Catalysis Science & Technology最新文献_第2页

An overview: dinuclear palladium complexes for organic synthesis 综述：用于有机合成的双核钯络合物

IF 5 3区化学

Catalysis Science & Technology Pub Date : 2024-09-10 DOI: 10.1039/d4cy00425f

Sarita Yadav, Sangeeta Yadav, Mookan Natarajan, Kamal Kishore Pant, Ravi Tomar

{"title":"An overview: dinuclear palladium complexes for organic synthesis","authors":"Sarita Yadav, Sangeeta Yadav, Mookan Natarajan, Kamal Kishore Pant, Ravi Tomar","doi":"10.1039/d4cy00425f","DOIUrl":"https://doi.org/10.1039/d4cy00425f","url":null,"abstract":"From materials science and polymer chemistry to organic synthesis and medicinal chemistry, cross-coupling has influenced many scientific fields. Cross-coupling reactions with palladium have revolutionized the synthesis of compounds. These reactions have been studied and optimized to an extent that permits their application on an industrial scale. The remarkable activity and selectivity of palladium catalysts, and enzymes inspired synergistic and cooperative effects of multinuclear active sites, have urged scientists to develop and employ dinuclear palladium catalysts in various cross-coupling reactions. When two metal centers are forced to be near each other, cooperativity results, allowing the metals to stabilize one another electrically and produce a catalytically active form that is not conceivable with monometallic complexes. In comparison to equivalent catalysts with isolated metal centers, dinuclear catalysts catalyze processes either more effectively or with distinctive chemo-, regio-, or stereoselectivity. Cooperative activation can be improved by affixing covalent or non-covalent linkages to two catalytic units. Despite these developments, it is still unclear how many Pd sites function during catalysis. This study carefully examines the use of dinuclear Pd catalysts in cross-coupling processes that generate C–C and C–X bonds.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142226295","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

Ag co-catalyst prepared by ultrasonic reduction method for efficient photocatalytic conversion of CO2 with H2O using ZnTa2O6 photocatalyst 利用 ZnTa2O6 光催化剂，通过超声还原法制备银助催化剂，实现 CO2 与 H2O 的高效光催化转化

IF 5 3区化学

Catalysis Science & Technology Pub Date : 2024-09-10 DOI: 10.1039/d4cy00564c

Kio Kawata, Shoji Iguchi, Shimpei Naniwa, Tsunehiro Tanaka, Masamu Nishimoto, Kentaro Teramura

{"title":"Ag co-catalyst prepared by ultrasonic reduction method for efficient photocatalytic conversion of CO2 with H2O using ZnTa2O6 photocatalyst","authors":"Kio Kawata, Shoji Iguchi, Shimpei Naniwa, Tsunehiro Tanaka, Masamu Nishimoto, Kentaro Teramura","doi":"10.1039/d4cy00564c","DOIUrl":"https://doi.org/10.1039/d4cy00564c","url":null,"abstract":"Towards the realisation of carbon neutrality by utilising renewable energy sources, the photocatalytic conversion of CO2 with H2O—known as artificial photosynthesis—is important because H2O is non-toxic or non-hazardous, and an abundant source of protons for CO2 reduction. Many studies on the photocatalytic conversion of CO2 have revealed that Ag nanoparticles are an effective co-catalyst for the selective conversion of CO2 to CO in water. To improve the activity of the photocatalytic conversion of CO2 in water, modifying the surface of the photocatalyst is essential to load small Ag nanoparticles with high dispersity, which is difficult to achieve using conventional methods. In this study, ultrasonic reduction (USR) was used as an advanced modification method for photocatalysts with an Ag co-catalyst. Ag/ZnTa2O6 prepared using the USR method exhibited good selectivity towards CO (>90%) evolution and a higher CO formation rate compared to those prepared using the conventional modification methods. High-resolution transmission electron microscopy images of the Ag co-catalyst revealed that Ag nanoparticles with a size of a single nanometre were loaded onto the surface of ZnTa2O6 by the USR method, whereas much larger Ag particles loaded onto it were observed in the case of other methods. Accordingly, a small Ag co-catalyst with a single nanometre size exhibits superior activity towards the selective conversion of CO2 to CO. Thus, we successfully achieved a high CO formation rate with high selectivity using a Ag/ZnTa2O6 photocatalyst prepared via USR.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260050","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

Bioinspired copper-catalysed nitrous oxide reduction with simultaneous N–H or O–H bond oxidation 生物启发的铜催化氧化亚氮还原，同时进行 N-H 或 O-H 键氧化

