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Hydrogenation of CO2 to Methanol over Amine-Doped Ordered Mesoporous Polymers Under Dynamic Reaction Conditions 动态反应条件下胺掺杂有序介孔聚合物上CO2加氢制甲醇的研究
IF 3.9 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-11-16 DOI: 10.1002/cctc.202501297
Huidong Xu, Dr. Stephan Bartling, Prof. Dr. Evgenii V. Kondratenko, Prof. Dr. Andreas Jentys

A one-step method was developed to synthesize highly ordered, primary amine–functionalized two-dimensional (2D) hexagonal mesoporous polymers, designed to enhance the density of catalytically active sites for CO2 capture and subsequent hydrogenation to methanol. Incorporation of Pt nanoparticles generates an ordered bifunctional (base/metal) mesoporous system, enabling efficient CO2 adsorption and optimal metal utilization for effective methanol synthesis from the captured CO2 at the amine–metal interface. Compared with silica-based materials,[1,2] this novel polymer achieves a fourfold increase in methanol yield while maintaining 100% selectivity under mild reaction conditions.

采用一步法合成了高度有序的、伯胺功能化的二维(2D)六方介孔聚合物,旨在提高二氧化碳捕获和随后加氢制甲醇的催化活性位点的密度。Pt纳米颗粒的加入产生了有序的双功能(碱/金属)介孔体系,实现了高效的CO2吸附和最佳的金属利用,从而在胺-金属界面上从捕获的CO2中有效合成甲醇。与硅基材料相比[1,2],在温和的反应条件下,这种新型聚合物在保持100%选择性的同时,甲醇收率提高了4倍。
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引用次数: 0
Heteronuclear Dual-Atom Anchored g-C3N4: p-d Orbital Coupling Enable Efficient Urea Electrosynthesis from Gaseous Pollutants 异核双原子锚定g-C3N4: p-d轨道偶联实现气态污染物的高效尿素电合成
IF 3.9 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-11-14 DOI: 10.1002/cctc.202501449
Md Tarikal Nasir, Qingchao Fang, Xin Mao, Dimuthu Wijethunge, Xiuwen Zhou, Aijun Du

Electrocatalytic C–N coupling using gaseous pollutants NO and CO offers a promising alternative to conventional industrial urea synthesis. However, designing efficient electrocatalysts remains challenging due to the complexity of multi-step reactions, which yield diverse products. Herein, based on density functional theory (DFT) calculations, we explore Cu and p-block atoms (B, Al, and Ga) anchored on graphitic carbon nitride as novel heteronuclear double-atom catalysts (DACs) for urea synthesis from NO and CO. The reactants are stably adsorbed on the DACs, while strong dp orbital hybridization facilitates effective activation and efficient C–N coupling. Among the candidates, CuB@g-C3N4 and CuGa@g-C3N4 exhibit particularly promising performance, with limiting potentials of −0.55 V and −0.36 V, respectively. Furthermore, these catalysts significantly suppress competing reactions, including the hydrogen evolution reaction (HER) and the formation of *NOH, *COH, and *CHO intermediates, ensuring high selectivity. Our work not only highlights highly efficient p-d DACs for electrocatalytic urea production but also provides a theoretical framework in catalyst design.

电催化C-N偶联利用气态污染物NO和CO提供了一个有前途的替代传统工业尿素合成。然而,由于多步反应的复杂性,产生不同的产物,设计高效的电催化剂仍然具有挑战性。本文基于密度泛函理论(DFT)计算,研究了锚定在石墨氮化碳上的Cu和p嵌段原子(B、Al和Ga)作为新型异核双原子催化剂(DACs),用于NO和CO合成尿素。反应物稳定吸附在DACs上,而强d-p轨道杂化有利于有效活化和高效的C-N偶联。在候选材料中,CuB@g-C3N4和CuGa@g-C3N4表现出特别有前景的性能,其极限电位分别为- 0.55 V和- 0.36 V。此外,这些催化剂显著抑制竞争反应,包括析氢反应(HER)和*NOH、*COH和*CHO中间体的形成,确保了高选择性。我们的工作不仅强调了高效的p-d dac用于电催化尿素生产,而且为催化剂设计提供了理论框架。
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引用次数: 0
Synergistic Hydrogen-Bonding and CO2 Activation: A Sustainable Metal, Halogen, and Solvent-Free Strategy for CO2 Cycloaddition 协同氢键和CO2活化:一个可持续的金属、卤素和无溶剂的CO2环加成策略
IF 3.9 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-11-12 DOI: 10.1002/cctc.202501611
Biplop Jyoti Hazarika, Khushboo S Paliwal, Antarip Mitra, Pratyay Pan, Aditi Chandrasekar, Venkataramanan Mahalingam

