Catalysis Science & Technology最新文献

{"title":"Hydrogen production through photocatalytic acceptorless alcohol dehydrogenation with a homogeneous nickel complex","authors":"Eman Mohamad and Darrin Richeson","doi":"10.1039/D5CY00647C","DOIUrl":"https://doi.org/10.1039/D5CY00647C","url":null,"abstract":"<p >The need for sustainable hydrogen production has driven the search for efficient, earth-abundant catalysts. We report a breakthrough in photocatalytic acceptorless alcohol dehydrogenation (AAD) using a well-defined, air-stable nickel(<small>II</small>) complex, [Ni(2,6-{Ph<small>₂</small>PNH}<small>₂</small>(NC<small>₅</small>H<small>₃</small>))Br]<small>⁺</small> (<strong>1</strong><small>⁺</small>) which represents the first fully characterized nickel complex to catalyze photocatalytic AAD. This catalyst operates at room temperature under visible light irradiation to selectively produce hydrogen from various aliphatic alcohols. Catalyst performance is significantly enhanced by introducing dimethylethanolamine (DMEA) as an efficient electron donor, an electron donor previously unexplored in photoredox reactions. Mechanistic studies, supported by computational analysis, reveal the crucial role of the flexible pincer ligand in facilitating the catalytic cycle. The proposed transformation of the “PN<small>³</small>P” ligand to a bidentate PN configuration, supported by DFT optimization, creates an open coordination environment at the nickel centre, key for β-hydrogen elimination. This work addresses challenges in hydrogen production and bridges the gap between traditional catalysis and photoredox chemistry and represents a significant step towards more economical and environmentally friendly hydrogen generation.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 19","pages":" 5747-5752"},"PeriodicalIF":4.2,"publicationDate":"2025-08-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cy/d5cy00647c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183989","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}

{"title":"High-efficiency transalkylation of C10 aromatics with 2-methylnaphthalene over shape-selective SiO2-Cu-HMOR with nanoneedle crystals","authors":"Jiahao Wang, Qihao Yang and Junhui Li","doi":"10.1039/D5CY00469A","DOIUrl":"https://doi.org/10.1039/D5CY00469A","url":null,"abstract":"<p >Here, a nanoneedle HMOR zeolite modified by loading 2.5 wt% Cu and subsequently by SiO<small>₂</small> deposition with four cycles was designed as a catalyst for the transalkylation of C<small>₁₀</small> aromatics with 2-methylnaphthalene (2-MN) for synthesizing 2,6-dimethylnaphthalene (2,6-DMN) in a H<small>₂</small> atmosphere. Firstly, a remarkably improved transalkylation reactivity for dimethylnaphthalene generation (catalyzed by protonic acid sites) was achieved depending on two key factors: (1) a probable concerted catalysis of the internal metal-Cu and acid sites under a H<small>₂</small> atmosphere; (2) the high-efficiency diffusion of the molecules into/out the shorter and shape-selective micropores of modified nanoneedle crystals. Secondly, the side-reactions resulting in multi-alkylnaphthalene formation and naphthalene-ring loss were effectively suppressed, and the greatly enhanced selectivities of 2,6-DMN and β,β-dimethylnaphthalenes were also obtained. It is due to the combined effects of the elimination of external reactive sites, the interspace limitation inside channels, and the product shape-selectivity at the reasonably narrowed pore-openings. Furthermore, the catalyst also exhibited good catalytic stability attributed to its strong capabilities of resisting coke deposition depending on reasonable hydrogenation catalyzed by metal Cu sites and high-efficiency molecule diffusion of short channels, and accommodating considerable coke on its nanoneedle crystals. As a result, a 2-MN conversion of &gt;73.78%, a dimethylnaphthalene selectivity of &gt;85.98%, and a 2,6-DMN yield of &gt;19.56% were obtained during a 180 h on-stream reaction.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 19","pages":" 5782-5793"},"PeriodicalIF":4.2,"publicationDate":"2025-08-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183999","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}

