Molecular Catalysis最新文献

{"title":"Enzymatic and convenient synthesis of polyhydroxyalkyl pyrroles from unprotected sugars, benzoylacetonitriles, and NH4OAc/Benzylamines in water","authors":"Jinglin Ma ,&nbsp;Fengxi Li ,&nbsp;Hanqing Xie ,&nbsp;Chunyu Wang ,&nbsp;Wenhan Shi ,&nbsp;Lei Wang ,&nbsp;Peng Chen ,&nbsp;Zhi Wang","doi":"10.1016/j.mcat.2024.114725","DOIUrl":"10.1016/j.mcat.2024.114725","url":null,"abstract":"<div><div>A lipase-catalyzed, mild and environmentally friendly synthesis of polyhydroxyalkyl pyrroles from various unprotected sugars, benzoylacetonitriles and NH₄OAc/benzylamine in water was reported for the first time in this work. Moreover, the synthetic potentiality of this enzymatic method was demonstrated by easy isolation of the final products using filtration. This green synthesis and purification approach not only enriches the strategies for synthesis of polyhydroxyalkyl pyrroles, but also expands the application of lipase in organic synthesis.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"572 ","pages":"Article 114725"},"PeriodicalIF":3.9,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142757604","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}

{"title":"10-camphor sulfonic acid: A simple and efficient organocatalyst to access anti-SARS-COV-2 Benzoxanthene derivatives","authors":"Jayalakshmi M ,&nbsp;Jyothis Devasia ,&nbsp;Sampath Chinnam ,&nbsp;Aatika Nizam ,&nbsp;Ganga Periyasamy ,&nbsp;Pankaj Wadhwa ,&nbsp;Suresh Babu Naidu Krishna","doi":"10.1016/j.mcat.2024.114691","DOIUrl":"10.1016/j.mcat.2024.114691","url":null,"abstract":"<div><div>10-Camphor sulfonic acid (10-CSA) has gained popularity as an organocatalyst due to its broad range of solubility and user-friendliness. Affordable multicomponent reactions (MCRs) for the preparation of benzoxanthenes (4a-4 h) (5a-5i) are presented in this work. Extensive investigations and records have been conducted on the diverse biological features exhibited by xanthenes and benzoxanthenones, such as their antiviral, antibacterial, and anti-inflammatory capabilities.Using β-naphthol, dimedone, and aldehydes, we demonstrate a cost-effective and environmentally friendly catalytic method. Under ideal circumstances, the 10-CSA catalyzes one-pot reaction, procuring impressive amounts of benzoanthenes (85–95 %). All the synthesized compounds were characterized by ¹H NMR and ¹³C NMR. A wide variety of suitable chemicals, simple work-up procedures, and solvent-free synthesis outperforms numerous existing methods for procuring biologically relevant benzoxanthene derivatives are some of the interesting features of this organocatalyzed bronsted acid process. Therefore this synthesis is industrially inevitable. Furthermore, computational studies such as molecular docking and ADMET data analysis were performed on a number of the synthesized benzoxanthene molecules. This has led to the identification of the most potent synthetic against the SARS-CoV-2 spike protein. Additionally, to mimic how medicinal compounds interact to target proteins, computational docking and dynamics techniques were used. These studies showed that, in terms of binding affinity and other crucial traits, 4a, 4b, and 5a are potential possibilities. Overall, the current study should be of great help in the development of benzoxanthene analogs which can be potential drugs for treatment of COVID-19.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"572 ","pages":"Article 114691"},"PeriodicalIF":3.9,"publicationDate":"2024-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142748005","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}