Conventional catalytic methodologies for the cycloaddition of CO2 into epoxides predominantly rely on transition metal-based catalysts in conjunction with detrimental halide-containing cocatalysts. Thus, developing metal and halide-free catalysts that function under ambient conditions is highly desirable. The current research endeavours to synthesize a pyrimidine-based bifunctional organocatalyst via a facile one-step Schiff-base condensation reaction. The synthesized organocatalyst efficiently transforms a wide range of epoxides (35 different epoxides, including 6 challenging internal epoxides) into cyclic carbonates with a minimal catalyst loading of just 0.1 mol% under mild conditions (60 °C–100 °C, atmospheric CO2 pressure) without solvents and cocatalysts. Comprehensive experimental investigations elucidate how the catalyst facilitates the reaction, emphasizing the intricate interplay of hydrogen (H) bonding, spatial arrangement, and catalyst-substrate interactions. The meticulous analysis, using advanced spectroscopic techniques and density functional theory (DFT) calculations, reveals that hydroxyl groups play a pivotal role in epoxide activation through H-bonding interactions, whereas the imine nitrogen facilitates CO2 activation through the formation of a carbamate intermediate. These two interactions collectively accelerate the overall catalytic process. Furthermore, the catalyst exhibits remarkable recyclability over six consecutive catalytic cycles. Therefore, this study underscores the potential of rationally designed metal-free catalysts in advancing sustainable catalysis through carbon capture and utilization technologies.

二氧化碳环加成成环氧化物的传统催化方法主要依赖于过渡金属基催化剂和有害的含卤化物助催化剂。因此,开发在环境条件下起作用的无金属和无卤化物催化剂是非常需要的。目前的研究是通过简单的一步希夫碱缩合反应合成一种基于嘧啶的双功能有机催化剂。合成的有机催化剂在温和条件下(60°C - 100°C,大气CO2压力),无溶剂和助催化剂,催化剂负载仅为0.1 mol%,有效地将各种环氧化合物(35种不同的环氧化合物,包括6种具有挑战性的内部环氧化合物)转化为环状碳酸盐。全面的实验研究阐明了催化剂如何促进反应,强调了氢(H)键、空间排列和催化剂-底物相互作用的复杂相互作用。细致的分析,使用先进的光谱技术和密度泛函理论(DFT)计算,揭示了羟基通过氢键相互作用在环氧化物活化中起关键作用,而亚胺氮通过形成氨基甲酸酯中间体促进CO2活化。这两种相互作用共同加速了整个催化过程。此外,该催化剂在连续六个催化循环中表现出显著的可回收性。因此,本研究强调了合理设计无金属催化剂在通过碳捕获和利用技术推进可持续催化方面的潜力。
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引用次数: 0
Spark Ablation Coupled with Powder Aerosolization for the One-Step Preparation of Ru/TiO2 Catalysts for CO2 Methanation 火花烧蚀耦合粉末雾化一步法制备Ru/TiO2 CO2甲烷化催化剂
IF 3.9 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-11-12 DOI: 10.1002/cctc.202501472
Plaifa Hongmanorom, François Devred, Damien P. Debecker

The preparation of powdery heterogeneous catalysts often involves the use of solvents, costly precursors, and thermal treatments in multi-step processes. Herein, we demonstrate the preparation of Ru nanoparticles on TiO2 via spark ablation coupled with powder aerosolization, offering a clean and simple route with minimal waste generation and reduced pre- and post-synthesis processing. The as-prepared Ru/TiO2 catalyst is readily active in CO2 methanation reaction, achieving CH4 formation rate of 0.21 mmolgRu−1s−1 and TOF of 0.11 s−1 at 200 °C, outperforming the corresponding formulation prepared by wetness impregnation followed by calcination. The enhanced performance is attributed to a higher fraction of surface metallic Ru, as spark ablation under inert atmosphere typically yields metallic Ru nanoparticles. Additionally, Ru nanoparticles in the spark-made catalyst are well-distributed over both anatase and rutile TiO2, driven by Brownian motion and van der Waals adhesion. By contrast, Ru/TiO2-WI exhibits preferential Ru layer around rutile TiO2 due to pre-existing RuO2-rutile TiO2 epitaxial interactions formed during calcination. This work highlights a sustainable approach for designing highly active low-temperature CO2 methanation catalysts, with potential versatility for broader catalytic applications.

