Journal of Catalysis最新文献

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Alkanol dehydration and dehydrogenation pathways on anatase TiO2 under oxidative and nonoxidative conditions 氧化和非氧化条件下锐钛矿TiO2的醇脱水和脱氢途径
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-09-10 DOI: 10.1016/j.jcat.2025.116414
Manasi Vyas, Lynsey Patterson, Stephanie Kwon
{"title":"Alkanol dehydration and dehydrogenation pathways on anatase TiO2 under oxidative and nonoxidative conditions","authors":"Manasi Vyas,&nbsp;Lynsey Patterson,&nbsp;Stephanie Kwon","doi":"10.1016/j.jcat.2025.116414","DOIUrl":"10.1016/j.jcat.2025.116414","url":null,"abstract":"<div><div>Alkanol dehydration offers a promising route for converting biomass-derived short-chain oxygenates into alkenes, which are valuable industrial intermediates. Titanium dioxide (TiO<sub>2</sub>) has been extensively studied for this reaction due to its high activity and low cost. However, the inherent heterogeneity of commercially available TiO<sub>2</sub> has led to conflicting reports on reactivity and product selectivity, further complicated by the diverse reaction conditions employed in previous studies. This work aims to update our understanding of alkanol reactions on anatase TiO<sub>2</sub> by integrating transient, titration, kinetic, and spectroscopic methods, using 2-propanol and 1-propanol as model reactants. Under anerobic conditions, 2-propanol primarily undergoes dehydration to form propene and water. A minor pathway forms acetone via nonoxidative dehydrogenation, but only after an induction period during which surface oxygen vacancies accumulate. Notably, propene formation rates remain largely constant, even as acetone formation rates decrease by ∼60 % during the initial induction period. These transient behaviors, together with pretreatment and characterization data, suggest that dehydration predominantly occurs on smaller TiO<sub>2</sub> crystallites that provide most of the surface area, whereas dehydrogenation is favored on larger crystallites with smaller band gap energies. In situ pyridine titration was used to quantify the number of active sites for each pathway, enabling accurate turnover rate normalization. Detailed kinetic analysis showed that both dehydration and nonoxidative dehydrogenation are inhibited by 2-propanol, water, and 2-propanol–water dimers, but to different extents. The rate constant for nonoxidative dehydrogenation reflects a significantly lower activation enthalpy than that for the oxidative route; however, this is offset by a large entropic penalty, resulting in higher free energy barriers at relevant temperatures and thus a lower overall rate constant. This kinetic framework offers mechanistic insight into the temperature- and pressure-dependent shifts in reaction rates and product selectivity, while also reconciling prior discrepancies reported in the literature.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"452 ","pages":"Article 116414"},"PeriodicalIF":6.5,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145043680","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
A tailored polyoxometalate-based metal-organic framework: Boosting photocatalytic Knoevenagel condensation through efficient proton and hydrogen atom transfer 定制的多金属氧酸盐基金属有机框架:通过有效的质子和氢原子转移促进光催化Knoevenagel缩合
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-09-09 DOI: 10.1016/j.jcat.2025.116416
Jie Li , Xueling Liu , Jing Zheng , Fei Li , Yahong Chen , Qiuxia Han