IF 5 3区化学

Catalysis Science & Technology Pub Date : 2024-09-10 DOI: 10.1039/d4cy00760c

Bruce A. Lobo Sacchelli, Suellen M. P. Onguene, Ruben S. M. Almeida, Alexandra M. M. Antunes, Dmytro S. Nesterov, Leandro H. Andrade, Elisabete C. B. A. Alegria, Martin H. G. Prechtl

{"title":"Bioinspired copper-catalysed nitrous oxide reduction with simultaneous N–H or O–H bond oxidation","authors":"Bruce A. Lobo Sacchelli, Suellen M. P. Onguene, Ruben S. M. Almeida, Alexandra M. M. Antunes, Dmytro S. Nesterov, Leandro H. Andrade, Elisabete C. B. A. Alegria, Martin H. G. Prechtl","doi":"10.1039/d4cy00760c","DOIUrl":"https://doi.org/10.1039/d4cy00760c","url":null,"abstract":"Herein, we report on a bioinspired reduction of nitrous oxide in the presence of hydrogen-donating molecules, which are simultaneously oxidised. The copper-/TEMPO-based molecular catalyst has been previously reported to oxidise, for example, alcohols to aldehydes, diols to lactones, amines to imines, and, more recently, for the N-formylation of amines with methanol using (aerial) oxygen as a terminal oxidant. In this report, we demonstrate that it is possible to decompose nitrous oxide, a natural greenhouse gas and industrial waste gas, at low temperatures. This process simultaneously enables the oxidation of amines to imines and the formation of aminoacetal/aminal through the addition and oxidation of methanol. In this context, the Cu/TEMPO catalyst mimics nitrous oxide reductase (N2OR) and alcohol oxidase (AO) simultaneously. The catalyst is formed in situ from inexpensive and commercially available precursors. Selectivities and yields can be controlled by varying the composition of the substrate mixture and oxidant. This approach is attractive for the synthetic valorisation of organic molecules and utilisation of nitrous oxide, which remains a critical greenhouse gas and a byproduct of large-scale industrial processes, such as fertilizer production. These reactions, facilitated by a robust and affordable catalyst, are easy to carry out, making them highly practical for industrial applications.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142205439","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

Influence of redox treatments on the low-temperature water gas shift reaction over Pt/CeO2 catalysts 氧化还原处理对 Pt/CeO2 催化剂上的低温水气变换反应的影响

IF 5 3区化学

Catalysis Science & Technology Pub Date : 2024-09-09 DOI: 10.1039/d4cy00741g

Clément Molinet-Chinaglia, Elizabeth Vera, Philippe Vernoux, Laurent Piccolo, Stéphane Loridant

{"title":"Influence of redox treatments on the low-temperature water gas shift reaction over Pt/CeO2 catalysts","authors":"Clément Molinet-Chinaglia, Elizabeth Vera, Philippe Vernoux, Laurent Piccolo, Stéphane Loridant","doi":"10.1039/d4cy00741g","DOIUrl":"https://doi.org/10.1039/d4cy00741g","url":null,"abstract":"Pt/CeO2 catalysts are promising for the low-temperature water gas shift (LT-WGS) reaction, which is an important step to produce H2 from syngas. When prepared by impregnation of platinum salt and calcination at 500 °C, they contain Pt2+ single atoms (SAs) and/or PtOx clusters which need to be converted into Pt0 nanoparticles (NPs) to obtain higher activity for the LT-WGS reaction. In this work, it was shown that reducing pretreatments at 250 °C under H2 promote the molar activity of catalysts containing from 0.10 to 1.06 wt% Pt by increasing the number of Pt0 NPs formed during reaction at 230 °C. An improvement was also obtained via pretreatment at 500 °C but only for low-Pt-content catalysts, underlying the importance of the pretreatment temperature. Furthermore, it was shown that all prepared Pt/CeO2 catalysts which slowly deactivate over reaction time can be regenerated by oxidative post-treatment at only 230 °C, which is industrially interesting. Even more original, a strong improvement in activity of the low-Pt-content catalysts was observed after a 12 h oxidative post-treatment at 500 °C. This treatment was shown to redisperse and reoxidize Pt atoms into PtOx species different from the initial ones. Such species are highly reducible on the surface of CeO2 and easily transformed into active Pt0 NPs.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260048","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

Theoretical insights into Pt–Rh alloy nanoparticles: stability, elemental distribution, and catalytic mechanisms for NO + CO reactions 铂铑合金纳米颗粒的理论见解：稳定性、元素分布以及 NO + CO 反应的催化机理