制备粉状非均相催化剂通常需要使用溶剂、昂贵的前驱体和多步骤的热处理。在此,我们展示了通过火花烧蚀结合粉末雾化在TiO2上制备Ru纳米颗粒,提供了一个清洁和简单的路线,产生的废物最少,减少了合成前和合成后的加工。制备的Ru/TiO2催化剂在CO2甲烷化反应中具有良好的活性,在200℃时CH4的生成速率为0.21 mmolgRu−1s−1,TOF为0.11 s−1,优于湿浸渍焙烧制得的相应配方。由于惰性气氛下的火花烧蚀通常会产生金属Ru纳米颗粒,因此表面金属Ru的比例更高,从而提高了性能。此外,在布朗运动和范德华附着力的驱动下,火花制备催化剂中的Ru纳米颗粒均匀分布在锐钛矿和金红石型TiO2上。相比之下,Ru/TiO2- wi在金红石TiO2周围表现出优先的Ru层,这是由于在煅烧过程中形成的预先存在的ruo2 -金红石TiO2外延相互作用。这项工作强调了设计高活性低温二氧化碳甲烷化催化剂的可持续方法,具有更广泛的催化应用潜力。
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引用次数: 0
Front Cover: Self-Propelling μ-Catbots Targeting On-The-Fly Energy Harvesting (ChemCatChem 21/2025) 封面:瞄准飞行能量收集的自推进μ-Catbots (ChemCatChem 21/2025)
IF 3.9 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-11-11 DOI: 10.1002/cctc.70419
Saurabh Dubey, Sachin Kumar Sharma, Rishabh Kumar, Srijita De, Rahul Deka, Musaddique Mahfuz Ahmed, Omkar S. Deshmukh, Dipankar Bandyopadhyay

The Front Cover shows self-propelling catalytic micro-/nanobots (μ-Catbots) coated with Fe3O4 and Fe nanoparticles, which decompose H2O2 to O2 and HCOOH to H2, thus enabling real-time fuel cell powering. Magnetic control allows propulsion, bubble demixing, and easy retrieval. Image-based bubble analysis correlates with L–H kinetics, offering a novel approach for reaction rate evaluation and portable oxygen concentrators. More information can be found in the Research Article by D. Bandyopadhyay and co-workers (DOI: 10.1002/cctc.202500767).

前封面展示了包裹有Fe3O4和Fe纳米颗粒的自推进催化微纳米机器人(μ-Catbots),它们将H2O2分解为O2,将HCOOH分解为H2,从而实现实时燃料电池供电。磁控制允许推进,气泡脱混,并易于检索。基于图像的气泡分析与L-H动力学相关,为反应速率评估和便携式氧气浓缩器提供了一种新的方法。更多信息可以在D. Bandyopadhyay及其同事的研究文章中找到(DOI: 10.1002/ cccc .202500767)。
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引用次数: 0
Molybdenum Carbide Electro-Converted from CO2 and MoO3 for Hydrogen Evolution Reaction 由CO2和MoO3电转化碳化钼的析氢反应
IF 3.9 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-11-11 DOI: 10.1002/cctc.202501320
Yixin Wang, Yonghui Song, Yunfei Chen, Ning Yin, Yuan Zhang, Shilei Lang, Zeyu Wang, Chenyang Wang

Molybdenum carbide (MoC/Mo2C), due to its unique noble-like metallic electronic structure, high conductivity, and abundant surface-active sites, exhibits promising catalytic performance for the hydrogen evolution reaction (HER). The directional and controllable synthesis of molybdenum carbide with specific phase composition is crucial for enhancing catalytic performance. This study employs a green and clean electrochemical method to achieve one-step controllable synthesis of a dual-phase MoC–Mo2C in molten salt. The electrolytic mechanism analysis reveals that MoO3 reacts with molten salt components to form soluble molybdate. Subsequently, CO32− and MoO42− as the electroactive ions are co-reduced, and then molybdenum carbide is in situ formatted at the cathode. By controlling the electrolysis temperature, the phase composition and morphology of molybdenum carbide are effectively regulated, yielding a feather-like dual-phase MoC–Mo2C catalyst. In a 1.0 M KOH solution, the dual-phase MoC–Mo2C catalyst exhibits a superior HER activity. The low overpotential is only 118 mV at a current density of 10 mA cm−2 for HER. Furthermore, it exhibits excellent stability, with only a 34 mV overpotential increase at 10 mA cm−2 after 30 h. This study provides a novel strategy for the clean and resource-efficient utilization of CO2 to synthesize molybdenum carbide catalysts for high performance.