{"title":"Hydrotalcite-derived well-dispersed and thermally stable cobalt nanoparticle catalyst for ammonia decomposition","authors":"Xiaofeng Wei,&nbsp;Jiaxin Su,&nbsp;Yuyin Ji,&nbsp;Hongyang Huang,&nbsp;Dalin Li,&nbsp;Huihuang Fang,&nbsp;Chongqi Chen,&nbsp;Yu Luo,&nbsp;Lilong Jiang","doi":"10.1016/j.mcat.2024.114741","DOIUrl":"10.1016/j.mcat.2024.114741","url":null,"abstract":"<div><div>Ammonia is a carbon-free hydrogen carrier, and development of non-noble metal catalyst to decompose ammonia into hydrogen is desirable for practical applications. However, the metal catalyst is challenged by the sintering of metal particles under high-temperature reaction conditions. In this study, a series of Li-, Al-, and Co-containing hydrotalcite-like compounds (HTlc) were synthesized by co-precipitation and used as precursors to prepare well-dispersed and thermally stable Co nanoparticle catalysts for ammonia decomposition. The obtained precursors and catalysts were characterized by means of X-ray powder diffraction (XRD), temperature-programmed reduction (H₂-TPR), X-ray photoelectron spectroscopy (XPS), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), and so on. All of the precursors formed hydrotalcite-like phase, which consisted of Li–Al–(Co) HTlc and/or Co–Al HTlc dependent on the Co content. Upon calcination at 500 °C, HTlc decomposed into an Al-substituted Co₃O₄ spinel oxide, as confirmed by two distinctly separated reduction steps in H₂-TPR. Following reduction at 700 °C, well-dispersed Co metal nanoparticles with an average particle size of ∼9.2–12.4 nm were obtained. It was suggested that the incorporation of Al³⁺ into Co₃O₄ led to a strong interaction between cobalt and aluminum, which suppressed the crystal growth of Co₃O₄ and the sintering of Co metal during the thermal treatments, resulting in good Co dispersion. The optimal LiAlCo(1.5) catalyst showed superior activity than that prepared by impregnation method, giving almost complete conversion of ammonia at 575 °C under a space velocity of 5,000 mL g_cat^–1 h^–1. More importantly, this catalyst maintained stable activity at 625 °C for 100 h, exhibiting high stability and sintering resistance. The good catalytic performance was attributed to the high Co metal dispersion and strong metal–support interaction benefiting from the uniform distribution of cobalt in the HTlc precursor. These results demonstrate the applicability of HTlc to the preparation of metal catalysts with improved dispersion and thermal stability.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"572 ","pages":"Article 114741"},"PeriodicalIF":3.9,"publicationDate":"2024-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142747912","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}

{"title":"Molecular oxygen uptake behavior of crystalline porous complex metal oxide based on ε-Keggin polyoxometalate unit framework","authors":"Satoshi Ishikawa ,&nbsp;Hirokazu Nito ,&nbsp;Wataru Ueda","doi":"10.1016/j.mcat.2024.114723","DOIUrl":"10.1016/j.mcat.2024.114723","url":null,"abstract":"<div><div>ε-Keggin polyoxometalate based complex metal oxides are composed of the structural arrangement of ε-Keggin [Mo₁₂O₄₀], which connects with octahedral linker, {MO₆}, to form a microporous structure that localizes counter cations X similar to FAU-type zeolites. In the present study, O₂ adsorption properties of these materials (ε-[X]MoMO) are investigated. ε-[X]MoCoO with X = Fe and Cu showed significant O₂ adsorption in an irreversible manner and the adsorption amount was saturated when 1.0 of O₂ was adsorbed in the unit cell. The ε-Keggin unit of these materials were oxidized after the O₂ adsorption at room temperature, resulting in the shrinkage of their lattice. Based on the characterization results and adsorption behavior, we suggest the O₂ adsorption behavior as follows; O₂ can freely access the whole ε-Keggin unit in ε-[Fe or Cu]MoCoO through the micropores involving redox between O₂ and the ε-Keggin unit. The oxidation of this unit reduces the lattice size, which slows down the migration of O₂ and results in the quasi-equilibrium adsorption near the surface. The selection of M element in ε-[Fe]MoMO was also crucial for the O₂ adsorption.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"572 ","pages":"Article 114723"},"PeriodicalIF":3.9,"publicationDate":"2024-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142747911","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}

{"title":"When less is more: Ligand and solvent effects in Ni2+ Lewis acid transfer hydrogenation coupled with aldol condensation","authors":"Nicholas L. Gadinas,&nbsp;Emily A. Anderson,&nbsp;Konstantinos A. Goulas","doi":"10.1016/j.mcat.2024.114711","DOIUrl":"10.1016/j.mcat.2024.114711","url":null,"abstract":"<div><div>The coupling of furfural with aliphatic alcohols can yield precursor molecules for the production of high-performance detergents. In the present work, we use Ni-based homogeneous catalysts for this transformation and specifically examine ligand, solvent and base effects. We show that chloride and phosphine-ligated Ni catalysts exhibit long induction periods, while Ni catalysts with O ligands do not. We use operando X-ray absorption spectroscopy to attribute this induction to the requirement for the P and Cl ligand substitution during reaction. Solvent effect experiments demonstrate that hydrocarbon solvents, such as toluene and cyclohexane show the highest performance, while tert‑butanol is least optimal. Potassium carbonate as a base shows highest rates, while amine bases require higher temperatures and excess furfural to achieve equivalent product yields.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"572 ","pages":"Article 114711"},"PeriodicalIF":3.9,"publicationDate":"2024-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142757407","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}