{"title":"Catalytic valorisation of d-fructose and alcohols using silica–PEI–polyoxometalate composites","authors":"Israel T. Pulido-Díaz, Itzel Guerrero-Ríos and Dominique Agustin","doi":"10.1039/D5CY00465A","DOIUrl":"https://doi.org/10.1039/D5CY00465A","url":null,"abstract":"<p >A nano-catalyst composed of polyoxometalates (POMs) ionically immobilized on polyethyleneimine (PEI) functionalized silica (SiO<small>₂</small>–[PEIH]<small>_<em>x</em></small>[POM]) was used for the dehydration of <small>D</small>-fructose to 5-hydroxymethylfurfural (HMF) and the subsequent oxidation of HMF to 2,5-diformylfuran (DFF). The morphology and textural properties of silica supports, SBA-15 and Stöber nanoparticles, influenced the catalytic outcome. SiO<small>₂</small>–[PEIH]<small>_<em>x</em></small>[POM] demonstrated high thermal stability and exceptional catalytic activity in fructose transformation. Using DMSO as solvent in a one-pot synthesis, we achieved an HMF yield of 95% after 0.5 hours at 150 °C and a DFF yield of 69% after 20 hours, whereas HMF oxidation afforded a DFF yield of 86% under the same conditions with a considerable turnover number (TON) of 1720. These findings suggested that SiO<small>₂</small>–[PEIH]<small>_<em>x</em></small>[POM] catalysts are promising candidates for the valorization of fructose into sustainable chemical sources.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 19","pages":" 5794-5806"},"PeriodicalIF":4.2,"publicationDate":"2025-08-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cy/d5cy00465a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183975","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}

{"title":"8-Hydroxyquinoline catalysed regioselective synthesis of 1,4-disubstituted-1,2,3-triazoles: realizing Cu-free click chemistry","authors":"Surbhi Bansal, Gopika R. Sreerekha, Ayanangshu Biswas, Alisha Sharma, Devika Girish, Debashis Adhikari and Sanjay Singh","doi":"10.1039/D5CY00598A","DOIUrl":"https://doi.org/10.1039/D5CY00598A","url":null,"abstract":"<p >Despite numerous reports on the Cu-catalysed click reaction and faster rates of reaction using such catalysts, the pharmacological application of this important synthetic method has become limited and hence advancement towards metal-free click chemistry has increasingly grabbed attention in recent years. Herein we report a regioselective synthesis of 1,4-disubstituted-1,2,3-triazoles <em>via</em> a one-pot azide-alkyne cycloaddition reaction under metal-free conditions using the 8-hydroxyquinoline (8-HQ) catalyst. Along with a plethora of simple triazole derivatives, the protocol has been successfully applied to the synthesis of some bioactive compounds incorporating triazole motifs. Thorough control experiments including deuterium-labelling studies support the proposed mechanism for the reaction wherein the catalyst works as both a proton-abstractor and proton-donor synergistically.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 19","pages":" 5850-5856"},"PeriodicalIF":4.2,"publicationDate":"2025-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cy/d5cy00598a?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145184015","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}

{"title":"Protein engineering of cellulase enzymes for enhanced binding to single-walled carbon nanotubes: a computational approach to enzyme recycling in biofuel applications","authors":"Shubhashree Barik, Supriyo Mukherjee and Moumita Saharay","doi":"10.1039/D5CY00460H","DOIUrl":"https://doi.org/10.1039/D5CY00460H","url":null,"abstract":"<p >Cellulases serve as essential biocatalysts in the industrial conversion of cellulosic biomass into bioethanol. Immobilizing these enzymes on carbon nanotubes (CNTs) enhances their recyclability, offering a promising strategy for cost-effective biofuel production. This study investigates the structural dynamics and binding stability of CNT-immobilized cellulases from bacteria and fungi (Cel6A, Cel7A, Cel7D, Cel48F, and CelS) in both wild-type (WT) and the computationally engineered or mutant-type (MT) variants. Initially, molecular docking and network analysis were employed to identify optimal CNT-binding domains in WT enzymes. Targeted mutations, specifically hydrophilic-to-tryptophan substitutions, were introduced in the CNT-binding domain of WT enzymes to enhance π–π interactions between the enzymes and CNTs. Subsequently, molecular dynamics simulations were performed under physiological conditions. We observed that MT enzymes exhibited stronger CNT binding than WT enzymes while maintaining catalytic functionality, with minimal deviation from their native structures. These findings provide valuable insights into enzyme immobilization strategies, enabling the design of biocatalysts for industrial bioprocessing, materials science, and biomedical applications.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 19","pages":" 5893-5906"},"PeriodicalIF":4.2,"publicationDate":"2025-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145184020","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}

