Catalysis Letters最新文献

英文中文

MoO3 Catalyst Supported on Micro-Mesoporous Structure for Biodiesel Production 微介孔结构负载MoO3催化剂制备生物柴油

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2024-12-12 DOI: 10.1007/s10562-024-04901-w

Joyce S. B. Figueiredo, Nayara E. Souza, Bruno T. S. Alves, André M. Silva, Bianca V. S. Barbosa, Noemi R. C. Huaman, Romualdo R. Menezes, José J. N. Alves

This study reports the synthesis and characterization of x_MoO₃/H-Z/S micro-mesoporous catalyst, which combines the properties of ZSM-5 and SBA-15, as well as its performance for biodiesel production from the transesterification of soybean oil. ZSM-5 was added to the SBA-15 synthesis gel, calcinated, and molybdenum trioxide (MoO₃) was incorporated by incipient wetness using ammonium heptamolybdate salt [(NH₄)₆Mo₇O₂₄‧4H₂O] as a metal precursor. The diffractograms and micrographics showed a micro-mesoporous structure of the support with the characteristic peaks of MoO₃. The textural analysis showed that increasing the MoO₃ content decreases the specific area and the pore diameter of the catalysts. The Raman spectrum of the catalysts indicated vibration modes characteristic of the active species MoO₃ in the orthorhombic phase. The methanol/oil molar ratio was the variable that most influenced the yield of methyl esters within the levels of a design of experiments matrix. The highest biodiesel yield of 79.2% was obtained with 6 (wt.%) of MoO₃, 4 h of reaction time, and a methanol/oil molar ratio of 20/1. This reaction condition uses a lower molybdenum content, lower catalyst load, and lower methanol/oil molar ratio than those reported in the literature, which qualitatively reduces the process costs. A quantitative economic analysis must be further performed to define the economic viability of the process.

Graphical Abstract

本研究报道了x_MoO3/H-Z/S微介孔催化剂的合成和表征，该催化剂结合了ZSM-5和SBA-15的性能，以及其用于大豆油酯交换制生物柴油的性能。将ZSM-5加入SBA-15合成凝胶中，煅烧后，以七钼酸铵盐[(NH4)6Mo7O24·4H2O]为金属前驱体，用初湿法掺入三氧化钼（MoO3）。衍射图和显微图显示该载体为微介孔结构，具有MoO3的特征峰。结构分析表明，MoO3含量的增加使催化剂的比表面积和孔径减小。催化剂的拉曼光谱显示了活性物质MoO3在正交相中的振动模式特征。在设计的实验基质水平内，甲醇/油的摩尔比是影响甲酯收率最大的变量。当MoO3用量为6 (wt.%)，反应时间为4 h，甲醇/油摩尔比为20/1时，生物柴油收率最高，为79.2%。该反应条件使用较低的钼含量、较低的催化剂负荷和较低的甲醇/油摩尔比，从而定性地降低了工艺成本。必须进一步进行定量经济分析，以确定该过程的经济可行性。图形抽象

{"title":"MoO3 Catalyst Supported on Micro-Mesoporous Structure for Biodiesel Production","authors":"Joyce S. B. Figueiredo, Nayara E. Souza, Bruno T. S. Alves, André M. Silva, Bianca V. S. Barbosa, Noemi R. C. Huaman, Romualdo R. Menezes, José J. N. Alves","doi":"10.1007/s10562-024-04901-w","DOIUrl":"10.1007/s10562-024-04901-w","url":null,"abstract":"<div><p>This study reports the synthesis and characterization of x_MoO<sub>3</sub>/H-Z/S micro-mesoporous catalyst, which combines the properties of ZSM-5 and SBA-15, as well as its performance for biodiesel production from the transesterification of soybean oil. ZSM-5 was added to the SBA-15 synthesis gel, calcinated, and molybdenum trioxide (MoO<sub>3</sub>) was incorporated by incipient wetness using ammonium heptamolybdate salt [(NH<sub>4</sub>)<sub>6</sub>Mo<sub>7</sub>O<sub>24</sub>‧4H<sub>2</sub>O] as a metal precursor. The diffractograms and micrographics showed a micro-mesoporous structure of the support with the characteristic peaks of MoO<sub>3</sub>. The textural analysis showed that increasing the MoO<sub>3</sub> content decreases the specific area and the pore diameter of the catalysts. The Raman spectrum of the catalysts indicated vibration modes characteristic of the active species MoO<sub>3</sub> in the orthorhombic phase. The methanol/oil molar ratio was the variable that most influenced the yield of methyl esters within the levels of a design of experiments matrix. The highest biodiesel yield of 79.2% was obtained with 6 (wt.%) of MoO<sub>3</sub>, 4 h of reaction time, and a methanol/oil molar ratio of 20/1. This reaction condition uses a lower molybdenum content, lower catalyst load, and lower methanol/oil molar ratio than those reported in the literature, which qualitatively reduces the process costs. A quantitative economic analysis must be further performed to define the economic viability of the process.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 1","pages":""},"PeriodicalIF":2.3,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142811164","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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