碳化钼(MoC/Mo2C)由于其独特的类贵金属电子结构、高导电性和丰富的表面活性位点,在析氢反应(HER)中表现出良好的催化性能。定向可控合成具有特定相组成的碳化钼是提高催化性能的关键。本研究采用绿色清洁的电化学方法,在熔盐中一步可控合成双相MoC-Mo2C。电解机理分析表明,MoO3与熔盐组分反应生成可溶钼酸盐。随后,CO32−和MoO42−作为电活性离子被共还原,碳化钼在阴极原位成形。通过控制电解温度,可以有效调节碳化钼的相组成和形貌,制备出羽毛状的MoC-Mo2C双相催化剂。在1.0 M KOH溶液中,MoC-Mo2C双相催化剂表现出优异的HER活性。在电流密度为10 mA cm−2时,HER的低过电位仅为118 mV。在10 mA cm−2条件下,30 h后过电位仅增加34 mV。该研究为清洁高效利用CO2合成高性能碳化钼催化剂提供了一种新策略。
{"title":"Molybdenum Carbide Electro-Converted from CO2 and MoO3 for Hydrogen Evolution Reaction","authors":"Yixin Wang,&nbsp;Yonghui Song,&nbsp;Yunfei Chen,&nbsp;Ning Yin,&nbsp;Yuan Zhang,&nbsp;Shilei Lang,&nbsp;Zeyu Wang,&nbsp;Chenyang Wang","doi":"10.1002/cctc.202501320","DOIUrl":"https://doi.org/10.1002/cctc.202501320","url":null,"abstract":"<p>Molybdenum carbide (MoC/Mo<sub>2</sub>C), due to its unique noble-like metallic electronic structure, high conductivity, and abundant surface-active sites, exhibits promising catalytic performance for the hydrogen evolution reaction (HER). The directional and controllable synthesis of molybdenum carbide with specific phase composition is crucial for enhancing catalytic performance. This study employs a green and clean electrochemical method to achieve one-step controllable synthesis of a dual-phase MoC–Mo<sub>2</sub>C in molten salt. The electrolytic mechanism analysis reveals that MoO<sub>3</sub> reacts with molten salt components to form soluble molybdate. Subsequently, CO<sub>3</sub><sup>2−</sup> and MoO<sub>4</sub><sup>2−</sup> as the electroactive ions are co-reduced, and then molybdenum carbide is in situ formatted at the cathode. By controlling the electrolysis temperature, the phase composition and morphology of molybdenum carbide are effectively regulated, yielding a feather-like dual-phase MoC–Mo<sub>2</sub>C catalyst. In a 1.0 M KOH solution, the dual-phase MoC–Mo<sub>2</sub>C catalyst exhibits a superior HER activity. The low overpotential is only 118 mV at a current density of 10 mA cm<sup>−2</sup> for HER. Furthermore, it exhibits excellent stability, with only a 34 mV overpotential increase at 10 mA cm<sup>−2</sup> after 30 h. This study provides a novel strategy for the clean and resource-efficient utilization of CO<sub>2</sub> to synthesize molybdenum carbide catalysts for high performance.</p>","PeriodicalId":141,"journal":{"name":"ChemCatChem","volume":"17 24","pages":""},"PeriodicalIF":3.9,"publicationDate":"2025-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145792395","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Cover Feature: Sustainable CO2 Fixation into Cyclic Carbonates via NiO–CuO–ZnO Heterogenous Catalyst at Ambient Temperature (ChemCatChem 21/2025) 封面专题:室温下通过NiO-CuO-ZnO多相催化剂将CO2持续固定为环状碳酸盐(ChemCatChem 21/2025)
IF 3.9 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-11-11 DOI: 10.1002/cctc.70418

The Cover Feature shows a sustainable, solvent-free route for CO2 utilization using a trimetallic NiO–CuO–ZnO catalyst, enabling room-temperature conversion of epichlorohydrin to chloropropene carbonate with 80% yield. This energy-efficient, scalable process avoids precious metals, supports green chemistry, and advances circular carbon economy pathways. More information can be found in the Research Article by J. Rajalakshmi, D. Rajagopal, and A. S. Kumar (DOI: 10.1002/cctc.202500934).