{"title":"A tailored polyoxometalate-based metal-organic framework: Boosting photocatalytic Knoevenagel condensation through efficient proton and hydrogen atom transfer","authors":"Jie Li ,&nbsp;Xueling Liu ,&nbsp;Jing Zheng ,&nbsp;Fei Li ,&nbsp;Yahong Chen ,&nbsp;Qiuxia Han","doi":"10.1016/j.jcat.2025.116416","DOIUrl":"10.1016/j.jcat.2025.116416","url":null,"abstract":"<div><div>The efficient photocatalytic Knoevenagel condensation under mild conditions provides a significant route to obtain α,β-unsaturated carbonyl compounds. Herein, a new polyoxometalate-based metal–organic framework (POMOF), [Co<sub>2</sub>(TPB)<sub>1.5</sub>(CoPW<sub>11</sub>O<sub>39</sub>)∙4H<sub>2</sub>O][Co<sub>0.5</sub>(TPB)<sub>0.5</sub>·5H<sub>2</sub>O]∙14H<sub>2</sub>O (<strong>PW<sub>11</sub>Co-TPB</strong>, TPB = 1,2,4,5-tetra(4-pyridyl)benzene), was synthesized and characterized. <strong>PW<sub>11</sub>Co-TPB</strong> features a three-dimensional (3D) structure by POM and MOF covalently connected into a staircase shape by Co(2) metal sites. Impressively, the plenty of water molecules in the structure construct tight hydrogen-bonding anchoring sites, laying the foundation for good proton conductivity. <strong>PW<sub>11</sub>Co-TPB</strong> exhibits higher thermal and chemical stability, wider light absorption range and lower LUMO energy level. Incorporating POM into photoactive MOF is beneficial to produce •O<sub>2</sub><sup>–</sup> by photogenerated electron transfer, which can abstract hydrogen atoms from substrate cyanoester to form a carbanion, thereby facilitating Knoevenagel condensation. <strong>PW<sub>11</sub>Co-TPB</strong> exhibits a 99 % yield for α,β-unsaturated carbonyl compounds in the Knoevenagel condensation of aldehydes with ethyl cyanoacetate in a methanol/H<sub>2</sub>O solvent system under ambient conditions with 20 W white LED irradiation for 24h.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"452 ","pages":"Article 116416"},"PeriodicalIF":6.5,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145017183","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Engineering Pt-O coordination microenvironment toward an active, durable, and antipoisoning catalyst in CO oxidation 工程Pt-O配位微环境对CO氧化的活性,耐用和抗毒催化剂
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-09-08 DOI: 10.1016/j.jcat.2025.116413
Bao-Ju Wang , Xin Zhang , Wenyao Chen , Hongzi Tan , Hai-Long Liao , Xiangxue Zhang , Dingsheng Wang , Xuezhi Duan , Yong Luo , Jian-Feng Chen
{"title":"Engineering Pt-O coordination microenvironment toward an active, durable, and antipoisoning catalyst in CO oxidation","authors":"Bao-Ju Wang ,&nbsp;Xin Zhang ,&nbsp;Wenyao Chen ,&nbsp;Hongzi Tan ,&nbsp;Hai-Long Liao ,&nbsp;Xiangxue Zhang ,&nbsp;Dingsheng Wang ,&nbsp;Xuezhi Duan ,&nbsp;Yong Luo ,&nbsp;Jian-Feng Chen","doi":"10.1016/j.jcat.2025.116413","DOIUrl":"10.1016/j.jcat.2025.116413","url":null,"abstract":"<div><div>Platinum stands as a leading catalyst for oxidation reactions, with its catalytic performance intricately governed by the fine-tuning of its local coordination environment. In this study, we present an effective Na<sup>+</sup>-decoration strategy to reconstruct the Pt-O coordination microenvironment. Evidenced by experimental characterizations and DFT calculation, the alkali cation of Na<sup>+</sup> stabilizes Pt clusters via the Pt-Na-O interaction. Such decoration promotes electron migration from Ce<sup>3+</sup>-oxygen vacancy to PtO<sub>x</sub> clusters, preserving of a low Pt-O coordination number (CN) even under oxidative conditions. The Na<sup>+</sup>-stabilized Pt sites exhibit a 20-fold enhancement in CO oxidation turnover frequency (TOF = 0.39 s<sup>-1</sup>) compared to Na<sup>+</sup>-free counterparts (TOF = 0.02 s<sup>-1</sup>) at 100 °C, attributable to a lowered apparent activation energy (37 vs. 82 kJ/mol). The Na<sup>+</sup>-decoration also effectively suppresses hydrocarbon adsorption, mitigating hydrocarbon poisoning during CO oxidation. By adopting alkali cations to modulate Pt-O coordination, this strategy may extend to other metals suffering from oxygen overstabilization (e.g., Co/Al<sub>2</sub>O<sub>3</sub>, Fe/TiO<sub>2</sub>), leveraging alkali-induced electron transfer to unlock low M−O coordination.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"452 ","pages":"Article 116413"},"PeriodicalIF":6.5,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009515","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Impact of effective magnetic moment of manganese oxides with different oxidation states on the ortho–para hydrogen conversion at 77 K 不同氧化态锰氧化物的有效磁矩对77 K下邻对氢转化的影响
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-09-08 DOI: 10.1016/j.jcat.2025.116412