Metal-Free Photoredox Catalysis for the S-Trifluoromethylation of Thiols 硫醇s -三氟甲基化的无金属光氧化还原催化

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2024-12-12 DOI: 10.1007/s10562-024-04860-2

Raheemat Rafiu, Puspa Aryal, V. Prakash Reddy

The S-trifluoromethylation of thiols is accomplished using a simple and cost-effective organic catalyst (diacetyl) along with a bench-stable and environmentally friendly trifluoromethylating reagent (Langlois reagent). Under optimized conditions (2.5 equivalents of Langlois reagent, Blue LED irradiation, 48-h reaction time at room temperature), the reaction yielded up to 81% S-trifluoromethylated product. This method’s high yields, compatibility with a broad substrate scope (aliphatic, heteroaromatic, and aromatic thiols), and environmentally friendly conditions demonstrate its potential for broader synthetic applications. In contrast to traditional methods that rely on organometallic catalysts and environmentally hazardous reagents, this novel photoredox catalysis method offers a more economical and sustainable alternative for S-trifluoromethylation of thiols.

Graphical Abstract

硫醇的s -三氟甲基化是使用一种简单且具有成本效益的有机催化剂（二乙酰基）和一种稳定且环保的三氟甲基化试剂（朗格卢瓦试剂）完成的。在优化条件下（2.5当量朗格卢瓦试剂，蓝光LED照射，室温下反应48 h）， s -三氟甲基化产物收率高达81%。该方法的产率高，与广泛的底物范围（脂肪族，杂芳烃和芳香族硫醇）的相容性，以及环境友好的条件表明其具有更广泛的合成应用潜力。与依赖有机金属催化剂和环境有害试剂的传统方法相比，这种新型光氧化还原催化方法为硫醇的s -三氟甲基化提供了一种更经济、更可持续的替代方法。图形抽象

引用次数: 0

Metal-Free Sustainable N-α-C(sp3)-H Functionalization of Arylmethylamines with Arylmethylketones to Synthesis of Kröhnke Pyridines Under Solvent-free Condition 无溶剂条件下芳基甲基胺与芳基甲基酮持续N-α-C(sp3)-H功能化合成Kröhnke吡啶

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2024-12-02 DOI: 10.1007/s10562-024-04873-x

Vikas D. Kadu, Sankala Naga Chandrudu, Mahesh G. Hublikar, Shahaji I. Bansode, Raghunath B. Bhosale

An efficient “one pot” direct N-α-C(sp³)-H functionalization of arylmethylamines towards synthesis of substituted 2,4,6-triarylpyridines has developed. Fascinatingly, this method features O₂ as an oxidant, metal-free simple reaction operation and the dual role of arylmethylamines. The self-oxidative coupling of readily available simple methylamines followed by their sequential deamination/cyclization cascade with arylmethylketones has accomplished anticipated 2,4,6-triarylpyridines (20 examples) up to 95% yield with good functional groups tolerance. The straightforward reaction condition in the presence of an oxidant O₂ and generated H₂O as a sole byproduct made this process environmentally friendly.