{"title":"In-situ confinement growth of FeNi alloy within B/N co-doped carbon nanotubes as efficient electrocatalyst for water splitting","authors":"Shide Wu ,&nbsp;Yapeng Li ,&nbsp;Dan Ping ,&nbsp;Weitao Liu ,&nbsp;Yichen Feng ,&nbsp;Qingshuo Zhang ,&nbsp;Mengjin Gao ,&nbsp;Shuqing Liu ,&nbsp;Di Wu ,&nbsp;Shiwen Wang ,&nbsp;Jianqiang Zhang ,&nbsp;Shaoming Fang","doi":"10.1016/j.mcat.2024.114737","DOIUrl":"10.1016/j.mcat.2024.114737","url":null,"abstract":"<div><div>Developing low-cost and efficient catalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) still remains a challenge in water electrolysis. Herein, FeNi alloy encapsulated within boron and nitrogen co-doped carbon (FeNi@BNC) nanotubes are synthesized through a simple one-step pyrolysis method using FeCl₃·6H₂O, NiCl₂·6H₂O, H₃BO₃, urea and PEG-2000 as precursors. The BNC nanotubes are quite requisite for dispersing and stabilizing FeNi alloy nanoparticles (NPs) during pyrolysis. Benefiting from the synergistic catalytic effect of Fe and Ni, as well as the confinement effect of BNC nanotubes, such FeNi@BNC catalyst demonstrates impressive activities for both HER and OER, much superior to pristine Fe@BNC and Ni@BNC. Notably, the overpotentials needed to achieve a current density of 10 mA·cm⁻² are just 230 mV for HER and 280 mV for OER. Moreover, the FeNi@BNC catalyst demonstrates significant stability, showing no noticeable degradation during potentiostatic electrolysis or repeated CV tests. Furthermore, FeNi@BNC exhibits remarkable activity for overall water splitting, requiring cell voltages of just 1.24 V and 1.60 V vs. RHE to achieve current densities of 10 mA·cm⁻² and 20 mA·cm⁻², respectively. This study introduces a novel strategy for developing bifunctional electrocatalysts with high-efficiency water splitting performance.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"572 ","pages":"Article 114737"},"PeriodicalIF":3.9,"publicationDate":"2024-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142748004","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}

{"title":"Regulating the electronic state of MFI zeolite encapsulated Pt nanoparticles to boost the atom efficiency in reductive amination of biomass-derived furfural","authors":"Meng Xu ,&nbsp;Xiaoling Liu ,&nbsp;Zhuo Xiong ,&nbsp;Yue Wu ,&nbsp;Zhen Meng ,&nbsp;Yu Zhou ,&nbsp;Jun Wang","doi":"10.1016/j.mcat.2024.114740","DOIUrl":"10.1016/j.mcat.2024.114740","url":null,"abstract":"<div><div>Furfural is an abundant biomass-derived building block that can be converted into furan-based N-containing compounds through direct reductive amination by using dihydrogen (H₂). Nonetheless, the synthesis of furan-based tertiary amines is highly limited <em>via</em> this route. Herein, we reported the straightforward synthesis of MFI zeolite encapsulated Pt nanoparticles and finely modulated the surface electronic state by facilely controlling the reduction process. The constructed catalyst Pt@Z5 effectively catalyzed the amination of furfural with diethylamine for the synthesis of N-ethyl-N-(furan-2-ylmethyl)ethanamine, affording the high yield (&gt;95 %), large turnover number (TON) of 2058, turnover frequency (TOF) of 1029 <em>h</em>⁻¹, and stable recyclability. Systematic investigations comprising <em>in-situ</em> Fourier transform infrared spectroscopy (FTIR) spectra and kinetic isotope effect (KIE) unraveled that the mild reduction condition allowed the catalyst with a superior affinity towards H atom and beneficial furfural adsorption behavior, accelerating the H₂ activation in the rate-determining step for the conversion of furfural into furan-based amine.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"572 ","pages":"Article 114740"},"PeriodicalIF":3.9,"publicationDate":"2024-11-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142747910","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}

