Journal of Catalysis最新文献_第7页

CuPt dual-atom synergistic catalyst boost carbon-oxygen bonds hydrogenation

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-02-24 DOI: 10.1016/j.jcat.2025.116047

Ziheng Zhen , Antai Li , Tiantian Xiao , Maoshuai Li , Jing Lv , Shouying Huang , Yue Wang , Xinbin Ma

{"title":"CuPt dual-atom synergistic catalyst boost carbon-oxygen bonds hydrogenation","authors":"Ziheng Zhen , Antai Li , Tiantian Xiao , Maoshuai Li , Jing Lv , Shouying Huang , Yue Wang , Xinbin Ma","doi":"10.1016/j.jcat.2025.116047","DOIUrl":"10.1016/j.jcat.2025.116047","url":null,"abstract":"<div><div>Bimetallic catalyst with dual-atom pairs has drawn much attention in heterogeneous catalysis due to their unique synergistic effects. In this work, we prepared a series CeO<sub>2</sub> supported Cu-Pt dual sites catalysts and found the optimized one of 2Cu0.025Pt/CeO<sub>2</sub> exhibited excellent performance in the hydrogenation of methyl acetate (MA). Its product yield of ethanol was as 4 times as that of 2Cu/CeO<sub>2</sub> catalyst under the same reaction conditions, with only 0.025 wt% Pt addition. Combined with various characterizations and contrast samples, it is demonstrated that the post-deposited trace Pt species preferentially located besides the copper atoms and formed Cu-Pt atomic pairs. But when further increasing the loading of Pt, the aggregation of Cu happened, leading to a rapid decrease of activity. To reveal the role of Cu-Pt atom pairs in the hydrogenation of carbon–oxygen bonds reactions, we conducted chemisorption experiments and DFT simulations. It is suggested that Cu-Pt atomic pairs significantly enhanced the adsorption and activation capability of both the MA and H<sub>2</sub> molecules during the reaction. These insights may provide synthesis and design strategy for high-performance dual-atom sites catalysts for the carbon–oxygen bonds hydrogenation reactions.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"445 ","pages":"Article 116047"},"PeriodicalIF":6.5,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143477550","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

Direct synthesis of amides from nitroarenes and carboxylic acids via CO-mediated reduction

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-02-22 DOI: 10.1016/j.jcat.2025.116042

Mikhail A. Losev , Oleg I. Afanasyev , Denis Chusov

引用次数: 0

Exhaustive reduction of aromatic esters and carboxylic acids with a homogeneous cobalt catalyst

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-02-21 DOI: 10.1016/j.jcat.2025.116034

Zi-Heng Zhang , Rui Sun , Yuan-Yuan Jiang , Jin-Qing Lin , Yan-Qiang Zhang , Bao-Hua Xu

{"title":"Exhaustive reduction of aromatic esters and carboxylic acids with a homogeneous cobalt catalyst","authors":"Zi-Heng Zhang , Rui Sun , Yuan-Yuan Jiang , Jin-Qing Lin , Yan-Qiang Zhang , Bao-Hua Xu","doi":"10.1016/j.jcat.2025.116034","DOIUrl":"10.1016/j.jcat.2025.116034","url":null,"abstract":"<div><div>A one-step procedure to exhaustively reduce aromatic esters and carboxylic acids to their corresponding tolyl derivatives is a significant transformation in organic synthesis, which remains challenging in homogeneous catalysis. In this study, it’s achieved by using the well-defined phosphinesulfonate chelated cobalt-based catalyst (Co(dppbsa)), along with NaBAr<sup>F</sup><sub>4</sub> as the basic additive and (MeO)<sub>2</sub>MeSiH as the reductant. Particularly, this cobalt catalysis proceeds through ether intermediates. Experimental combined theoretical results support it follows an outer-sphere ionic hydrosilylation mechanism and the in situ formed cationic siloxane species are involved in the rate-limiting hydride transfer. The same system also enables the catalytic deoxygenation of aliphatic esters, aliphatic acids, and amides but terminating at the corresponding ethers, alkanols and secondary amines, respectively. These findings open up novel avenues for the catalytic application of phosphinesulfonate chelated complexes, potentially serving as the foundation for the exhaustive reduction of carboxylic skeletons with cobalt.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"445 ","pages":"Article 116034"},"PeriodicalIF":6.5,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143462321","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