Graphical Abstract

提出了一种用N-α-C(sp3)-H直接功能化芳基甲胺合成取代2,4,6-三芳基吡啶的高效“一锅法”。令人着迷的是，这种方法的特点是O2作为氧化剂，无金属的简单反应操作和芳基甲胺的双重作用。易得的简单甲胺的自氧化偶联，以及它们与芳基甲基酮的顺序脱胺/环化级联，已经完成了预期的2,4,6-三芳基吡啶（20个例子），产率高达95%，具有良好的官能团耐受性。在氧化剂O2存在下的直接反应条件和生成的唯一副产物H2O使该过程对环境友好。图形抽象

引用次数: 0

Mechanistic Investigation of Dimethyl Carbonate Synthesis Over Palladium Chloride Catalyst 氯化钯催化合成碳酸二甲酯的机理研究

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2024-12-02 DOI: 10.1007/s10562-024-04855-z

Zhi-Shen Huang, Zhang-Feng Zhou, Lu-Yang Qiao, Yun-Yun Zeng, Shan-Shan Zong, Yuan-Gen Yao

The production of dimethyl carbonate (DMC) from CO and methyl nitrite (MN) is of great industrial interest for chemicals upgrading. As one of the most efficient catalysts, PdCl₂ based catalyst has been widely investigated and been verified to be highly selective toward DMC yielding. However, the underlying mechanism is unclear so far. Herein, we identified the active sites and corresponding reaction pathway on PdCl₂ (140) surface by the density functional theory (DFT) calculations, combining with X-ray absorption fine structure (XAFS) and in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) measurements. The dissociation of MN resulted in the construction of Cl vacancies on PdCl₂ (140) surface, which are the specific sites for DMC formation. On the other hand, the continuous loss of Cl induced the reduction of PdCl₂ to Pd, leading to changed pathway of reaction and decreased yield of DMC. These insights highlighted the importance of Cl-balance in PdCl₂ based catalyst system, which determined the final products of CO oxidative esterification.

Graphical Abstract

以CO和亚硝酸盐甲酯（MN）为原料生产碳酸二甲酯（DMC）具有重要的工业意义。作为最高效的催化剂之一，PdCl2基催化剂已被广泛研究，并被证明对DMC的产率具有高选择性。然而，到目前为止，其潜在机制尚不清楚。本文通过密度泛函理论（DFT）计算，结合x射线吸收精细结构（XAFS）和原位漫反射红外傅立叶变换光谱（DRIFTS）测量，确定了PdCl2（140）表面的活性位点和相应的反应途径。MN的解离导致PdCl2（140）表面形成Cl空位，这是DMC形成的特定位点。另一方面，Cl的持续损失诱导PdCl2还原为Pd，导致反应途径改变，DMC产率降低。这些发现强调了基于PdCl2的催化剂体系中cl平衡的重要性，它决定了CO氧化酯化的最终产物。图形抽象

{"title":"Mechanistic Investigation of Dimethyl Carbonate Synthesis Over Palladium Chloride Catalyst","authors":"Zhi-Shen Huang, Zhang-Feng Zhou, Lu-Yang Qiao, Yun-Yun Zeng, Shan-Shan Zong, Yuan-Gen Yao","doi":"10.1007/s10562-024-04855-z","DOIUrl":"10.1007/s10562-024-04855-z","url":null,"abstract":"<div><p>The production of dimethyl carbonate (DMC) from CO and methyl nitrite (MN) is of great industrial interest for chemicals upgrading. As one of the most efficient catalysts, PdCl<sub>2</sub> based catalyst has been widely investigated and been verified to be highly selective toward DMC yielding. However, the underlying mechanism is unclear so far. Herein, we identified the active sites and corresponding reaction pathway on PdCl<sub>2</sub> (140) surface by the density functional theory (DFT) calculations, combining with X-ray absorption fine structure (XAFS) and <i>in-situ</i> diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) measurements. The dissociation of MN resulted in the construction of Cl vacancies on PdCl<sub>2</sub> (140) surface, which are the specific sites for DMC formation. On the other hand, the continuous loss of Cl induced the reduction of PdCl<sub>2</sub> to Pd, leading to changed pathway of reaction and decreased yield of DMC. These insights highlighted the importance of Cl-balance in PdCl<sub>2</sub> based catalyst system, which determined the final products of CO oxidative esterification.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 1","pages":""},"PeriodicalIF":2.3,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142761715","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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

