Catalysis Science & Technology最新文献_第2页

On the mechanisms of ethane dehydrogenation on silica-supported mononuclear Fe† 二氧化硅负载单核铁†上乙烷脱氢机理的研究

IF 4.4 3区化学

Catalysis Science & Technology Pub Date : 2024-12-05 DOI: 10.1039/D4CY01118J

Sakshi Satyanand, Sanjana Srinivas, Dionisios G. Vlachos and Stavros Caratzoulas

{"title":"On the mechanisms of ethane dehydrogenation on silica-supported mononuclear Fe†","authors":"Sakshi Satyanand, Sanjana Srinivas, Dionisios G. Vlachos and Stavros Caratzoulas","doi":"10.1039/D4CY01118J","DOIUrl":"https://doi.org/10.1039/D4CY01118J","url":null,"abstract":"With the increasing interest in developing catalytic materials based on atomically dispersed transition metals on heterogeneous supports, it is necessary to have an atomic-level understanding of the factors that impact their structural and electronic properties and, ultimately, their reactivity. In this contribution, we address and elucidate with electronic structure calculations open questions related to the ethane dehydrogenation mechanism on silica-supported mononuclear Fe(II) and Fe(III) sites. Contrary to prior hypotheses, we determine that the σ-metathesis on Fe(II) sites is an unlikely dehydrogenation mechanism. On tricoordinate and tetracoordinate Fe(II)@SiO2, the reaction proceeds via heterolytic C–H bond activation and β-hydride elimination facilitated by spin-crossing. Atomically dispersed Fe(III) grafted on SiO2 exhibits a more complex behavior as it seems to be undergoing autoreduction and we propose a new redox ethane dehydrogenation mechanism which, remarkably, is energetically competitive with the heterolytic C–H activation mechanism previously identified for other transition metals.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 1","pages":" 114-122"},"PeriodicalIF":4.4,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cy/d4cy01118j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142912667","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Direct conversion of syngas to aromatics via a two-stage C–C coupling over MnZr/HZSM-5 bifunctional catalysts employing OX-ZEO strategy† 采用OX-ZEO策略的MnZr/HZSM-5双功能催化剂通过两级C-C耦合直接将合成气转化为芳烃

IF 4.4 3区化学

Catalysis Science & Technology Pub Date : 2024-12-05 DOI: 10.1039/D4CY01388C

Shiyu Liu, Qiuyun Huang, Ijaz Ul Haq, Zixu Yang, Weihua Shen and Yunjin Fang

{"title":"Direct conversion of syngas to aromatics via a two-stage C–C coupling over MnZr/HZSM-5 bifunctional catalysts employing OX-ZEO strategy†","authors":"Shiyu Liu, Qiuyun Huang, Ijaz Ul Haq, Zixu Yang, Weihua Shen and Yunjin Fang","doi":"10.1039/D4CY01388C","DOIUrl":"https://doi.org/10.1039/D4CY01388C","url":null,"abstract":"Even though the oxide–zeolite (OX-ZEO) strategy is generally applied for the direct conversion of syngas into aromatics (STA), previous researches have rarely studied the evolution of the surface species. In this work, MnZrOx binary oxides were synthesized and bifunctional catalysts were prepared by physically mixing powders of the binary oxides with H-ZSM-5. In situ diffuse reflection Fourier transform infrared spectroscopy was performed, and surface C–C coupling between the alkyl and formate groups over the surface of the oxides was observed, which was named as primary C–C coupling. As products of the primary C–C coupling, the higher alkyl carboxylate groups could be hydrogenated to surface aldehydes, and both the species could diffuse into the zeolite for secondary C–C coupling, thereby generating aromatics. The reaction pathway of CO was shortened by the insertion of surface formate, thus promoting CO conversion. Under optimal reaction conditions, the CO conversion reached 55% with the selectivity of aromatics exceeding 80%. Coke deposition was also observed on the external surface of H-ZSM-5, which might be the reason for the further decline in CO conversion.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 2","pages":" 580-591"},"PeriodicalIF":4.4,"publicationDate":"2024-12-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142994060","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Chemical kinetic mechanism for selective catalytic reduction of nitrogen oxides† 选择性催化还原氮氧化物的化学动力学机理

IF 4.4 3区化学

Catalysis Science & Technology Pub Date : 2024-12-05 DOI: 10.1039/D4CY01205D

Alexey A. Burluka and Andrew P. Manning

引用次数: 0

Correction: Integrated adsorption and photocatalytic degradation of VOCs using a TiO2/diatomite composite: effects of relative humidity and reaction atmosphere 修正：二氧化钛/硅藻土复合材料对VOCs的综合吸附和光催化降解：相对湿度和反应气氛的影响

IF 4.4 3区化学

Catalysis Science & Technology Pub Date : 2024-12-05 DOI: 10.1039/D4CY90098G

Guangxin Zhang, Arman Peyravi, Zaher Hashisho, Zhiming Sun, Yangyu Liu, Shuilin Zheng and Lexuan Zhong