IF 5 3区化学

Catalysis Science & Technology Pub Date : 2024-09-09 DOI: 10.1039/d4cy00755g

Yuzheng Li, Xianbao Duan, Zhang Liu, Caoran Li, Fangwen Ye, Zhihong Zhang, Liuqing Chen, Chun Du, Qingbo Wang, Bin Shan

{"title":"Theoretical insights into Pt–Rh alloy nanoparticles: stability, elemental distribution, and catalytic mechanisms for NO + CO reactions","authors":"Yuzheng Li, Xianbao Duan, Zhang Liu, Caoran Li, Fangwen Ye, Zhihong Zhang, Liuqing Chen, Chun Du, Qingbo Wang, Bin Shan","doi":"10.1039/d4cy00755g","DOIUrl":"https://doi.org/10.1039/d4cy00755g","url":null,"abstract":"Pt–Rh bimetallic alloys hold significant promise in catalysis. This study theoretically delves into the stable configurations and elemental distributions of Pt–Rh alloy nanoparticles (NPs) and their influence on the NO + CO catalytic reaction. Initially, a comprehensive dataset for the Pt–Rh system is compiled via calculations based on density functional theory (DFT), followed by developing machine learning potential with accuracy akin to DFT. By employing hybrid Monte Carlo/molecular dynamics simulations, the study unveils that the octahedron-shaped NP is the most stable. Elemental distribution analysis highlights the prevalence of Rh atoms within the interior, particularly in the sub-surface layer, with Pt atoms predominantly occupying the top-surface layer. Building upon these insights, four surface models are crafted and their catalytic efficacy in the NO + CO reaction is evaluated via DFT calculations. The findings indicate that Pt atoms at the top-surface foster N2 recombination, Rh atoms facilitate NO dissociation, while Rh atoms in the sub-surface layer modestly enhance both processes. Hence, Pt–Rh alloy NPs featuring surfaces with both Pt and Rh atoms, with a dominance of Rh atoms in the sub-surface layer, are poised to demonstrate bifunctional catalytic prowess in the NO + CO reaction. This study offers crucial guidance for designing bifunctional catalysts for exhaust gas treatment.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142205435","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

Efficient LED-driven MOF-catalysis for aerobic C–H and C–C bond oxidation 发光二极管驱动的 MOF 催化有氧 C-H 和 C-C 键氧化作用

IF 5 3区化学

Catalysis Science & Technology Pub Date : 2024-09-05 DOI: 10.1039/d4cy00892h

Mehdi Sheykhan, Mona Bahmani, Masoumeh Abbasnia

引用次数: 0

Directed evolution of C-methyltransferase PsmD for enantioselective pyrroloindole derivative production 定向进化 C-甲基转移酶 PsmD，实现对映体选择性生产吡咯吲哚衍生物

IF 5 3区化学

Catalysis Science & Technology Pub Date : 2024-09-05 DOI: 10.1039/d4cy00657g

Diana A. Amariei, Julia Tenhaef, Thomas Classen, Benoit David, Tobias M. Rosch, Holger Gohlke, Stephan Noack, Jörg Pietruszka

{"title":"Directed evolution of C-methyltransferase PsmD for enantioselective pyrroloindole derivative production","authors":"Diana A. Amariei, Julia Tenhaef, Thomas Classen, Benoit David, Tobias M. Rosch, Holger Gohlke, Stephan Noack, Jörg Pietruszka","doi":"10.1039/d4cy00657g","DOIUrl":"https://doi.org/10.1039/d4cy00657g","url":null,"abstract":"The natural product physostigmine is known for its capacity to inhibit acetylcholinesterase (AChE). The pyrroloindole-based scaffold of physostigmine is prevalent among various compounds demonstrating AChE inhibition, suggesting that its structural diversification holds promise as a strategy for the development of novel AChE inhibitors. The C-methyltransferase PsmD is involved in the biosynthesis of physostigmine. While the two described variants from Streptomyces griseofuscus and Streptomyces albulus display an extended substrate range, their specificity hinders the efficient methylation of substrate derivatives. In order to improve the activity of PsmD towards voluminous non-natural substrates, we employed an iterative saturation mutagenesis strategy, which led to an increase in the available space in the catalytic site, while maintaining stereoselectivity. To aid our efforts and provide an efficient platform for the evolution of pyrroloindole-forming enzymes, we developed a modular automated process for the expression, enzymatic reaction and activity screening of the obtained mutant libraries, using an integrated robotic system. In this way, we identified multiple mutants, which led to increased specific activity towards our target substrates. Our results enabled the identification of amino acid position 166 as a key site for the modulation of substrate specificity. We immobilized the best mutant W166C, and used it for the preparative synthesis of an AChE inhibitor, in the presence of a SAM cofactor recycling system.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142205440","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

