thereby establishing a catalytic environment more favorable for the selective reduction of nitro groups. This catalyst, characterized by its unique three-dimensional pore structure and the interface synergistic effect resulting from boron modification, enables a uniform distribution of catalytically active centers and enhances the efficiency of reaction mass transfer. Through the optimization of process parameters, the yield of the target product was significantly improved, providing an innovative technological path for the preparation of the key intermediate of mirabilon.

治疗膀胱过动症（OAB）药物mirabellone的氢化催化合成面临催化效率和核心中间体选择性调控的挑战。在本研究中，我们提出了一种创新的策略，利用浸渍法在泡沫陶瓷衬底上构建Pd/B-Al2O3复合催化体系，并系统地研究了不同硼掺杂比例对催化剂性能的调节机理。实验和密度泛函数理论研究表明，硼的加入协同增强了反应中间体的表面吸附，促进了PdO的高效还原，并精确调节了酸性位点的分布，从而建立了更有利于硝基选择性还原的催化环境。该催化剂具有独特的三维孔隙结构和硼改性产生的界面协同效应，使催化活性中心分布均匀，提高了反应传质效率。通过工艺参数的优化，目标产物的收率显著提高，为mirabilon关键中间体的制备提供了一条创新的技术路径。

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引用次数: 0

{FeMo6}@Ru(N^N)3-covalent organic frameworks for enhanced aldehyde photooxidation {FeMo6}@Ru(N^N)3-共价有机骨架增强醛光氧化

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-11-15 DOI: 10.1016/j.apcata.2025.120706

Bi-Ying Wang , Zhan-Xin Zhang , Tao Zhang , Ai-Juan Li , Jing Li , Sheng-Li Huang

An efficient green oxidative synthesis was achieved through the development of a bi-functional {FeMo₆}⊂[Ru(N^N)₃@Q-COF] photocatalyst. This catalyst integrates a Ru(N^N)₃ photosensitizer, a stable quinoline-based covalent organic framework (COF), and Anderson polyoxometalates (POMs) via coordination and electrostatic interactions. The combination enhances light absorption, charge transfer, Lewis acid activity, and substrate enrichment within a confined nano-channel environment. Compared to individual catalytic systems, this integrated catalyst demonstrates superior efficiency and selectivity in the photocatalytic oxidation of aldehydes to carboxylic acids. Moreover, it shows excellent recyclability, making it a promising platform for sustainable and efficient catalytic processes.

通过开发双功能{FeMo6}∧[Ru(N^N)3@Q-COF]光催化剂，实现了高效的绿色氧化合成。该催化剂通过配位和静电相互作用将Ru(N^N)3光敏剂、稳定的喹啉共价有机骨架（COF）和Anderson多金属氧酸盐（pom）集成在一起。这种组合增强了光吸收、电荷转移、路易斯酸活性和在受限纳米通道环境中的底物富集。与单独的催化系统相比，这种集成催化剂在光催化氧化醛制羧酸方面表现出优越的效率和选择性。此外，它具有良好的可回收性，使其成为可持续和高效催化过程的有前途的平台。

引用次数: 0

Co/SiO₂ eggshell catalysts: An efficient and controllable synthesis method Co/ sio2蛋壳催化剂：一种高效可控的合成方法

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-11-15 DOI: 10.1016/j.apcata.2025.120707

Fernanda S. Pimenta, Alexis Godet, Babu Joseph, John N. Kuhn

Eggshell catalysts are characterized by the deposition of the active phase near the outer layer of the pellet, offering advantages for diffusion-limited reactions. In this work, a scalable and reproducible method for synthesizing Co/SiO₂ eggshell catalysts using 2 mm spherical silica pellets is presented. Unlike reported procedures, this method does not require multiple impregnations, the use of a nitrogen glovebox, drying of pellets soaked in non-polar solvent, and the use of viscosifying agents. The influence of contact time in the precursor solution on shell thickness and Co loading was investigated. Shell thicknesses between 0.21 and 0.37 mm were achieved, with standard deviations of 0.02 – 0.06 mm. A cobalt loading of 19.6 wt% (XRF) was obtained in one impregnation step, with average crystallite sizes of 13–16 nm (Scherrer analysis). Fischer–Tropsch Synthesis (230 ℃ and 10 bar) confirmed that shell thickness impacts product selectivity. The catalyst with 0.37 mm shell thickness resulted in higher C₅⁺ selectivity and lower CO₂ and CH₄ formation than catalysts with thinner shells and one with a uniform distribution, which highlights the importance of precision in tuning the shell thickness during synthesis. The catalysis trends with shell thickness are attributed to residence time in the pores and Co particles encountered during the diffusion path, which promotes olefin re-adsorption and chain growth to middle distillates (

C_{10}

-

C_{20})

hydrocarbons while deterring saturation of light hydrocarbons. Overall, the proposed method enables high Co loading with one impregnation and controlled shell thickness with improved reproducibility and scalability.