The enhanced reactivity of graphitic supports for Pd catalyzed toluene hydrogenation

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-02-20 DOI: 10.1016/j.jcat.2025.116029

Alaba U. Ojo , Deependra M. Shakya , Julian Stetzler , Musbau Gbadamosi , Rahman Md. Masudur , Narayan Acharya , Nathan Thornburg , John Tengco , Santosh Kiran Balijepalli , John R. Monnier , Donna A. Chen , John R. Regalbuto

引用次数: 0

Divergent photoreduction of nitroaromatic compounds catalysed by dithienoquinoxaline

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-02-19 DOI: 10.1016/j.jcat.2025.116033

Zuzana Burešová , Monika Grygarová , Eva Prokopová , Milan Klikar , Oldřich Pytela , Jiří Váňa , Abul Mansur Muhammed Fahim , Kanyashree Jana , Ekaterina Zubova , Jan Bartáček , Jiří Tydlitát , Zdeňka Růžičková , Radek Cibulka , Kirk S. Schanze , Filip Bureš

{"title":"Divergent photoreduction of nitroaromatic compounds catalysed by dithienoquinoxaline","authors":"Zuzana Burešová , Monika Grygarová , Eva Prokopová , Milan Klikar , Oldřich Pytela , Jiří Váňa , Abul Mansur Muhammed Fahim , Kanyashree Jana , Ekaterina Zubova , Jan Bartáček , Jiří Tydlitát , Zdeňka Růžičková , Radek Cibulka , Kirk S. Schanze , Filip Bureš","doi":"10.1016/j.jcat.2025.116033","DOIUrl":"10.1016/j.jcat.2025.116033","url":null,"abstract":"<div><div>Nitroaromatic compounds can be conveniently reduced to anilines with the aid of a variety of chemical reductants. However, chemodivergent and chemoselective reduction of functionalized nitroaromatics into valuable nitroso, azo(xy), (hydr)azo and (hydroxyl)amino derivatives remains rather elusive. Electro- and photochemical strategies utilizing various catalytic systems and reaction media have been tested but most have been directed towards individual reduction products. Here, we present the photoredox-enabled chemodivergent reduction of nitroaromatics to nitroso, bis-(<em>N</em>,<em>O</em>-diacetyl)-<em>N</em>-arylhydroxylamine, azoxy, azo and amino derivatives. The developed protocol utilizes a novel photocatalyst, 6,9-dimethoxydithieno[2,3-<em>f</em>:3′,2′-<em>h</em>]quinoxaline-2,3-dicarbonitrile, and Hantzsch ester/triethanolamine as reductants. With the single organic photocatalyst, the reaction environment, temperature, time and catalyst loading can be varied to achieve chemodivergent photoreduction of nitroaromatics bearing various functional groups and to access a library of valuable products. The application of this methodology to multigram preparations of molecules of pharmaceutical and industrial relevance highlights its practical utility.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"445 ","pages":"Article 116033"},"PeriodicalIF":6.5,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143451572","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

Boosting low-concentration toluene oxidation by decorating ultrasmall Pt nanoparticles on La0.8Sr0.2MnO3-δ with hydrogen plasma treatment

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-02-18 DOI: 10.1016/j.jcat.2025.116031