Synergistic effect of Pd/CZO catalysts and an electric field on complete combustion of lean and humid methane at low temperatures Pd/CZO 催化剂和电场对低温下完全燃烧贫湿甲烷的协同效应

IF 5 3区化学

Catalysis Science & Technology Pub Date : 2024-09-04 DOI: 10.1039/d4cy00699b

Kei Sugiura, Takuma Higo, Nobuki Matsumoto, Harunobu Tedzuka, Yasushi Sekine

{"title":"Synergistic effect of Pd/CZO catalysts and an electric field on complete combustion of lean and humid methane at low temperatures","authors":"Kei Sugiura, Takuma Higo, Nobuki Matsumoto, Harunobu Tedzuka, Yasushi Sekine","doi":"10.1039/d4cy00699b","DOIUrl":"https://doi.org/10.1039/d4cy00699b","url":null,"abstract":"The elimination of unburned methane produced by internal combustion engines is extremely important because of the strong greenhouse effect of methane. Difficulties in controlling unburned methane arise from its characteristics, such as its difficulty of adsorption, low exhaust gas temperatures in an efficient engine, low concentrations of unburned emitted methane, and the coexistence of steam and residual oxygen as coexisting substances in the exit gas. Results of the present study demonstrate that the removal activity of methane by complete combustion was improved dramatically at low temperatures by the application of a DC electric field to the Pd/CexZr1−xO2 catalyst system, even under a humid atmosphere. Specifically, 1 wt% Pd/Ce0.25Zr0.75O2 showed very higher methane conversion under humid conditions than under dry conditions at 473 K in the presence of an electric field. To elucidate the reaction mechanisms involved in this process of steam adsorption, we conducted partial pressure dependence tests and activity tests with steam under an electric field.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142205467","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

Recent progress in heterogeneous CO2 hydrogenation to formic acid towards practical application 二氧化碳异相加氢制甲酸走向实际应用的最新进展

IF 5 3区化学

Catalysis Science & Technology Pub Date : 2024-09-04 DOI: 10.1039/d4cy00798k

Kwangho Park, Hongjin Park, Hayoung Yoon, Kyung Rok Lee, Sunghee Ahn, Changsoo Kim, Ung Lee, Kwang-Deog Jung, Sungho Yoon

引用次数: 0

Reducing meso-lactide formation from racemic lactic acid using shape-selective H-Beta zeolite 利用形状选择性 H-Beta 沸石减少外消旋乳酸生成中乳酸

IF 5 3区化学

Catalysis Science & Technology Pub Date : 2024-09-03 DOI: 10.1039/d4cy01046a

Ling Ding, Lou Gao, Di Pan, Ke Du, Jiayu Yu, Wanyi Li, Yahong Zhang, Yi Tang

{"title":"Reducing meso-lactide formation from racemic lactic acid using shape-selective H-Beta zeolite","authors":"Ling Ding, Lou Gao, Di Pan, Ke Du, Jiayu Yu, Wanyi Li, Yahong Zhang, Yi Tang","doi":"10.1039/d4cy01046a","DOIUrl":"https://doi.org/10.1039/d4cy01046a","url":null,"abstract":"The utilization of racemic lactic acid (rac-LA) produced via chemocatalytic conversion for polylactic acid (PLA) synthesis remains limited due to the formation of undesired mesomeric lactide (meso-LD), a by-product that arises during the conversion process. This study proposes the use of shape-selective H-Beta zeolite to reduce the formation of meso-LD in lactide (LD) by leveraging its selectivity towards different lactic dimers (L2A) in a one-step catalytic conversion of rac-LA to LD. Experimental results from various LA solutions with different L2A content indicate that the L2A content is critical for maximizing the selectivity of racemic lactide (D/L-LD), thus confirming the shape-selective nature of H-Beta zeolite towards L2A. Additionally, it is found that increasing the reaction temperature and employing structurally reconstructed H-Beta zeolite with more regularized channels as a catalyst can further decrease meso-LD formation, and a LD yield of 60% with a D/L-LD/meso-LD ratio of 2.26 can be achieved under optimal catalyst and reaction conditions. Despite the coexistence of D/L-LD and meso-LD in the final product, this study marks a significant step towards controlling the stereoisomer distribution of LD synthesized from rac-LA derived from chemical conversion.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142260051","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