{"title":"Catalytic oxidation of low-carbon polyols to primary carboxylic acids: Advances on catalyst design and mechanistic studies","authors":"Yaqian Li,&nbsp;Xiuhui Zheng,&nbsp;Jie Li,&nbsp;Jiarong Lu,&nbsp;Rong Fan,&nbsp;Mengnan Ma,&nbsp;Yibin Liu,&nbsp;Hao Yan,&nbsp;Xiang Feng,&nbsp;Chaohe Yang","doi":"10.1016/j.mcat.2024.114706","DOIUrl":"10.1016/j.mcat.2024.114706","url":null,"abstract":"<div><div>Catalytic oxidation of low-carbon polyols to primary carboxylic acids is regarded as an important technology for sustainable traditional oxidation processes in industry. Despite decades of research and several breakthroughs in catalyst design, the precise reaction mechanism underlying the formation of specific carboxylic acids remains elusive. In this review, the oxidation of low-carbon polyols to primary carboxylic acids over metallic catalysts is systematically summarized with a focus on surface reaction mechanisms and catalyst design strategies. Essentially, the activation of C-H bond and the competitive adsorption/desorption of oxygen-containing intermediates serve as critical issues in determining the reaction mechanism. Insights into the reaction mechanism, the structure-performance relationships of oxophilic metal-based catalysts in various low-carbon polyol oxidation reactions lay the groundwork for rational catalyst design and manufacturing: (I) well-dispersed acidic sites can enhance the electronic density of oxophilic metals, thereby improving the H abstraction efficiency, while an adequate number of weak basic sites on the surface is beneficial for the adsorption of oxygen-containing intermediates; (II) the downshifted d-band center of oxophilic metal sites results in greater catalytic efficiency for C-H bond activation. This review aims to provide a comprehensive understanding of oxidation mechanisms and guide the rational design of efficient catalysts.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"572 ","pages":"Article 114706"},"PeriodicalIF":3.9,"publicationDate":"2024-11-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142747913","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}

{"title":"Hollow Pt/CeO2 nanocatalysts pretreated with pulsed steam for enhanced CO oxidation performance","authors":"Mingzhen Huang,&nbsp;Jinxin He,&nbsp;Kaiji Xu,&nbsp;Dongren Cai,&nbsp;Guowu Zhan","doi":"10.1016/j.mcat.2024.114720","DOIUrl":"10.1016/j.mcat.2024.114720","url":null,"abstract":"<div><div>The supported Pt/CeO₂ catalysts are widely used for the catalytic oxidation of CO at ambient conditions. Herein, we reported a new strategy for modifying the interaction between Pt and CeO₂ support via pulsed steam treatment, which significantly optimized the catalytic performance of Pt/CeO₂ for CO oxidation. Specifically, the hollow CeO₂ nanospheres were prepared by using carbon spheres as sacrificial templates and then subjected to pulsed steam treatment at 150 °C for different times to obtain the CeO₂-xH support (x means the time of pulsed steam treatment, min). It was found that the complete oxidation of CO can be achieved at 90 °C over the Pt/CeO₂–50H sample, which was much lower than that (130 °C) on Pt/CeO₂ without pulsed steam treatment. The XPS and <em>in-situ</em> DRIFTS characterizations were conducted to reveal the high performance of the Pt/CeO₂–50H catalyst for CO oxidation. It was found that the valence state of Pt significantly controlled by pulsed steam treatment was critical to the catalytic activity, whereby the presence of two types of active sites (Pt⁰-CO and Pt^δ+-CO) over Pt/CeO₂–50H greatly promoted the combination of adsorbed CO and O₂ to generate CO₂. Accordingly, this study provides a facile method to regulate the Pt valence state by pulsed steam treatment for CeO₂ support, which is critical to the CO oxidation activity.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"572 ","pages":"Article 114720"},"PeriodicalIF":3.9,"publicationDate":"2024-11-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142748007","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}

{"title":"Multi-amino functionalized triazine-based polymers as the catalyst for cycloaddition of CO2 to epoxides","authors":"Chaokun Yang ,&nbsp;Xin Wang ,&nbsp;Xin Zhao","doi":"10.1016/j.mcat.2024.114724","DOIUrl":"10.1016/j.mcat.2024.114724","url":null,"abstract":"<div><div>Designing efficient catalysts for CO₂ cycloaddition to reduce CO₂ emission is one of crucial for environmental issues technology. Herein, the multiple-amino functionalized triazine-based polymer (MAFTP) was prepared through the nucleophilic reaction of cyanuric chloride with melamine and ethylenediamine by a conventional heating method, which are favorable for CO₂ adsorption due to their nitrogen-rich structure. MAFTP was characterized entirely, the CO₂ adsorption capacity of MAFTP showed the CO₂ uptake performance with the values of 5.73 cm³ <em>g</em>⁻¹ at 273 K and 1 bar. MAFTP/KI catalyst exhibited efficient catalytic activity for CO₂ fixation to epoxides. 99 % propylene carbonate yield and 99 % selectivity were obtained under 120 °C, 2.0 MPa for 2.0 h without organic solvent. Additionally, the catalysts could be recycled easily from the products after reaction by centrifugation and then reused 5 times efficiently. Meanwhile, the catalytic activity of MAFTP/KI to other substituted epoxides was discussed. Moreover, DFT calculation was adopted to analyze the possible cycloaddition reaction mechanism. The MAFTP/KI system is a promising candidate for CO2 chemical fixation attributing to the low cost, abundant availability, easy separation and high catalytic activity for CO₂ chemical fixation.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"572 ","pages":"Article 114724"},"PeriodicalIF":3.9,"publicationDate":"2024-11-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142747906","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}