Applied Catalysis A: General最新文献

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The role of the ZnO promoter in the structural evolution of Cu2O in the Rochow-Müller reaction for dimethyldichlorosilane synthesis 氧化锌促进剂在二甲基二氯硅烷合成的 Rochow-Müller 反应中 Cu2O 结构演变中的作用
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2024-09-05 DOI: 10.1016/j.apcata.2024.119941
{"title":"The role of the ZnO promoter in the structural evolution of Cu2O in the Rochow-Müller reaction for dimethyldichlorosilane synthesis","authors":"","doi":"10.1016/j.apcata.2024.119941","DOIUrl":"10.1016/j.apcata.2024.119941","url":null,"abstract":"<div><p>Zinc oxide (ZnO) is commonly used as a promoter in Cu-based catalysts for the Rochow-Müller reaction, which is used to produce organosilane monomers in the organosilicon industry. However, the impact of ZnO on the phase transformation of Cu-based catalysts during the Rochow-Müller reaction has not been fully revealed. In this work, we synthesized two ZnO-modified Cu<sub>2</sub>O model catalysts by simple ball milling (Cu<sub>2</sub>O-ZnO) and physical mixing (Cu<sub>2</sub>O+ZnO) methods. The addition of ZnO enhanced catalytic properties, resulting in higher dimethyldichlorosilane (M2) selectivity and Si conversion compared to using the pure Cu<sub>2</sub>O catalyst. The introduction of ZnO into Cu<sub>2</sub>O enhanced the adsorption of methyl chloride (MeCl) on the Cu<sub>2</sub>O surface, causing Cu<sub>2</sub>O to transform into Cu and CuCl. Subsequently, CuCl reacted with active Si to form active Cu<sub><em>x</em></sub>Si species. This work provides valuable insights into the roles of ZnO in Cu<sub>2</sub>O-based catalysts and sheds light on their catalytic mechanism in the Rochow-Müller reaction.</p></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":null,"pages":null},"PeriodicalIF":4.7,"publicationDate":"2024-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142150840","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}
引用次数: 0
A novel Ti³⁺-mediated approach for supporting palladium on anodic TiO2 nanotubes: Toward efficient and recyclable catalysis in the heck reaction 以 Ti³⁺ 为媒介在阳极 TiO2 纳米管上支撑钯的新方法:在赫克反应中实现高效和可循环催化
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2024-09-03 DOI: 10.1016/j.apcata.2024.119942
{"title":"A novel Ti³⁺-mediated approach for supporting palladium on anodic TiO2 nanotubes: Toward efficient and recyclable catalysis in the heck reaction","authors":"","doi":"10.1016/j.apcata.2024.119942","DOIUrl":"10.1016/j.apcata.2024.119942","url":null,"abstract":"<div><p>A simple electrochemical reduction technique was employed to generate Ti<sup>3+</sup> with strong reducing property on the anodic TiO<sub>2</sub> nanotubes (ATNTs). Utilizing Ti<sup>3+</sup> as the reducing agent, Pd<sup>2+</sup> was successfully reduced in situ to Pd<sup>0</sup> on the anodic TiO<sub>2</sub> nanotubes (Pd@ATNTs). Various characterization methods were employed to confirm that the proportion of Ti<sup>3+</sup> and the size of Pd nanoparticles could be controlled by adjusting the electrochemical reduction voltage. The obtained [email protected] exhibited satisfactory catalytic efficiency (TOF: 1302 h<sup>−1</sup>) in the Heck reaction between various aryl halides and olefins. Furthermore, [email protected] demonstrated high stability, with no significant loss of catalytic activity observed even after six cycles.</p></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":null,"pages":null},"PeriodicalIF":4.7,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142150839","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}
引用次数: 0
On-site hydrogen-rich gas production from diesel: A comprehensive study on catalyst development with nickel and diverse metal oxides (MgO, La2O3, CeO2, SiO2) supported on alumina 从柴油中现场生产富氢气体:以氧化铝为载体的镍和多种金属氧化物(MgO、La2O3、CeO2、SiO2)催化剂开发综合研究
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2024-08-31 DOI: 10.1016/j.apcata.2024.119940
{"title":"On-site hydrogen-rich gas production from diesel: A comprehensive study on catalyst development with nickel and diverse metal oxides (MgO, La2O3, CeO2, SiO2) supported on alumina","authors":"","doi":"10.1016/j.apcata.2024.119940","DOIUrl":"10.1016/j.apcata.2024.119940","url":null,"abstract":"<div><p>The study aimed to investigate the impact of nickel-incorporating diverse metal oxides (MgO, La<sub>2</sub>O<sub>3</sub>, CeO<sub>2</sub>, SiO<sub>2</sub>) supported on alumina on the Diesel steam reforming reaction. Catalytic activity tests were performed within a reaction period of 6 h at 800°C and atmospheric pressure. The amount of catalyst is 30 gr in each experiment corresponding to a LHSV value