{"title":"Bare La2O3 in non-oxidative propane dehydrogenation: in situ decoration of active sites for enhanced catalyst performance","authors":"Tatiana Otroshchenko, Shanlei Han, Thanh Huyen Vuong, Vita A. Kondratenko, Jabor Rabeah, Stephan Bartling and Evgenii V. Kondratenko","doi":"10.1039/D5CY00750J","DOIUrl":"https://doi.org/10.1039/D5CY00750J","url":null,"abstract":"<p >To replace toxic or expensive CrO<small>_<em>x</em></small>- or Pt-based catalysts currently used in large-scale production of propene through non-oxidative dehydrogenation of propane, ecologically friendly and cost-effective alternatives are needed. In this context, we introduce La<small>₂</small>O<small>₃</small> as a promising catalyst for this reaction. Our characterization and catalytic experiments as well as density functional theory calculations revealed that coordinatively unsaturated La<small>³⁺</small> cations (La<small>_cus</small>) possess high activity to the cleavage of the C–H bond in propane. However, they strongly adsorb propene and hydrogen atoms formed from propane, favoring the formation of coke but hindering their recovery by H<small>₂</small> desorption. La<small>_cus</small> can, however, be decorated with hydrogen species in the presence of gas-phase H<small>₂</small>. These new species show high activity for propane activation but low ability to adsorb propene and open a more energetically favorable pathway for H<small>₂</small> formation. La<small>₂</small>O<small>₃</small> does not obviously differ from an industrial analogue of K-CrO<small>_<em>x</em></small>/Al<small>₂</small>O<small>₃</small> in terms of propene selectivity up to 60% equilibrium propane conversion at 600 °C using a feed with 40 vol% C<small>₃</small>H<small>₈</small> and 30 vol% H<small>₂</small> in N<small>₂</small>. The effect of hydrogen on the PDH performance of La<small>₂</small>O<small>₃</small> may inspire other researchers involved in the development of alternative catalysts, which are typically tested in the absence of hydrogen.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 19","pages":" 5737-5746"},"PeriodicalIF":4.2,"publicationDate":"2025-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cy/d5cy00750j?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183988","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}

{"title":"Unveiling the support effect in Pt-based catalysts for the selective catalytic oxidation of NH3 under realistic diesel engine conditions","authors":"Daekun Kim, Shaohua Xie, Kailong Ye, Xing Zhang, Matthew T. Caudle, Lu Ma, Steven N. Ehrlich and Fudong Liu","doi":"10.1039/D5CY00681C","DOIUrl":"https://doi.org/10.1039/D5CY00681C","url":null,"abstract":"<p >Pt catalysts have been widely used for the selective catalytic oxidation of NH<small>₃</small> (NH<small>₃</small>-SCO) in practical applications due to their high activity at low temperatures. However, more stringent regulations require further enhancement of low-temperature NH<small>₃</small>-SCO activity. In this study, we investigated the influence of different supports, including aluminum oxide (Al<small>₂</small>O<small>₃</small>), silica (SiO<small>₂</small>), and chabazite (CHA), on the NH<small>₃</small>-SCO performance of Pt catalysts. Our findings demonstrate that the Pt/CHA catalyst exhibited superior NH<small>₃</small>-SCO performance under realistic diesel engine conditions, characterized by high space velocity and the presence of water vapor. Notably, the Pt/CHA catalyst achieved a significantly lower <em>T</em><small>₅₀</small> (temperature at which 50% NH<small>₃</small> conversion is achieved) of 218 °C under conditions with both CO<small>₂</small> and H<small>₂</small>O, with a 56 °C reduction compared to the state-of-the-art Pt/Al<small>₂</small>O<small>₃</small> catalyst. The exceptional NH<small>₃</small>-SCO performance is attributed to the high abundance of metallic Pt<small>⁰</small> species and the presence of rich and stable acid sites that facilitate NH<small>₃</small> adsorption and activation. These results highlight CHA as a promising support for the Pt catalyst in NH<small>₃</small>-SCO applications for diesel engine emission control.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 19","pages":" 5816-5826"},"PeriodicalIF":4.2,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145184001","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}