Electric Field-assisted Photocatalytic Reduction of Carbon Dioxide over Titanium Dioxide: Influence of the Type and Strength of Electric Field 电场辅助光催化氧化二氧化钛还原二氧化碳：电场类型和强度的影响

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2024-12-02 DOI: 10.1007/s10562-024-04887-5

Oleksandr Shtyka, Radoslaw Ciesielski, Adam Kedziora, Malgorzata Szynkowska-Jozwik, Tomasz Maniecki

This study focuses on investigating the sole impact of an external electric field on the photocatalytic activity of TiO₂-based materials. Typically, built-in electric fields are used to efficiently separate free energy carriers and improve the photocatalytic performance of semiconductors. The creation of such field requires modifications to the photocatalyst that alter various properties such as adsorption and optical characteristics. These modifications make it challenging to isolate and interpret the promotion effect associated with the electric field alone. The investigations were carried out in the gas-phase conditions in a specially constructed reactor equipped with two electrodes connected to a high – voltage that provides a field strength of up to 5.7·10³ V/cm. The results showed that the effect of electric field promotion varied significantly depending on the properties of titanium dioxide, such as structure, adsorption, and presence of impurities. The strength and the type (direct or alternating current) of the electric field also played a determining role. The greatest promoting effect was observed for rutile, the photocatalytic activity of which under an electric field increased threefold in the process of reduction of CO₂ with water vapor.

Graphical Abstract

本研究的重点是研究外电场对tio2基材料光催化活性的唯一影响。通常，内置电场用于有效地分离自由能载流子和提高半导体的光催化性能。创造这样的场需要修改光催化剂，改变各种性质，如吸附和光学特性。这些修改使得分离和解释与电场单独相关的促进效应具有挑战性。研究是在气相条件下在一个特制的反应器中进行的，该反应器配备了两个连接到高压的电极，提供高达5.7·103 V/cm的场强。结果表明，电场促进的效果因二氧化钛的结构、吸附和杂质的存在等性质而有显著差异。电场的强度和类型（直流电或交流电）也起决定性作用。金红石对水蒸气还原CO2的促进作用最大，电场作用下金红石的光催化活性提高了3倍。图形抽象

{"title":"Electric Field-assisted Photocatalytic Reduction of Carbon Dioxide over Titanium Dioxide: Influence of the Type and Strength of Electric Field","authors":"Oleksandr Shtyka, Radoslaw Ciesielski, Adam Kedziora, Malgorzata Szynkowska-Jozwik, Tomasz Maniecki","doi":"10.1007/s10562-024-04887-5","DOIUrl":"10.1007/s10562-024-04887-5","url":null,"abstract":"<div><p>This study focuses on investigating the sole impact of an external electric field on the photocatalytic activity of TiO<sub>2</sub>-based materials. Typically, built-in electric fields are used to efficiently separate free energy carriers and improve the photocatalytic performance of semiconductors. The creation of such field requires modifications to the photocatalyst that alter various properties such as adsorption and optical characteristics. These modifications make it challenging to isolate and interpret the promotion effect associated with the electric field alone. The investigations were carried out in the gas-phase conditions in a specially constructed reactor equipped with two electrodes connected to a high – voltage that provides a field strength of up to 5.7·10<sup>3</sup> V/cm. The results showed that the effect of electric field promotion varied significantly depending on the properties of titanium dioxide, such as structure, adsorption, and presence of impurities. The strength and the type (direct or alternating current) of the electric field also played a determining role. The greatest promoting effect was observed for rutile, the photocatalytic activity of which under an electric field increased threefold in the process of reduction of CO<sub>2</sub> with water vapor.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 1","pages":""},"PeriodicalIF":2.3,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s10562-024-04887-5.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142761714","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Diesel Production by Catalytic Cracking of Castor Oil Using Aluminas and Silicas 用氧化铝和二氧化硅催化蓖麻油裂解生产柴油

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2024-12-02 DOI: 10.1007/s10562-024-04874-w

Eric B. Ribeiro, Leila O. Daher, Elaine A. Faria, Fernando C. Garcia, Mirian S. C. Pereira, Joel C. Rubim, Alexandre G. S. Prado, Paulo A. Z. Suarez, Romulo D. A. Andrade