Bin Zhu , Xin He , Lingze Liu , Jinglin Liu , Xiaomin Zhang , Ben W.-L. Jang

{"title":"Boosting low-concentration toluene oxidation by decorating ultrasmall Pt nanoparticles on La0.8Sr0.2MnO3-δ with hydrogen plasma treatment","authors":"Bin Zhu , Xin He , Lingze Liu , Jinglin Liu , Xiaomin Zhang , Ben W.-L. Jang","doi":"10.1016/j.jcat.2025.116031","DOIUrl":"10.1016/j.jcat.2025.116031","url":null,"abstract":"<div><div>Perovskite is one of the most promising materials for catalytic oxidation of volatile organic compounds (VOCs) because of its special tunable structure and properties as well as high stability. However, it commonly suffers from relatively low catalytic activity due to the low specific surface area and limited numbers of active sites caused by high synthesis temperature required. To improve thereactivity of the perovskite catalyst, a promising strategy is to construct highly dispersed noble metal sites on surfaces perovskite. However, generating highly active metallic sites while exhibiting good thermal stability remains a formidable challenge. Here, it’s demonstrated that the construction of highly efficient and robust platinum (Pt) sites on La<sub>0.8</sub>Sr<sub>0.2</sub>MnO<sub>3-δ</sub> (Pt/LSMO) for toluene oxidation resulted in an almost three-fold increase in toluene conversion with a good stability. The key to the construction of these Pt sites is treating the oxidized Pt species on LSMO with hydrogen (H<sub>2</sub>) plasma at low temperatures, which leads to the formation of high metallic Pt (Pt<sup>0</sup>), ultrasmall Pt nanoparticles (∼1.3 nm), and high concentration of oxygen vacancy (O<sub>v</sub>). These features facilitate the generation of a large number of highly active and stable Pt<sup>0</sup>-Mn<sup>3+</sup>-O<sub>v</sub> sites on Pt/LSMO, which contribute to the activation of toluene and oxygen species and, therefore, the catalytic reaction. This investigation demonstrates a promising approach of using the cold plasma technique to design and construct high-performing noble-based perovskite catalysts for toluene oxidation.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"445 ","pages":"Article 116031"},"PeriodicalIF":6.5,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143443797","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

Insight into the role of Na distribution in Cu-SSZ-39 catalysts

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-02-18 DOI: 10.1016/j.jcat.2025.116032

Na Zhu, Lingyu Yu, Lisen Hou, Siying Wang

{"title":"Insight into the role of Na distribution in Cu-SSZ-39 catalysts","authors":"Na Zhu, Lingyu Yu, Lisen Hou, Siying Wang","doi":"10.1016/j.jcat.2025.116032","DOIUrl":"10.1016/j.jcat.2025.116032","url":null,"abstract":"<div><div>Cu-SSZ-39 has garnered significant attention because of its outstanding NH<sub>3</sub>-SCR activity and hydrothermal stability. To facilitate commercial application of Cu-SSZ-39, it is crucial to streamline the synthesis process, adopt eco-friendly synthesis methods, enhance the catalytic performance, and explore the underlying catalytic mechanisms. Herein, ammonia exchange was skipped and Cu-SSZ-39 was directly synthesized via Cu-exchange of Na-SSZ-39. This approach yielded a Cu-SSZ-39 with superior catalytic performance compared to that prepared using the conventional NH<sub>4</sub>-SSZ-39. Comparative characterization of the Cu-SSZ-39 catalysts, derived from both Na-SSZ-39 and NH<sub>4</sub>-SSZ-39 exchanges demonstrated that the positioning of Na cations affected Cu distribution, and controlling Na distribution can enhance deNO<em><sub>x</sub></em> activity. It was also found that while cation locations did not alter the reaction mechanism of Cu-SSZ-39 at low temperature, they did increase the concentration of active NO<em><sub>x</sub></em> intermediates, thereby boosting catalytic performance. This study facilitates a more sustainable synthesis of Cu-SSZ-39 and provides deeper insights into how cations’ distribution in zeolites affects catalytic efficiency.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"445 ","pages":"Article 116032"},"PeriodicalIF":6.5,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143443798","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

Catalysts for ethanol dry reforming based on high-entropy perovskites

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-02-17 DOI: 10.1016/j.jcat.2025.116028

Nikita F. Eremeev , Semon A. Hanna , Ekaterina M. Sadovskaya , Aleksandra A. Leonova , Olga A. Bulavchenko , Arcady V. Ishchenko , Igor P. Prosvirin , Vladislav A. Sadykov , Yuliya N. Bespalko