引用次数: 0

Synthesis of a novel hydrophobic CeO2–BiOCl/CF composite cathode for efficient heterogeneous electro-Fenton degradation of tetracycline 新型疏水CeO2-BiOCl /CF复合阴极的合成及其在四环素非均相电fenton降解中的应用

IF 4.4 3区化学

Catalysis Science & Technology Pub Date : 2024-12-04 DOI: 10.1039/D4CY01211A

Huiqi Lv, Jiangshan Kuai, Rongshuai Wang, Yiwen Mou and Weilin Guo

{"title":"Synthesis of a novel hydrophobic CeO2–BiOCl/CF composite cathode for efficient heterogeneous electro-Fenton degradation of tetracycline","authors":"Huiqi Lv, Jiangshan Kuai, Rongshuai Wang, Yiwen Mou and Weilin Guo","doi":"10.1039/D4CY01211A","DOIUrl":"https://doi.org/10.1039/D4CY01211A","url":null,"abstract":"Bifunctional electrodes have attracted significant research interest in the field of electro-Fenton (EF) processes for the efficient treatment of antibiotic-contaminated wastewater. In this study, carbon felt (CF) was selected as the matrix material because of its excellent electrochemical properties, high porosity, and large specific surface area. BiOCl and CeO2 were in situ synthesized on the CF electrode using a hydrothermal method, followed by the application of a hydrophobic polytetrafluoroethylene (PTFE) coating on the CF surface. The resulting composite electrode was employed in the EF process for in situ electro-generation and activation of hydrogen peroxide (H2O2), facilitating the efficient degradation of tetracycline (TC). Free-radical quenching experiments revealed that hydroxyl radical and superoxide anion radical were the predominant reactive species in the EF process, with hydroxyl radicals playing a major role in the degradation of TC. The electrode exhibited excellent stability over consecutive runs. Furthermore, a plausible mechanism for the production and activation of H2O2, as well as the degradation of TC, was proposed. This study provides a new strategy for the construction of efficient and stable bifunctional cathodes for the advanced treatment of antibiotic-contaminated wastewater.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 2","pages":" 537-546"},"PeriodicalIF":4.4,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142993888","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Relationship between Lewis acid sites and carbohydrate reactivity over Sn-β catalysts† Sn-β催化剂上Lewis酸位点与碳水化合物反应性的关系

IF 4.4 3区化学

Catalysis Science & Technology Pub Date : 2024-12-04 DOI: 10.1039/D4CY01147C

Yacine Boudjema, Antoine Brunel, Raphaël Del Cerro, Gerhard Pirngruber, Céline Chizallet and Kim Larmier

{"title":"Relationship between Lewis acid sites and carbohydrate reactivity over Sn-β catalysts†","authors":"Yacine Boudjema, Antoine Brunel, Raphaël Del Cerro, Gerhard Pirngruber, Céline Chizallet and Kim Larmier","doi":"10.1039/D4CY01147C","DOIUrl":"https://doi.org/10.1039/D4CY01147C","url":null,"abstract":"Sn-β is a promising Lewis acid zeolite for carbohydrate conversion. This material can be prepared either directly by hydrothermal synthesis or by a dealumination – metal incorporation sequence starting from a pre-made zeolite (post-synthesis modification). The synthesis method and the metallic precursors significantly influence the formation of Lewis acid sites in the zeolite, which is the primary factor determining the activity of the catalyst in many reactions. We synthesized various materials through post-synthesis modifications and a hydrothermal method using three different precursors. Pyridine adsorption monitored by FTIR spectroscopy shows that Sn-β samples synthesized by solid state insertion with tin chloride as a precursor feature a concentration of Lewis acid sites proportional to the tin content (up to 1.5 wt% of tin) without forming an oxide phase. Hydrothermal synthesis leads to a sample exhibiting weaker acid sites. The catalyst yields three major products in glucose conversion: fructose, mannose, and lactic acid. The high yield of lactic acid (≈30%) indicates a faster ketose retro-aldolization compared to aldose (no C4 or C2 products detected).","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 2","pages":" 396-404"},"PeriodicalIF":4.4,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142993927","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Towards continuous Rh-hydroformylation of long chain alkenes: handling methodology for the long-term stability of Biphephos in a continuous reactor with an attached membrane separation unit† 长链烯烃的连续rh -氢甲酰化：附膜分离装置的连续反应器中双磷长期稳定性的处理方法