The purely thermal cracking of castor oil produces a mixture of compounds with unsatisfactory fuel properties, as high viscosity, high acid value and low cetane index. This low quality is associated with high value of oxygenated products in obtained product composition. The aim of this work was to improve the physical–chemical properties of cracking product (pyrolysis) of castor oil using different catalysts, such as silica and silica doped with titanium (IV) oxide, and alumina and alumina doped with zinc(II), tin(II), titanium(IV) and zirconium(IV) oxides. The study of the physical–chemical properties of the castor oil cracking products showed that all these catalysts have activity in the deoxygenating, being the better results reached using pure and doped alumina. We also studied the catalytic activity of laboratory synthesized alumina (pure and as support for Lewis acid metals), commercial silica (Merck) and titanium (IV) oxide supported on silica, in the cracking of castor oil. It was observed that the aluminas showed better activity in the deoxygenating of the products than silicas. This fact can be explained by higher acidity and mesoporous characteristic of the aluminas.

Graphical Abstract

蓖麻油的纯热裂解产生的混合物具有令人不满意的燃料性能，如高粘度，高酸值和低十六烷指数。这种低质量与所获得的产品组成中氧化产物的高价值有关。采用不同的催化剂，如掺杂氧化钛（IV）的二氧化硅和二氧化硅，以及掺杂锌（II）、锡（II）、钛（IV）和锆（IV）氧化物的氧化铝和氧化铝，以改善蓖麻油裂解产物（热解）的物理化学性质。对蓖麻油裂解产物的理化性质进行了研究，结果表明，这些催化剂都具有一定的脱氧活性，其中纯氧化铝和掺杂氧化铝的脱氧效果较好。我们还研究了实验室合成的氧化铝（纯的，作为路易斯酸金属的载体），商业二氧化硅（默克）和二氧化硅负载的氧化钛（IV）在蓖麻油裂解中的催化活性。结果表明，氧化铝对产物的脱氧活性优于二氧化硅。这可以用氧化铝的高酸性和介孔特性来解释。图形抽象

{"title":"Diesel Production by Catalytic Cracking of Castor Oil Using Aluminas and Silicas","authors":"Eric B. Ribeiro, Leila O. Daher, Elaine A. Faria, Fernando C. Garcia, Mirian S. C. Pereira, Joel C. Rubim, Alexandre G. S. Prado, Paulo A. Z. Suarez, Romulo D. A. Andrade","doi":"10.1007/s10562-024-04874-w","DOIUrl":"10.1007/s10562-024-04874-w","url":null,"abstract":"<div><p>The purely thermal cracking of castor oil produces a mixture of compounds with unsatisfactory fuel properties, as high viscosity, high acid value and low cetane index. This low quality is associated with high value of oxygenated products in obtained product composition. The aim of this work was to improve the physical–chemical properties of cracking product (pyrolysis) of castor oil using different catalysts, such as silica and silica doped with titanium (IV) oxide, and alumina and alumina doped with zinc(II), tin(II), titanium(IV) and zirconium(IV) oxides. The study of the physical–chemical properties of the castor oil cracking products showed that all these catalysts have activity in the deoxygenating, being the better results reached using pure and doped alumina. We also studied the catalytic activity of laboratory synthesized alumina (pure and as support for Lewis acid metals), commercial silica (Merck) and titanium (IV) oxide supported on silica, in the cracking of castor oil. It was observed that the aluminas showed better activity in the deoxygenating of the products than silicas. This fact can be explained by higher acidity and mesoporous characteristic of the aluminas.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><img></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 1","pages":""},"PeriodicalIF":2.3,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142761685","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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

Synthesis of a Novel Highly Active NiMoO4 Nanocatalyst for the Sustainable Production of Anhydrous Formaldehyde from the Non-oxidative Dehydrogenation of Methanol at Relatively Low Temperature 低温甲醇非氧化脱氢可持续生产无水甲醛的新型高活性NiMoO4纳米催化剂的合成

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2024-12-02 DOI: 10.1007/s10562-024-04865-x

Aya Farouk Farghal, Abd El-Aziz Ahmed Said, Mohamed M. M. Abd El-Wahab, Mohamed Nady Goda