of 0.2 hr<sup>−1</sup>. The tests proved that the performances of Ni-containing La<sub>2</sub>O<sub>3</sub> and CeO<sub>2</sub>-supported catalysts were highly stable and active in steam reforming of Diesel, giving complete conversion. The incorporation of CeO<sub>2</sub> (20 % wt) into Al<sub>2</sub>O<sub>3</sub> support resulted in a significant reduction in the amount of coke formation from 0.85 % to 0.26 %. In order to investigate catalyst stability, time-on stream tests extending to 6 days, totaling 36 hours were performed using 5Ni@10La<sub>2</sub>O<sub>3</sub>-Al<sub>2</sub>O<sub>3</sub>. As a result of the long-term stability test, no deactivation has been observed under the test conditions despite very few amounts of carbon (1.33 wt%) formed. When comparing the short-term and long-term tests, similar syn-gas production results were observed, along with approximately the same amount of carbon formation.</p></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":null,"pages":null},"PeriodicalIF":4.7,"publicationDate":"2024-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142150837","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}
引用次数: 0
Selective oxidation of methane to formaldehyde and carbon monoxide over V/MSN catalysts with isolated VO4 sites 在具有孤立 VO4 位点的 V/MSN 催化剂上将甲烷选择性氧化为甲醛和一氧化碳
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2024-08-30 DOI: 10.1016/j.apcata.2024.119928
{"title":"Selective oxidation of methane to formaldehyde and carbon monoxide over V/MSN catalysts with isolated VO4 sites","authors":"","doi":"10.1016/j.apcata.2024.119928","DOIUrl":"10.1016/j.apcata.2024.119928","url":null,"abstract":"<div><p>The selective oxidation of methane to value-added C<sub>1</sub> chemicals (e.g., HCHO and CO) is a crucial process in the chemical industry. Recent studies indicate that the generation of highly dispersed isolated active sites is crucial for improving the performance in the selective oxidation of methane and studying the corresponding structure–activity relationship. Therefore, we used mesoporous silica nanoparticles (MSN) as supports and utilized grafting method to prepare catalysts with more selective oxidation active centers (isolated VO<sub>4</sub>). The study found that isolated VO<sub>4</sub> centers are the active sites for the selective oxidation of methane to formaldehyde, and CO is the product of further oxidation of formaldehyde. The total selectivity of formaldehyde and CO on all catalysts is higher than 83.6 %. Among them, the highly dispersed and isolated VO<sub>4</sub> tetrahedral active centers on the 2 V/MSN catalyst could stably convert methane to formaldehyde, achieving the highest formaldehyde yield of 3.7 % at 670 °C.</p></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":null,"pages":null},"PeriodicalIF":4.7,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142095636","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}
引用次数: 0
Active site requirements for bio-alcohol dehydration: Effect of chemical structure and site proximity 生物酒精脱水的活性位点要求:化学结构和邻近部位的影响
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2024-08-30 DOI: 10.1016/j.apcata.2024.119939
{"title":"Active site requirements for bio-alcohol dehydration: Effect of chemical structure and site proximity","authors":"","doi":"10.1016/j.apcata.2024.119939","DOIUrl":"10.1016/j.apcata.2024.119939","url":null,"abstract":"<div><p>Synthesis-structure-activity relations are reported, describing how interzeolite conversion (IZC) allows synthesis of ZSM-5 (MFI framework) with fixed physicochemical properties, except the variable local acid site (Al) arrangement, by variation of the synthesis time. Local confinement and acidity effects are probed by applying both H-ZSM-5 and Na-ZSM-5 samples in alcohol dehydration. Pyridine and divalent cobalt ion probing are used to quantify the amount of accessible acid sites and of Al in close proximity. Al in close proximity shows a strong influence on n-butanol dehydration turnover rates. The turnover rates are also strongly dependent on local confinement: in Na-form, ZSM-5 synthesized with more Al present as isolated species is a factor of 3–7 times more active than Na-ZSM-5 with fewer isolated Al. However if the zeolites are in proton form, ZSM-5 with more proximate sites show a higher activity compared to ZSM-5 with more isolated sites. Linear butene selectivity increases in Na-ZSM-5 compared to H-ZSM-5, caused by a suppressed dibutyl ether formation. The selectivity towards 1-butene is enhanced to a greater extent on proximate sites, likely due to a local/steric constraint at the active site. Decomposition of DBE over Na-ZSM-5 is more active compared to n-butanol dehydration, independent of acid site proximity. Also for 2-propanol dehydration, Na-ZSM-5 is less active than H-ZSM-5, yet the activity difference is attenuated compared to n-butanol dehydration. Essentially, due to the intrinsic higher reactivity of 2-propanol, the acid site requirement is less stringent. These findings highlight the importance of local confinement and Al proximity in acid-catalyzed conversion of oxygenated compounds.</p></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":null,"pages":null},"PeriodicalIF":4.7,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142137302","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}