Cover Feature展示了一种可持续的、无溶剂的CO2利用途径,使用三金属NiO-CuO-ZnO催化剂,可以在室温下将环氧氯丙烷转化为碳酸氯丙烯,收率为80%。这种节能、可扩展的工艺避免了贵金属,支持绿色化学,并推进了循环碳经济途径。更多信息可以在J. Rajalakshmi, D. Rajagopal和A. S. Kumar的研究文章中找到(DOI: 10.1002/ cccc .202500934)。
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引用次数: 0
Self-Supported Ru-CoFe Prussian Blue Analogues for Selective and Scalable Electrooxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic Acid 自支撑Ru-CoFe普鲁士蓝类似物选择性和可扩展电氧化5-羟甲基糠醛为2,5-呋喃二羧酸
IF 3.9 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-11-11 DOI: 10.1002/cctc.202501428
Yiqin Zhao, Yiwei Hong, Zhichen Liu, Bowen Zhang, Cejun Hu, Hongwei Zhang, Pei Yuan

The electrochemical upgrading of biomass-derived 5-hydroxymethylfurfural (HMF) into 2,5-furandicarboxylic acid (FDCA) represents a promising route for producing renewable monomers for biodegradable plastics. However, achieving high conversion and selectivity under industrially relevant conditions remains challenging due to sluggish kinetics and catalyst instability. Herein, we report the rational design of a Ru-doped CoFe Prussian blue analogue (Ru-CoFe PBA) catalyst directly grown on copper foam via a one-step hydrothermal process. Comprehensive structural and electronic characterizations reveal that Ru incorporation induces an electron-deficient state in Co and Fe centers, thereby facilitating the formation of hydroxide species and enhancing HMF adsorption. As a result, the Ru-CoFe PBA/CF electrode exhibits outstanding electrocatalytic activity for HMF oxidation, achieving 100% conversion, 98.9% FDCA selectivity, and 97% Faradaic efficiency in 1 M KOH with 100 mM HMF, along with excellent cycling stability. Furthermore, deployment in a multi-stage continuous flow reactor enables high HMF conversion and FDCA selectivity under a broad range of operational parameters, maintaining stable performance over 150 h of continuous operation. This work highlights the synergistic benefits of heteroatom engineering and flow reactor design, offering a scalable platform for efficient biomass electrooxidation to value-added chemicals.

生物质衍生的5-羟甲基糠醛(HMF)电化学升级为2,5-呋喃二羧酸(FDCA)是生产生物降解塑料可再生单体的一条有前途的途径。然而,由于动力学缓慢和催化剂不稳定,在工业相关条件下实现高转化率和选择性仍然具有挑战性。在此,我们报告了通过一步水热法直接在泡沫铜上生长的ru掺杂CoFe普鲁士蓝类似物(Ru-CoFe PBA)催化剂的合理设计。综合结构和电子表征表明,Ru的掺入导致Co和Fe中心的缺电子态,从而促进氢氧化物的形成,增强HMF的吸附。结果表明,Ru-CoFe PBA/CF电极对HMF氧化表现出优异的电催化活性,在1 M KOH和100 mM HMF条件下,转化率为100%,FDCA选择性为98.9%,法拉第效率为97%,并且具有良好的循环稳定性。此外,在多级连续流反应器中部署可以在广泛的操作参数范围内实现高HMF转化率和FDCA选择性,在连续运行150小时以上保持稳定性能。这项工作强调了杂原子工程和流动反应器设计的协同效益,为高效的生物质电氧化生产增值化学品提供了一个可扩展的平台。
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引用次数: 0
Aryl- and Silyl-Substituted Silyliumylidene Ions in the Hydrosilylation of CO2 二氧化碳硅氢化反应中芳基和硅基取代的硅柳基离子
IF 3.9 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-11-09 DOI: 10.1002/cctc.202501195
Sebastian Stigler, Dr. Thaddäus Thorwart, Prof. Dr. Lutz Greb, Prof. Dr. Shigeyoshi Inoue

Tetryliumylidene ions, stabilized by N-heterocyclic carbenes (NHCs), have emerged as promising main-group catalysts for the reduction of carbon dioxide (CO2). Herein, we report the catalytic activity of aryl- and silyl-substituted silyliumylidenes (1 - 4) in the hydrosilylation of CO2 with diphenylsilane at room temperature, using acetonitrile as solvent. With a low catalyst loading of 5 mol%, full conversion of diphenylsilane was achieved within a moderate reaction time, yielding a mixture of silylformate, bis(silyl)acetal, and silylated methanol. Mechanistic studies, supported by nuclear magnetic resonance (NMR) spectroscopy and density functional theory (DFT) calculations, suggest that the silyliumylidene ions act as precatalysts, forming sila-acylium ion intermediates that subsequently generate the catalytically active siloxy-silylene species. These findings highlight the potential of NHC-stabilized silyliumylidene ions as efficient and selective main-group catalysts for CO2 hydrosilylation.