{"title":"Catalysts for ethanol dry reforming based on high-entropy perovskites","authors":"Nikita F. Eremeev , Semon A. Hanna , Ekaterina M. Sadovskaya , Aleksandra A. Leonova , Olga A. Bulavchenko , Arcady V. Ishchenko , Igor P. Prosvirin , Vladislav A. Sadykov , Yuliya N. Bespalko","doi":"10.1016/j.jcat.2025.116028","DOIUrl":"10.1016/j.jcat.2025.116028","url":null,"abstract":"<div><div>Ethanol dry reforming is a promising way to produce syngas and hydrogen due to utilization of carbon dioxide and ability to produce ethanol using renewable sources. Main problem associated with ethanol dry reforming reaction is coke formation. Coking suppression can be achieved in a few ways including use of catalysts possessing required oxygen transport properties. High entropy oxides are of interest in application as catalysts for ethanol dry reforming and other reactions due to their structural stability, disordering features and tunability of functional properties. In this work, the catalysts based on Ni and multiple doped La manganites are studied. The oxides are synthesized by modified Pechini and citrate techniques, and the catalysts are prepared by wetness impregnation. The samples are characterized by XRD, TEM with EDX analysis, XPS. Oxygen transport and redox properties are studied by temperature-programmed isotope exchange of oxygen and reduction. According to structural and morphological studies, the samples are nanosized and form perovskite-like structure. The surface features of samples were characterized by XPS. The samples demonstrate a moderate oxygen mobility (<em>D*</em> up to ∼10<sup>–12</sup> cm<sup>2</sup>/s at 700 °C) required for catalytic operation and coking suppression. Tests in ethanol dry reforming demonstrated fine performance and good stability in the reaction conditions.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"445 ","pages":"Article 116028"},"PeriodicalIF":6.5,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435366","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

Supremely high turnover numbers with a simple porphyrin photosensitizer: Kinetic and mechanistic insights into the oxidation of sulfides with singlet oxygen

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-02-17 DOI: 10.1016/j.jcat.2025.116008

Stepan M. Korobkov , Kirill P. Birin , Aslan Yu. Tsivadze

引用次数: 0

Construction of electron-rich nickel single atom catalyst by heteroatom doping for enhanced CO2 electroreduction

IF 6.5 1区化学

Journal of Catalysis Pub Date : 2025-02-16 DOI: 10.1016/j.jcat.2025.116020

Jiale Sun , Kaiqi Li , Zhen Liu , Junwei Xu , Ping Gao , Meng Wang , Yifei Li , Rilong Zhu , Ivan P. Parkin , Zhongyuan Huang

{"title":"Construction of electron-rich nickel single atom catalyst by heteroatom doping for enhanced CO2 electroreduction","authors":"Jiale Sun , Kaiqi Li , Zhen Liu , Junwei Xu , Ping Gao , Meng Wang , Yifei Li , Rilong Zhu , Ivan P. Parkin , Zhongyuan Huang","doi":"10.1016/j.jcat.2025.116020","DOIUrl":"10.1016/j.jcat.2025.116020","url":null,"abstract":"<div><div>Adjustment of electron distribution by heteroatom doping has emerged as a promising strategy to improve the electrochemical CO<sub>2</sub> reduction (ECR) performance of nickel single atom catalysts. Herein, density functional theory calculation (DFT) verifies that the doping of phosphorus atoms in the first shell regulates the valence state of the nickel centre and facilitates higher electron density in the outer shell, which is beneficial to intermediate adsorption, electron transfer and the decrease of reaction energy barrier, resulting in outstanding ECR performance. Guided by the theoretical calculation results, the asymmetrical nickel single atom catalyst doped with phosphorus atom was successfully fabricated by phytic acid modification and calcination treatment. X-ray photoelectron spectroscopy and X-ray absorption fine structure spectroscopy prove that the valence state of nickel exhibits a negative shift and makes them electron-rich after doping phosphorus atom, which is consistent with DFT results. Such catalyst displays superior ECR performance with CO faradaic efficiency above 90 % at a wide potential range and a high CO partial current density of −244.1 mA cm<sup>−2</sup> at −1.0 V in flow cell. The asymmetric electron regulation strategy can be potentially applied to the other transition metal single atoms to enhance their catalytic performance.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"445 ","pages":"Article 116020"},"PeriodicalIF":6.5,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418439","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