IF 4.4 3区化学

Catalysis Science & Technology Pub Date : 2024-12-04 DOI: 10.1039/D4CY01148A

Viktor Söderholm, Marc Stajer, Carolin Savage, Leon Splittgerber and Dieter Vogt

{"title":"Towards continuous Rh-hydroformylation of long chain alkenes: handling methodology for the long-term stability of Biphephos in a continuous reactor with an attached membrane separation unit†","authors":"Viktor Söderholm, Marc Stajer, Carolin Savage, Leon Splittgerber and Dieter Vogt","doi":"10.1039/D4CY01148A","DOIUrl":"https://doi.org/10.1039/D4CY01148A","url":null,"abstract":"Diphosphites like Biphephos are known for their combination of high activity and high linear selectivity in the Rh-catalyzed hydroformylation of terminal alkenes. However, like most phosphite-type ligands, Biphephos is prone to hydrolysis under acidic conditions and oxidation in the presence of oxygen, resulting in detrimental catalyst performance loss. In this work, we identified practical aspects that safeguard the long-term stability of Biphephos during the Rh-catalyzed hydroformylation of alkenes. Furthermore, different additives (amines and one epoxide) were explored as stabilizers for Biphephos. The Biphephos/Rh/stabilizer system was first extensively investigated via31P-NMR, followed by batch autoclave experiments (100 ml reactors), and finally applied in an upscaled reactor (300 ml) with an attached nanofiltration membrane unit for catalyst retention. With cyclohexene oxide (CHO) as a stabilizer for the ligand, stable operation with high catalyst retention (95%) was achieved for over 100 h at high product selectivity (l/b = 78).","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 2","pages":" 592-604"},"PeriodicalIF":4.4,"publicationDate":"2024-12-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cy/d4cy01148a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142994061","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

In situ grown Ru-doped Ni(OH)2 nanosheets on nickel foam for stable electrocatalytic hydrogen evolution reaction† 在泡沫镍上原位生长钌掺杂Ni(OH)2纳米片，用于稳定的电催化析氢反应†

IF 4.4 3区化学

Catalysis Science & Technology Pub Date : 2024-12-03 DOI: 10.1039/D4CY01074D

Ting Zhou, Shanshan Ye, Jing Gao, Hang Zhang and Shengliang Zhong

引用次数: 0

Accelerated photocatalytic hydrogen evolution over donor–acceptor type graphitic carbon nitride (g-CN) with simultaneous modification of pyrimidine and thiophene rings† 同时修饰嘧啶和噻吩环†的给受体型石墨氮化碳（g-CN）加速光催化析氢

IF 4.4 3区化学

Catalysis Science & Technology Pub Date : 2024-12-03 DOI: 10.1039/D4CY01401D

Shigen Watanabe, Hideyuki Katsumata, Monir Uzzaman, Ikki Tateishi, Mai Furukawa and Satoshi Kaneco

{"title":"Accelerated photocatalytic hydrogen evolution over donor–acceptor type graphitic carbon nitride (g-CN) with simultaneous modification of pyrimidine and thiophene rings†","authors":"Shigen Watanabe, Hideyuki Katsumata, Monir Uzzaman, Ikki Tateishi, Mai Furukawa and Satoshi Kaneco","doi":"10.1039/D4CY01401D","DOIUrl":"https://doi.org/10.1039/D4CY01401D","url":null,"abstract":"Graphitic carbon nitride (g-CN) has attracted interest due to its cost-effectiveness, ease of synthesis, and suitable band structure for hydrogen evolution. However, its application is limited by high charge recombination rates and restricted visible light absorption, which lower photocatalytic performance. This study presents a modified g-CN catalyst, termed UPDB, incorporating π-conjugated and donor–acceptor (DA) structures using urea, 2,4,6-triaminopyrimidine (P), and dibenzothiophene-2-carboxaldehyde (DB). DRS and PL measurements revealed that alongside the π–π* transitions originating from pristine g-CN, UPDB exhibits n–π* transitions influenced by the lone pair electrons and unpaired electrons present in P and DB. This interaction creates a new absorption band (midgap) that broadens visible-light absorption. FT-IR analysis confirmed that the electron donor DB binds to the end of the g-CN backbone, while DFT calculations suggested that DB induces a spatial separation between the HOMO and LUMO, significantly decreasing charge recombination. At the optimal dosage, the hydrogen evolution rate of UPDB-10 (U (10 g), P (10 mg), and DB (1 mg)) reached 1000 μmol g−1 h−1, which was approximately 10 times higher than that of the original carbon nitride (U) calcined from urea alone. Furthermore, the apparent quantum yield (AQY) was 13.7% at 400 nm, 15.5% at 420 nm, and 6.3% at 450 nm in the presence of K2HPO4 (KPH), demonstrating high visible-light responsivity. The one-pot calcination method used in this study to introduce π-conjugation and a DA structure provides a novel approach to overcome the limitations of g-CN, paving the way for the advancement of solar energy conversion technology.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 2","pages":" 416-426"},"PeriodicalIF":4.4,"publicationDate":"2024-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142993929","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Fluorinated covalent organic frameworks for visible-light driven CO2 reduction† 可见光驱动CO2还原的氟化共价有机框架

IF 4.4 3区化学

Catalysis Science & Technology Pub Date : 2024-12-02 DOI: 10.1039/D4CY01276C

Wei-Jia Wang, Bin Li, Jing Gao and Kaihong Chen

引用次数: 0