Xin Yu , Jiawei Wang , Jin Shen , Yulin Cui , Jianjian Xia , Hong Xu , Shaowei Zhu , Cunman Zhang , Mingzhe Xue
{"title":"Impact of effective magnetic moment of manganese oxides with different oxidation states on the ortho–para hydrogen conversion at 77 K","authors":"Xin Yu ,&nbsp;Jiawei Wang ,&nbsp;Jin Shen ,&nbsp;Yulin Cui ,&nbsp;Jianjian Xia ,&nbsp;Hong Xu ,&nbsp;Shaowei Zhu ,&nbsp;Cunman Zhang ,&nbsp;Mingzhe Xue","doi":"10.1016/j.jcat.2025.116412","DOIUrl":"10.1016/j.jcat.2025.116412","url":null,"abstract":"<div><div>Ortho-para hydrogen conversion (OPHC) is an essential step in liquid hydrogen production and storage. Herein, in order to investigate the impact of effective magnetic moment (μ<sub>eff</sub>) on the catalytic activity of OPHC, a series of manganese oxides (MnOx) at different oxidation states were synthesized using similar hydrothermal methods. The crystal phases, morphologies, chemical compositions, electron spin configurations and magnetic properties of the MnOx catalysts were characterized by XRD, SEM, TEM, XPS, EPR, ZFC, etc. OPHC at 77 K under various volume space velocities (VSV) showed that the catalytic performance of MnOx decreased with increasing Mn oxidation state, following an order of MnO &gt; Mn<sub>3</sub>O<sub>4</sub> &gt; Mn<sub>2</sub>O<sub>3</sub> &gt; MnO<sub>2</sub>. Electron spin configurations and magnetic properties analysis revealed that Mn<sup>2+</sup> in MnO, with the highest number of unpaired electrons (4.73) in the high-energy 3d orbitals, exhibited the largest μ<sub>eff</sub> (5.64 μ<sub>B</sub>). A linear fit of the square of the μ<sub>eff</sub> and the reaction rate constant (k) at different VSV with an average R<sup>2</sup> above 0.98, provides new insights for catalyst design and performance evaluation. Additionally, a simple one-pot synthesis method for supported catalyst was proposed, which eliminates the need for secondary granulation. The obtained MnO/MS catalyst achieved a p-H<sub>2</sub> content of 48.6 % at a VSV of 30,000 h<sup>−1</sup>, with a maximum k of 1.15 × 10<sup>3</sup> mol · L<sup>−1</sup> · s<sup>−1</sup>, which is 1.3 times higher than that of commercial catalyst, offering valuable guidance for development of new preparation method in OPHC applications.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"452 ","pages":"Article 116412"},"PeriodicalIF":6.5,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145017186","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Surface hydroxyl-mediated modulation of γ-Al2O3 to enhance Ni-catalyzed CO2 methanation at low temperatures 表面羟基介导的γ-Al2O3在低温下促进ni催化的CO2甲烷化
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-09-08 DOI: 10.1016/j.jcat.2025.116415
Ziyang Xu, Liang Chen, Chunbo Wang
{"title":"Surface hydroxyl-mediated modulation of γ-Al2O3 to enhance Ni-catalyzed CO2 methanation at low temperatures","authors":"Ziyang Xu,&nbsp;Liang Chen,&nbsp;Chunbo Wang","doi":"10.1016/j.jcat.2025.116415","DOIUrl":"10.1016/j.jcat.2025.116415","url":null,"abstract":"<div><div>Reaching high activity over Ni-based catalysts for CO<sub>2</sub> methanation at lower temperature remains a critical challenge. Herein, a surface hydroxylation strategy was developed to enhance the catalytic performance of Ni catalysts under mild conditions. By treating γ-Al<sub>2</sub>O<sub>3</sub> with H<sub>2</sub>O<sub>2</sub> solutions of varying concentrations, the surface hydroxyl (–OH) group density was effectively tuned. Catalytic evaluations revealed that hydroxylation of the support significantly enhances CO<sub>2</sub> methanation performance. Among the series, Ni/A-OH-6 exhibited the highest activity, achieving a turnover frequency (TOF) of 2.129 h<sup>−1</sup> at 240 °C, approximately eight times higher than that of the unmodified Ni/A catalyst (0.266 h<sup>−1</sup>), thereby demonstrating a remarkable enhancement in intrinsic activity. Comprehensive characterizations demonstrated that surface –OH significantly enhanced CO<sub>2</sub> adsorption via the formation of HCO<sub>3</sub>* species. In situ DRIFTS studies further confirmed that hydroxyl-induced HCO<sub>3</sub>* species convert more readily to HCOO*, facilitating the hydrogenation pathway and thus contributing to the improved low-temperature activity. This work highlights surface hydroxyl engineering as a simple yet effective approach to boost catalytic efficiency, delivering guidance for the rational development of high-efficiency CO<sub>2</sub> utilization catalysts.