The production of formaldehyde (FA) and clean hydrogen gas via the non-oxidative dehydrogenation of methanol is seen to be a promising approach where the anhydrous formaldehyde is an ideal for using in the subsequent manufacture of oxygenated synthetic fuels. In this investigation, NiMoO₄ with nanoaggregates morphology was synthesized by hydrothermal method in presence of triethylamine (TEA) as a surfactant and tested for the non-oxidative catalytic dehydrogenation of methanol into formaldehyde at relatively low temperature. Structural, morphological and textural properties were characterized by TGA, DSC, XPS, XRD, FT-IR, HR-TEM, pyridine-TPD and N₂-sorption assessments. Results of XRD verified the coexistence of mixed phases of both α and β-NiMoO₄. The catalysts' texture, structure, acidity and catalytic activity were greatly influenced by the introduction and the molar ratio of TEA. The variation of catalytic activity is strongly associated to the variation in S_BET and acidity. Activity results revealed that catalyst with Ni:TEA ratio of 1:1 (N₁T₁) was the most active catalyst with methanol conversion of 96% and selectivity to FA of 95% at reaction temperature of 325 °C. The outstanding catalytic performance of this catalyst is due to the presence of weak and intermediate strength Brønsted acidic sites on its surface. This catalyst showed remarkable stability for the synthesis of anhydrous formaldehyde over a 160 h period while maintaining the same conversion and selectivity.

Graphical Abstract

通过甲醇的非氧化脱氢生产甲醛（FA）和清洁氢气被认为是一种有前途的方法，其中无水甲醛是随后制造含氧合成燃料的理想选择。本研究以三乙胺（TEA）为表面活性剂，采用水热法合成纳米聚集体形态的NiMoO4，并在较低温度下进行甲醇非氧化催化脱氢制甲醛实验。通过TGA、DSC、XPS、XRD、FT-IR、HR-TEM、吡啶- tpd和n2吸附等方法表征了其结构、形态和织构性能。XRD结果证实α和β-NiMoO4混合相共存。催化剂的织构、结构、酸度和催化活性受茶的引入量和茶的摩尔比的影响较大。催化活性的变化与SBET和酸度的变化密切相关。活性结果表明，在325℃的反应温度下，Ni:TEA比为1:1 （N1T1）的催化剂活性最高，甲醇转化率为96%，FA选择性为95%。该催化剂的优异催化性能是由于其表面存在弱和中等强度的Brønsted酸性位点。该催化剂在160 h的合成周期内表现出良好的稳定性，同时保持了相同的转化率和选择性。图形抽象

{"title":"Synthesis of a Novel Highly Active NiMoO4 Nanocatalyst for the Sustainable Production of Anhydrous Formaldehyde from the Non-oxidative Dehydrogenation of Methanol at Relatively Low Temperature","authors":"Aya Farouk Farghal, Abd El-Aziz Ahmed Said, Mohamed M. M. Abd El-Wahab, Mohamed Nady Goda","doi":"10.1007/s10562-024-04865-x","DOIUrl":"10.1007/s10562-024-04865-x","url":null,"abstract":"<div><p>The production of formaldehyde (FA) and clean hydrogen gas via the non-oxidative dehydrogenation of methanol is seen to be a promising approach where the anhydrous formaldehyde is an ideal for using in the subsequent manufacture of oxygenated synthetic fuels. In this investigation, NiMoO<sub>4</sub> with nanoaggregates morphology was synthesized by hydrothermal method in presence of triethylamine (TEA) as a surfactant and tested for the non-oxidative catalytic dehydrogenation of methanol into formaldehyde at relatively low temperature. Structural, morphological and textural properties were characterized by TGA, DSC, XPS, XRD, FT-IR, HR-TEM, pyridine-TPD and N<sub>2</sub>-sorption assessments. Results of XRD verified the coexistence of mixed phases of both α and β-NiMoO<sub>4</sub>. The catalysts' texture, structure, acidity and catalytic activity were greatly influenced by the introduction and the molar ratio of TEA. The variation of catalytic activity is strongly associated to the variation in S<sub>BET</sub> and acidity. Activity results revealed that catalyst with Ni:TEA ratio of 1:1 (N<sub>1</sub>T<sub>1</sub>) was the most active catalyst with methanol conversion of 96% and selectivity to FA of 95% at reaction temperature of 325 °C. The outstanding catalytic performance of this catalyst is due to the presence of weak and intermediate strength Brønsted acidic sites on its surface. This catalyst showed remarkable stability for the synthesis of anhydrous formaldehyde over a 160 h period while maintaining the same conversion and selectivity.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 1","pages":""},"PeriodicalIF":2.3,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142761684","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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