蛋壳催化剂的特点是活性相沉积在颗粒的外层附近，为限制扩散的反应提供了优势。在这项工作中，提出了一种可扩展和可重复的方法，用于合成Co/ sio2蛋壳催化剂使用2 毫米球形硅球。与报道的方法不同，该方法不需要多次浸渍，使用氮气手套箱，干燥浸泡在非极性溶剂中的颗粒，以及使用增粘剂。研究了前驱体溶液中接触时间对壳体厚度和Co载荷的影响。壳体厚度在0.21 ~ 0.37 mm之间，标准偏差为0.02 ~ 0.06 mm。在一个浸渍步骤中获得了19.6 wt% （XRF）的钴负载，平均晶粒尺寸为13-16 nm （Scherrer分析）。费托合成（230℃，10 bar）证实了壳层厚度影响产物的选择性。壳层厚度为0.37 mm的催化剂比壳层较薄和分布均匀的催化剂具有更高的C₅⁺选择性，更低的CO₂和CH₄生成，这突出了在合成过程中调整壳层厚度精度的重要性。随着壳层厚度的增加，烯烃在孔隙中的停留时间和扩散过程中遇到的Co颗粒会促进烯烃的再吸附和链式生长，形成中间馏分（C10 - C20）烃，同时阻碍轻烃的饱和。总的来说，该方法可以在一次浸渍的情况下实现高Co负载，并控制外壳厚度，提高了可重复性和可扩展性。

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引用次数: 0

Mesoporous alumina-carbon supported copper nanocatalyst for ethanol dehydrogenation: Balancing acidic and metallic properties for optimal performance 用于乙醇脱氢的介孔铝碳负载铜纳米催化剂：平衡酸性和金属性质以获得最佳性能

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General

Pub Date : 2025-11-15 DOI: 10.1016/j.apcata.2025.120705

Yan Hao , Linlin Du , Yang Zhou , Zheng Gao , Yang Zhang , Qinghu Tang

The mesoporous alumina-carbon with the advantages of mesoporous structure and acid-base properties was selected as support, and the copper nanoparticles were prepared by a facile impregnation and subsequent pyrolysis procedure. Well distributed copper nanoparticles were obtained with a mean size of 3 nm due to the mesopore structure and strong metal-support interaction. At an operating temperature of 250 °C, the Cu/Al₂O₃-C catalyst was able to achieve up to 98 % ethanol conversion and an ideal > 99 % selectivity of acetaldehyde, owing to a high Cu active surface, a large (Cu⁰+Cu⁺)/Cu_total ratio, and suitable weak and moderate-strong acid active sites, which were conducive to the ethanol dehydrogenation reaction. By controlling the content of alumina in the support to regulate the acidic properties, the catalyst possessing an optimal weak and moderate-strong acid/total acid ratio of 0.86 was the most favorable for ethanol dehydrogenation. This catalyst also presented good reusability and regeneration ability, providing a good choice for ethanol dehydrogenation.

选择具有介孔结构和酸碱性能优点的介孔铝碳作为载体，采用快速浸渍和后续热解法制备纳米铜。由于介孔结构和强的金属-载体相互作用，获得了均匀分布的铜纳米颗粒，平均尺寸为3 nm。在250 ℃的操作温度下，Cu/Al2O3-C催化剂具有较高的Cu活性表面、较大的(Cu0+Cu+)/Cutotal比和适宜的弱、中强酸活性位点，有利于乙醇脱氢反应，可实现98% %的乙醇转化率和 99% %的乙醛选择性。通过控制载体中氧化铝的含量来调节催化剂的酸性，弱、中强酸/总酸比为0.86的催化剂最有利于乙醇脱氢。该催化剂具有良好的可重复使用性和再生能力，为乙醇脱氢提供了良好的选择。

{"title":"Mesoporous alumina-carbon supported copper nanocatalyst for ethanol dehydrogenation: Balancing acidic and metallic properties for optimal performance","authors":"Yan Hao , Linlin Du , Yang Zhou , Zheng Gao , Yang Zhang , Qinghu Tang","doi":"10.1016/j.apcata.2025.120705","DOIUrl":"10.1016/j.apcata.2025.120705","url":null,"abstract":"<div><div>The mesoporous alumina-carbon with the advantages of mesoporous structure and acid-base properties was selected as support, and the copper nanoparticles were prepared by a facile impregnation and subsequent pyrolysis procedure. Well distributed copper nanoparticles were obtained with a mean size of 3 nm due to the mesopore structure and strong metal-support interaction. At an operating temperature of 250 °C, the Cu/Al<sub>2</sub>O<sub>3</sub>-C catalyst was able to achieve up to 98 % ethanol conversion and an ideal > 99 % selectivity of acetaldehyde, owing to a high Cu active surface, a large (Cu<sup>0</sup>+Cu<sup>+</sup>)/Cu<sub>total</sub> ratio, and suitable weak and moderate-strong acid active sites, which were conducive to the ethanol dehydrogenation reaction. By controlling the content of alumina in the support to regulate the acidic properties, the catalyst possessing an optimal weak and moderate-strong acid/total acid ratio of 0.86 was the most favorable for ethanol dehydrogenation. This catalyst also presented good reusability and regeneration ability, providing a good choice for ethanol dehydrogenation.</div></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":"710 ","pages":"Article 120705"},"PeriodicalIF":4.8,"publicationDate":"2025-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145577513","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

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