引用次数: 0
Oxidation of 2,5-bis(hydroxymethyl)furan to 2,5-furandicarboxylic acid with morphology-dependent Au/CeO2 catalysts 使用形态依赖性 Au/CeO2 催化剂将 2,5-双(羟甲基)呋喃氧化为 2,5-呋喃二甲酸
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2024-08-28 DOI: 10.1016/j.apcata.2024.119929
{"title":"Oxidation of 2,5-bis(hydroxymethyl)furan to 2,5-furandicarboxylic acid with morphology-dependent Au/CeO2 catalysts","authors":"","doi":"10.1016/j.apcata.2024.119929","DOIUrl":"10.1016/j.apcata.2024.119929","url":null,"abstract":"<div><p>2,5-Furandicarboxylic acid (FDCA), a bio-based diacid with a rigid ring, has a similar structure to petroleum-based terephthalic acid. Its co-polyester with ethylene glycol has excellent performance in terms of thermal and mechanical properties. Herein, an Au/CeO<sub>2</sub>-rod catalyst with rich oxygen vacancies was developed to achieve the efficient oxidation of 2,5-bis(hydroxymethyl)furan (BHMF) to FDCA with a 92 % yield under mild conditions, with the addition of 4 equivalents of Na<sub>2</sub>CO<sub>3</sub> at 80℃ under 2 MPa O<sub>2</sub> for 6 h. The large specific surface area of CeO<sub>2</sub>-rod is beneficial for better dispersion of Au nanoparticles. Meanwhile, the high activity of Au/CeO<sub>2</sub>-rod can be attributed to that the rod-shaped CeO<sub>2</sub> exposed more active (100) facets, resulting in strong metal-support interaction between Au nanoparticles and CeO<sub>2</sub>-rod. This could generate more Au species with oxidized state and more oxygen vacancies, thus promoting the reactant adsorption and oxygen activation and enhancing the final oxidation activity. The oxidation of 5-hydroxymethyl-2-furancarboxylic acid to FDCA was determined as the rate-determining step in the oxidation of BHMF over the Au/CeO<sub>2</sub> catalyst.</p></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":null,"pages":null},"PeriodicalIF":4.7,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142129194","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}
引用次数: 0
2D/2D Bi2WO6/C3N5 S-scheme heterojunction for highly selective production of CH4 by photocatalytic CO2 reduction under visible light 二维/二维 Bi2WO6/C3N5 S 型异质结在可见光下通过光催化二氧化碳还原高选择性地生产 CH4
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2024-08-28 DOI: 10.1016/j.apcata.2024.119914
{"title":"2D/2D Bi2WO6/C3N5 S-scheme heterojunction for highly selective production of CH4 by photocatalytic CO2 reduction under visible light","authors":"","doi":"10.1016/j.apcata.2024.119914","DOIUrl":"10.1016/j.apcata.2024.119914","url":null,"abstract":"<div><p>Photocatalytic CO<sub>2</sub> reduction is a practical solution to the energy dilemma and environmental damage caused by greenhouse gases, and it is very important to explore high-efficiency photocatalysts. In this study, a novel Bi<sub>2</sub>WO<sub>6</sub>/C<sub>3</sub>N<sub>5</sub> step(S)-scheme heterojunction was successfully constructed and applied for CO<sub>2</sub> photoreduction. The 2D/2D structure showed excellent photocatalytic properties, with methane production reaching 1.976 μmol·g<sup>−1</sup>·h<sup>−1</sup> and selectivity reaching 100 % under 5 hours of visible light irradiation. The result indicates that combining Bi<sub>2</sub>WO<sub>6</sub> and C<sub>3</sub>N<sub>5</sub> can promote interfacial charge separation and maintain the optimal reducing ability of photogenerated electrons. Based on experimental and theoretical calculations, we characterized the reaction mechanism and heterojunction formation mechanism. This study offers a novel approach to improve the selectivity and photocatalytic efficiency of CO<sub>2</sub> reduction products.</p></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":null,"pages":null},"PeriodicalIF":4.7,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142095744","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}
引用次数: 0
Investigation of different ratio of CuCe catalysts applied in photothermal reverse water gas shift reaction 不同配比的 CuCe 催化剂在光热反向水气变换反应中的应用研究