Visible Light Induced Eosin Y Catalysed Green Synthesis of Substituted Pyrroles 可见光诱导曙红 Y 催化取代吡咯的绿色合成

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2024-11-29 DOI: 10.1007/s10562-024-04888-4

Rohit Kumar, Km Garima, Vishal Srivastava, Praveen P. Singh, Pravin K. Singh

A simple green method for synthesizing the substituted pyrroles through one-pot multicomponent reaction of primary amines, 1,3-dicarbonyls, nitromethane and benzaldehyde catalysed by eosin Y under visible light irradiation at room temperature have been developed. The aim of this study is develop a green and cost-effective approach to synthesize substituted pyrroles and its derivatives with high yields in a short reaction time using an organic photocatalyst.

Graphical Abstract

在室温可见光照射下，通过曙红 Y 催化伯胺、1,3-二羰基、硝基甲烷和苯甲醛的单锅多组分反应合成取代的吡咯的简单绿色方法已经开发出来。本研究的目的是开发一种绿色、经济高效的方法，利用有机光催化剂在较短的反应时间内高产率地合成取代的吡咯及其衍生物。

引用次数: 0

Correction to: In Silico Models for Prediction of Methanol Yield in CO2 Hydrogenation Reaction Using CuBased Catalysts 更正：使用铜基催化剂预测 CO2 加氢反应中甲醇产率的硅学模型

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2024-11-29 DOI: 10.1007/s10562-024-04882-w

Vanjari Pallavi, Reddi Kamesh, K. Yamuna Rani

引用次数: 0

Promotional Catalytic Activity of Bifunctional Ru-Ce-Zr Catalysts forNH3-SCO by Deposition Order of Dual Active Components 双活性组分沉积顺序对双功能Ru-Ce-Zr催化剂nh3 - sco催化活性的促进作用

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters

Pub Date : 2024-11-29 DOI: 10.1007/s10562-024-04891-9

Zhengxiong Jiang

The ammonia fuel injected into the combustion chamber cannot be completely combusted resulting in high levels of escaped ammonia in the ammonia-fueled engine exhaust. It is a feasible way to obtain ammonia selective catalytic oxidation (NH₃-SCO) catalysts with excellent performance using noble metal-transition metal catalysts. In this work, a series of Ru-Ce-Zr bifunctional catalysts were synthesized by precipitation and impregnation methods to investigate the influence of introduction methods of different active components (Ru and Ce) on their physicochemical properties and NH₃-SCO performance. Among them, the BET and NH₃-TPD results showed that Ru-Ce/ZrO₂ (RC/Z) catalyst had the largest specific surface area and NH₃ desorption amount, indicating that its surface could capture more NH₃. More importantly, compared to other catalysts, RC/Z catalyst exhibited highest relative concentration of Ce³⁺, which facilitated electron transfer via Ce⁴⁺ + Ru³⁺ ↔ Ce³⁺ + Ru⁴⁺. The Ru-Ce/ZrO₂ catalyst exhibited the best catalytic performance under the strong interaction between Ru and Ce species. its NH₃ conversion reached 100% and N₂ selectivity was 95.7% at 237 °C. The N₂ selectivity exceeded 70% over a wide temperature range of 150–400 °C. In situ diffuse reflectance infrared Fourier transform spectroscopy (in-situ DRIFTS) showed that the surface of RC/Z catalyst exhibited the highest amount of Lewis and Brønsted acid sites, which might be one of the reasons for its excellent N₂ selectivity. This work revealed the effect of the way of introduction of Ru and Ce active species on their NH₃-SCO performance.