{"title":"Computational insights into Ir-catalyzed transfer hydrogenation of CO2 to formate: critical roles of abnormal NHC ligands and hydrogen donors","authors":"Han Gao, Xiaofang Zhai, Feng Ye, Wujie Wang, Gang Lu and Yuliang Li","doi":"10.1039/D5CY00744E","DOIUrl":"https://doi.org/10.1039/D5CY00744E","url":null,"abstract":"<p >A computational study was conducted to elucidate the mechanism of Ir-catalyzed transfer hydrogenation of CO<small>₂</small> to formate, with a particular focus on investigating how abnormal <em>N</em>-heterocyclic carbene (aNHC) ligands and hydrogen donors influence reaction efficiency. The results reveal that β-H elimination serves as the rate-determining step in the catalytic cycle. The dissociation of the Ir–N bond is a prerequisite for the β-H elimination step, which is crucial for the formation of iridium hydride species. Compared to isopropanol, the higher reactivity observed with glycerol is attributed to H-bonding interactions between the dissociated anionic N ligand and the hydroxyl groups of glycerol. The rotational flexibility of aNHC ligands is critical for enhancing the reactivity of β-H elimination, as evidenced by the strong linear correlation between the dihedral angles of free aNHC ligands and the barriers of β-H elimination.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 19","pages":" 5765-5771"},"PeriodicalIF":4.2,"publicationDate":"2025-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183991","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}

{"title":"Correction: Effect of zirconia support crystal structure on the alloying of rhodium and iridium for the improvement of three-way catalysts","authors":"Yoshihide Nishida, Koki Aono, Hirona Yamagishi, Hiromi Togashi, Shunsuke Oishi and Masaaki Haneda","doi":"10.1039/D5CY90063H","DOIUrl":"https://doi.org/10.1039/D5CY90063H","url":null,"abstract":"<p >Correction for ‘Effect of zirconia support crystal structure on the alloying of rhodium and iridium for the improvement of three-way catalysts’ by Yoshihide Nishida <em>et al.</em>, <em>Catal. Sci. Technol.</em>, 2025, DOI: https://doi.org/10.1039/d5cy00561b.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 17","pages":" 5187-5187"},"PeriodicalIF":4.2,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cy/d5cy90063h?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144909547","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}

{"title":"Advances in CO2 capture and utilization: the role of DFT in understanding CO2 activation and its conversion mechanisms for methanol and cyclic carbonates production","authors":"Valeria Butera and Giampaolo Barone","doi":"10.1039/D5CY00658A","DOIUrl":"https://doi.org/10.1039/D5CY00658A","url":null,"abstract":"<p >As the amount of CO<small>₂</small> gas in the atmosphere is significantly increasing, leading to profound global climate changes, growing attention has been addressed to CO<small>₂</small> capture and utilization (CCU) processes, in which CO<small>₂</small> is captured from the atmosphere and used as an abundant and non-toxic building block for the production of added-value products. Two main approaches to convert CO<small>₂</small> into fuels and fine chemicals have been considered: <em>reductive</em> conversions in which the carbon atom is reduced to its lower oxidation states, and <em>non-reductive</em> processes, where the +4 oxidation state of carbon in CO<small>₂</small> is maintained. However, due to the high stability of this inert molecule, both <em>reductive</em> and <em>non-reductive</em> conversions are only possible upon utilization of a proper catalyst. Although the research focus on CCU strategies has been widely spreading, there is still a lack of a comprehensive understanding of the mechanism of CO<small>₂</small> conversion reactions, which is mainly due to the complexity of such conversion processes under reaction conditions. In this context, the contribution of quantum chemical investigations, particularly those based on density functional theory (DFT) calculations, have been of paramount importance to assist traditional experimental methods in a synergic combination able to boost the advancement in the missing knowledge. Based on those considerations, in this review we aim at discussing two main aspects of the CCU process. We will first focus on the importance of CO<small>₂</small> activation, pointing out how DFT investigations help provide crucial insights into the activation strengths. Moreover, we will discuss the contribution of DFT to the understanding of the reaction conversion mechanisms, with a specific focus on two main products: methanol and cyclic carbonates. Eventually, current limitations and future perspectives will be briefly discussed.</p>","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":" 19","pages":" 5574-5601"},"PeriodicalIF":4.2,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145183959","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}