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2024-08-27 DOI: 10.1016/j.apcata.2024.119927
{"title":"Investigation of different ratio of CuCe catalysts applied in photothermal reverse water gas shift reaction","authors":"","doi":"10.1016/j.apcata.2024.119927","DOIUrl":"10.1016/j.apcata.2024.119927","url":null,"abstract":"<div><p>The photothermal catalytic reverse water gas shift reaction (RWGS) can convert CO<sub>2</sub> into other high-value-added chemical resources under mild conditions. However, the design and development of high-performance catalysts is a major challenge. In this work, different proportions of CuCe bimetallic catalysts were synthesized using the sol-gel method and applied to RWGS. Under the visible light heat catalytic condition at 450 ℃, the CO yield can be increased by about 20 % compared to thermal catalysis, which is better than most metal-based catalysts reported in the literature. Moreover, the catalyst exhibited good stability and reusability, with the primary factor affecting the stability of the CuCe catalyst being the growth of Cu nanoparticles. The characterization shows that at Cu/Ce=1, the separation efficiency of electron-hole separation is the highest, and the hot electrons generated by the LSPR effect of Cu can be effectively separated and transferred, producing more oxygen vacancies and suitable alkaline sites, so it has the best photothermal catalytic performance. Furthermore, the catalyst is dominated by the formate pathway under light conditions, and this work provides a new RWGS strategy.</p></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":null,"pages":null},"PeriodicalIF":4.7,"publicationDate":"2024-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142089296","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}
引用次数: 0
Dipyridyl-anderson-polyoxometalate built-in metal–organic frameworks for aerobic photooxidation 用于有氧光氧化的二吡啶基-安德森-聚氧化金属内置金属有机框架
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2024-08-27 DOI: 10.1016/j.apcata.2024.119913
{"title":"Dipyridyl-anderson-polyoxometalate built-in metal–organic frameworks for aerobic photooxidation","authors":"","doi":"10.1016/j.apcata.2024.119913","DOIUrl":"10.1016/j.apcata.2024.119913","url":null,"abstract":"<div><p>Two POM-MOFs <strong>Co-1</strong> and <strong>Ni-1</strong> were synthesized from pyridyl-Anderson-POM linker. When combined with [Ru(bpy)<sub>3</sub>]<sup>2+</sup>, <strong>Ru(bpy)</strong><sub><strong>3</strong></sub><strong>@Co-1</strong> showed excellent photocatalytic performance in sulfide oxidation and oxidative coupling of benzylamines with good recyclability.</p></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":null,"pages":null},"PeriodicalIF":4.7,"publicationDate":"2024-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142095637","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}
引用次数: 0
Zinc ferro- and ferri-cyanides catalyst structures from point of colloid chemistry view 从胶体化学角度看锌铁氰化物和锌铁氰化物催化剂结构
IF 4.7 2区 化学
Applied Catalysis A: General Pub Date : 2024-08-25 DOI: 10.1016/j.apcata.2024.119902
{"title":"Zinc ferro- and ferri-cyanides catalyst structures from point of colloid chemistry view","authors":"","doi":"10.1016/j.apcata.2024.119902","DOIUrl":"10.1016/j.apcata.2024.119902","url":null,"abstract":"<div><p>The aim of this research was to comprehensively analyze zinc ferro- and ferri-cyanides for rationally choose or modify hexacyanoferrates in a range of application focused on catalysing the ring-opening copolymerization of epoxides and CO<sub>2</sub> to reduce the environmental toll. Scripts of the synthesis of 14 samples with variable morphology are given. Thermogravimetry, FT-IR, and XRD indicates the formation of two predominant types of bridging cyanide groups with different coordination environment, which accounts for a lack crystallinity aggregate with an amorphous part. Involving dynamic light scattering and laser Doppler electrophoresis as distinguishing features the formation of colloidal fractions is demonstrated and characterized. The switch from a negative surface rich in Lewis basic sites (Me–C<img>N<sup>–</sup>) to a surface rich in open-metal sites is either jump and stepwise successfully completed. The proposed structures of micelles of the catalysts allow great attention to be paid to every small detail of their catalytic activity.</p></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":null,"pages":null},"PeriodicalIF":4.7,"publicationDate":"2024-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142058228","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}
引用次数: 0
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