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"452 ","pages":"Article 116415"},"PeriodicalIF":6.5,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145017187","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Structure-dependent microkinetic modeling of the CO2 desorption with surface diffusion CO2表面扩散解吸的结构依赖微动力学模型
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-09-08 DOI: 10.1016/j.jcat.2025.116407
Bjarne Kreitz , Gandhali Kogekar , Raffaele Cheula , C. Franklin Goldsmith
{"title":"Structure-dependent microkinetic modeling of the CO2 desorption with surface diffusion","authors":"Bjarne Kreitz ,&nbsp;Gandhali Kogekar ,&nbsp;Raffaele Cheula ,&nbsp;C. Franklin Goldsmith","doi":"10.1016/j.jcat.2025.116407","DOIUrl":"10.1016/j.jcat.2025.116407","url":null,"abstract":"<div><div>The interaction of CO<sub>2</sub> with Ni catalysts is important for many industrial processes like methanation, which is known to be structure sensitive. Consequently, structure-dependent multiscale modeling is required to accurately capture the interaction of CO<sub>2</sub> with the various Ni facets and to provide accurate atomistic insights. While mean-field multiscale models can be constructed for multifaceted nanoparticles, surface diffusion of adsorbates between the facets is often not considered. In this study, we close the gap by extending the open-source Cantera toolkit with a universal framework for surface diffusion between facets in mean-field microkinetic models, making it the first widely adopted software tool that includes these features. We leverage these updates to develop a thermodynamically consistent microkinetic model for a Ni nanoparticle consisting of Ni(111), Ni(100), Ni(211), and Ni(110) using data from DFT calculations and single-crystal experiments to unravel the interaction of CO<sub>2</sub> with these facets through the simulation of temperature-programmed desorption profiles. Including surface diffusion and coverage effects into the mean-field microkinetic model leads to a significantly improved agreement between experiments from a <figure><img></figure> catalyst and the simulations. Through rigorous correlated uncertainty quantification of all structural and energetic parameters, we are able to identify a microkinetic model within the uncertainty space that is in excellent agreement with the recorded desorption profile. This model highlights that Ni(110), which contributes only to a small extent to the overall Ni surface area, dominates the desorption pattern and that surface diffusion plays a crucial role. The Cantera implementation is generic and can be applied to other metal nanoparticles and metal/metal oxide interfaces, providing a step towards closing the material gap.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"452 ","pages":"Article 116407"},"PeriodicalIF":6.5,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009516","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Surface oxygen functionalities on carbon supports modulate Pt stabilization for sustainable acetylene hydrochlorination 碳表面氧官能团支持调节铂稳定可持续乙炔氢氯化
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-09-07 DOI: 10.1016/j.jcat.2025.116410
Saisai Wang , Siyu Pei , Tengyun Ma , ZiKang Liu , Jianbo Wu , Chunxiao Jin , Renqin Chang , Yuxue Yue , Zhiyan Pan , Jia Zhao , Xiaonian Li