Graphical Abstract

注入燃烧室的氨燃料不能完全燃烧，导致氨燃料发动机排气中高浓度的氨逸出。贵金属-过渡金属催化剂是制备性能优良的氨选择性催化氧化（NH3-SCO）催化剂的可行途径。本文采用沉淀法和浸渍法合成了一系列Ru-Ce- zr双功能催化剂，研究了不同活性组分（Ru和Ce）的引入方式对其理化性能和NH3-SCO性能的影响。其中，BET和NH3- tpd结果表明，Ru-Ce/ZrO2 （RC/Z）催化剂具有最大的比表面积和NH3解吸量，表明其表面可以捕获更多的NH3。更重要的是，与其他催化剂相比，RC/Z催化剂表现出最高的Ce3+的相对浓度，这有助于通过Ce4+ + Ru3+↔Ce3+ + Ru4+传递电子。Ru-Ce/ZrO2催化剂在Ru和Ce的强相互作用下表现出最好的催化性能。在237℃下，NH3转化率达到100%，N2选择性为95.7%。在150 ~ 400℃的较宽温度范围内，N2选择性超过70%。原位漫反射红外傅里叶变换光谱（原位DRIFTS）表明，RC/Z催化剂表面具有最多的Lewis和Brønsted酸位，这可能是其具有优异的N2选择性的原因之一。本工作揭示了Ru和Ce活性物质的引入方式对其NH3-SCO性能的影响。图形抽象

{"title":"Promotional Catalytic Activity of Bifunctional Ru-Ce-Zr Catalysts forNH3-SCO by Deposition Order of Dual Active Components","authors":"Zhengxiong Jiang","doi":"10.1007/s10562-024-04891-9","DOIUrl":"10.1007/s10562-024-04891-9","url":null,"abstract":"<div><p>The ammonia fuel injected into the combustion chamber cannot be completely combusted resulting in high levels of escaped ammonia in the ammonia-fueled engine exhaust. It is a feasible way to obtain ammonia selective catalytic oxidation (NH<sub>3</sub>-SCO) catalysts with excellent performance using noble metal-transition metal catalysts. In this work, a series of Ru-Ce-Zr bifunctional catalysts were synthesized by precipitation and impregnation methods to investigate the influence of introduction methods of different active components (Ru and Ce) on their physicochemical properties and NH<sub>3</sub>-SCO performance. Among them, the BET and NH<sub>3</sub>-TPD results showed that Ru-Ce/ZrO<sub>2</sub> (RC/Z) catalyst had the largest specific surface area and NH<sub>3</sub> desorption amount, indicating that its surface could capture more NH<sub>3</sub>. More importantly, compared to other catalysts, RC/Z catalyst exhibited highest relative concentration of Ce<sup>3+</sup>, which facilitated electron transfer via Ce<sup>4+</sup> + Ru<sup>3+</sup> ↔ Ce<sup>3+</sup> + Ru<sup>4+</sup>. The Ru-Ce/ZrO<sub>2</sub> catalyst exhibited the best catalytic performance under the strong interaction between Ru and Ce species. its NH<sub>3</sub> conversion reached 100% and N<sub>2</sub> selectivity was 95.7% at 237 °C. The N<sub>2</sub> selectivity exceeded 70% over a wide temperature range of 150–400 °C. In situ diffuse reflectance infrared Fourier transform spectroscopy (in-situ DRIFTS) showed that the surface of RC/Z catalyst exhibited the highest amount of Lewis and Brønsted acid sites, which might be one of the reasons for its excellent N<sub>2</sub> selectivity. This work revealed the effect of the way of introduction of Ru and Ce active species on their NH<sub>3</sub>-SCO performance.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 1","pages":""},"PeriodicalIF":2.3,"publicationDate":"2024-11-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142754000","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"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

首页上一页

类型

全部化学•材料生命科学医学物理工程技术环境•农林材料科学地球科学法学管理学化学环境科学与生态学计算机科学教育学经济学农林科学人文科学生物学数学物理与天体物理心理学综合性期刊其他工业工程理学历史学农学文学信息工程

数据库

全部 ACS Publications Elsevier ieeexplore Springer The Royal Society of Chemistry Wiley

期刊

Catalysis Letters

全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.

﹀