n-杂环羰基(NHCs)稳定的四柳基二烯离子已成为催化二氧化碳还原的主基团催化剂。在此,我们报道了芳基和硅基取代的硅基酰基(1 - 4)在室温下以乙腈为溶剂催化二氧化碳与二苯硅烷的硅氢化反应的活性。在5摩尔%的低催化剂负载下,二苯基硅烷在适度的反应时间内实现了完全转化,生成了硅甲酸酯、双(硅基)缩醛和硅基化甲醇的混合物。核磁共振(NMR)光谱和密度泛函理论(DFT)计算支持的机理研究表明,硅柳基二烯离子作为预催化剂,形成硅-酰基离子中间体,随后产生催化活性的硅氧基硅烯。这些发现突出了nhc稳定的水飞蓟烷离子作为CO2氢硅氧烷化的高效和选择性主基团催化剂的潜力。
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引用次数: 0
Precipitate Washing Level as a Key Parameter of Ni-Al-LDH Catalyst Properties for CO2 Methanation 沉淀物洗涤度是Ni-Al-LDH催化剂CO2甲烷化性能的关键参数
IF 3.9 3区 化学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2025-11-09 DOI: 10.1002/cctc.202501350
Nailma J. Martins, Oscar W. Perez-Lopez

This study investigates the influence of the washing step on the physicochemical properties and catalytic performance of Ni–Al layered double hydroxide (LDH)-derived catalysts for CO2 methanation. Catalysts were synthesized via co-precipitation and subjected to different washing levels, resulting in final conductivities ranging from 21000 µS/cm (0 W) to < 50 µS/cm (10 W). Nitrogen physisorption and X-ray diffraction analyses revealed that lower conductivity values led to increased surface area, reduced crystallite size, and improved structural homogeneity. H2-TPR and CO2-TPD profiles demonstrated that efficient washing enhances metal–support interactions and promotes the formation of stronger basic sites, both of which are critical for CO2 activation. Catalytic tests showed that the 2 W sample washed to an intermediary level exhibited the highest CO2 conversion at low temperatures (200–300 °C), whereas more thoroughly washed samples (10 W and 5 W) performed better at higher temperatures (>300 °C), likely due to their superior thermal stability and resistance to sintering. Post-reaction XRD and XPS characterization confirmed the structural integrity of the catalysts, with minimal crystallite growth. Furthermore, the 2 W catalyst maintained structural integrity, showed no coke formation, and experienced less than 3% mass loss in TPO after 51 h of reaction, confirming its excellent long-term stability. These findings highlight the importance of controlling washing conditions during synthesis to optimize the redox behavior, basicity, and overall catalytic efficiency of Ni–Al LDH-derived materials for CO2 methanation.

研究了洗涤步骤对Ni-Al层状双氢氧化物(LDH)衍生催化剂的理化性质和催化CO2甲烷化性能的影响。催化剂通过共沉淀法合成,并经过不同洗涤水平,最终电导率从21000µS/cm (0 W)到50µS/cm (10 W)不等。氮物理吸附和x射线衍射分析表明,较低的电导率值导致表面积增加,晶粒尺寸减小,结构均匀性改善。H2-TPR和CO2- tpd分析表明,高效的洗涤增强了金属-载体的相互作用,促进了更强碱性位点的形成,这两者都是二氧化碳活化的关键。催化测试表明,洗涤至中间水平的2 W样品在低温(200-300°C)下表现出最高的CO2转化率,而洗涤更彻底的样品(10 W和5 W)在较高温度(>300°C)下表现更好,可能是由于其优越的热稳定性和抗烧结性。反应后的XRD和XPS表征证实了催化剂的结构完整,晶体生长最小。此外,2w催化剂在反应51 h后保持了结构的完整性,没有形成焦炭,TPO的质量损失小于3%,证实了其良好的长期稳定性。这些发现强调了在合成过程中控制洗涤条件对优化Ni-Al ldh衍生材料的氧化还原行为、碱度和总体催化效率的重要性。
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引用次数: 0
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