{"title":"Surface oxygen functionalities on carbon supports modulate Pt stabilization for sustainable acetylene hydrochlorination","authors":"Saisai Wang ,&nbsp;Siyu Pei ,&nbsp;Tengyun Ma ,&nbsp;ZiKang Liu ,&nbsp;Jianbo Wu ,&nbsp;Chunxiao Jin ,&nbsp;Renqin Chang ,&nbsp;Yuxue Yue ,&nbsp;Zhiyan Pan ,&nbsp;Jia Zhao ,&nbsp;Xiaonian Li","doi":"10.1016/j.jcat.2025.116410","DOIUrl":"10.1016/j.jcat.2025.116410","url":null,"abstract":"<div><div>In efforts to replace toxic catalysts in vinyl chloride production, Pt-based catalysts are recognized for their relatively high long-term stability; however, the rapid chlorination reaction of the highly active Pt(II) sites limits their catalytic potential. This study investigates how the surface properties of carbon supports influence the performance and activity of Pt single atoms by controlling these surface characteristics. Through advanced characterization, kinetic analysis, and density functional theory, we elucidate the mechanisms by which the interfacial effects of carbon supports impact catalyst activity and stability. Experimental and mechanistic results indicate that oxygen-deficient, basic supports promote the formation of highly active Pt(II) species, whereas oxygen-rich, acidic supports accelerate chlorination. Additionally, electron-rich oxygen groups on the carbon surface interact with adjacent electron-deficient Pt atoms to form frustrated Lewis acid-base pairs, facilitating the conversion of Pt single atoms from low to high chlorine coordination states, ultimately impairing catalytic performance.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"452 ","pages":"Article 116410"},"PeriodicalIF":6.5,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007214","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Facet-dependent *CO adsorption configuration on sputtered copper catalysts for selective electrocatalytic CO2 reduction to C2 products 溅射铜催化剂的选择性电催化CO2还原到C2产品的CO吸附配置
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-09-07 DOI: 10.1016/j.jcat.2025.116408
Ranran Niu, Hang Xiao, Baorong Xu, Gaoyang Li, Daolin Tan, Bo Lin, Guidong Yang
{"title":"Facet-dependent *CO adsorption configuration on sputtered copper catalysts for selective electrocatalytic CO2 reduction to C2 products","authors":"Ranran Niu,&nbsp;Hang Xiao,&nbsp;Baorong Xu,&nbsp;Gaoyang Li,&nbsp;Daolin Tan,&nbsp;Bo Lin,&nbsp;Guidong Yang","doi":"10.1016/j.jcat.2025.116408","DOIUrl":"10.1016/j.jcat.2025.116408","url":null,"abstract":"<div><div>Electrochemical CO<sub>2</sub> reduction (ECR) provides a sustainable and green strategy for converting CO<sub>2</sub> into valuable chemicals, especially for C<sub>2</sub> products. However, the poor C<sub>2</sub>-product selectivity of catalysts related to substantial activation energy required for C–C coupling severely limits the practical application of ECR. Herein, we systematically investigate the role of crystal facet engineering on modulating the performance of copper-based catalysts, which achieves selective ECR for C<sub>2</sub> products through the regulation of key intermediate adsorption configurations. Density functional theory (DFT) calculations, combined with various characterization methods, indicate that the exposure of specific crystal facets on the copper surface plays a critical role in determining the selectivity of the products. Compared to the *CO top adsorption on Cu (1 1 1), the specific *CO adsorption in the hollow site on the Cu (2 0 0) facet significantly lowers the energy barrier for C–C coupling. As a result, the SCF3 sputtered copper film sample with Cu (1 1 1) and Cu (2 0 0) facets shows a high C<sub>2</sub> product selectivity with a Faradaic efficiency of 70.6 ± 2.0 %, while the SCF1 sample with single Cu (1 1 1) facet shows a Faradaic efficiency of CH<sub>4</sub> at 49.8 ± 2.4 %. This work highlights the key role of facet-modulated *CO adsorption configuration in boosting the ECR performance and the selectivity of C<sub>2</sub> products for Cu-based materials.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"452 ","pages":"Article 116408"},"PeriodicalIF":6.5,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007215","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Upgrading of glycerol to solketal over mesoporous gallosilicates with tuned hydrophobicity 在疏水性调节的介孔无水硅酸盐上将甘油升级为索酮
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-09-07 DOI: 10.1016/j.jcat.2025.116409
Hussein Hussein , Luca Fusaro , Michel Devillers , Carmela Aprile
{"title":"Upgrading of glycerol to solketal over mesoporous gallosilicates with tuned hydrophobicity","authors":"Hussein Hussein ,&nbsp;Luca Fusaro ,&nbsp;Michel Devillers ,&nbsp;Carmela Aprile","doi":"10.1016/j.jcat.2025.116409","DOIUrl":"10.1016/j.jcat.2025.116409","url":null,"abstract":"<div><div>Novel mesoporous gallosilicates with tuned hydrophobicity were synthesized through methylation of extra small XS-SiO<sub>2</sub> silica particle via condensation with trimethoxymethylsilane CH<sub>3</sub>Si(OCH<sub>3</sub>)<sub>3</sub> followed by impregnation with gallium (III) precursors. The structural and textural properties of the solids obtained were extensively characterized by different techniques. The synthesized catalysts displayed excellent catalytic activity in the acetalization of acetone with glycerol to produce solketal. Among all the studied catalysts, the most active catalyst, XS-10 %Me-GaLac, displayed high turnover number and significantly improved glycerol conversion which is attributed to the relatively hydrophobic surface and high amount of accessible active acid sites. The high acidity and enhanced hydrophobicity of this catalyst was generated by the incorporation of the methyl groups which allowed a homogeneous dispersion of highly active gallium species on the silica matrix before calcination. The effect of reaction time, temperature, catalyst loading and acetone to glycerol molar ratio was investigated. Furthermore, the mesoporous gallosilicate materials were truly heterogeneous without leaching gallium active sites and can be efficiently reused in successive catalytic cycles.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"452 ","pages":"Article 116409"},"PeriodicalIF":6.5,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009355","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
A synthesis-structure-catalytic activity map for CO oxidation on dealloyed Au-Ag nanoparticles derived using multiscale simulations 基于多尺度模拟的合金金-银纳米颗粒CO氧化合成-结构-催化活性图
IF 6.5 1区 化学
Journal of Catalysis Pub Date : 2025-09-04 DOI: 10.1016/j.jcat.2025.116406
Prajwal Kumar Ayadathil, Abhijit Chatterjee
{"title":"A synthesis-structure-catalytic activity map for CO oxidation on dealloyed Au-Ag nanoparticles derived using multiscale simulations","authors":"Prajwal Kumar Ayadathil,&nbsp;Abhijit Chatterjee","doi":"10.1016/j.jcat.2025.116406","DOIUrl":"10.1016/j.jcat.2025.116406","url":null,"abstract":"<div><div>Dealloyed gold nanoparticles can be synthesized by selectively dissolving Ag from gold-silver alloy nanoparticles through the well-known process of dealloying. These nanoparticles exhibit remarkable catalytic activity towards the CO oxidation reaction owing to their large specific surface area, presence of rough surfaces that contain a high density of catalytically-active sites, and synergistic effects arising from the residual Ag leftover from the dealloying process. We introduce a computational framework aimed at determining the optimal dealloying conditions that can yield dealloyed nanoparticles with the highest CO oxidation specific activity. This is accomplished by establishing comprehensive synthesis-structure–activity relations for dealloyed nanoparticles. Through such an approach, we elucidate the link between the key catalyst attributes (active site density, reaction kinetics, and synergistic effects) and dealloying parameters (initial nanoparticle size, composition, dissolution condition, and dissolution time). Our methodology combines multiscale simulations to explore a vast synthesis-parameter space. The resulting size-dependent synthesis-structure–activity map reveals the optimal residual Ag for efficient CO oxidation catalysis.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"451 ","pages":"Article 116406"},"PeriodicalIF":6.5,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144995538","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
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