Journal of Catalysis最新文献

{"title":"Consequences of the co-existence of single-atom and nanoparticle catalysts","authors":"Muthuraja Velpandian ,&nbsp;Apurba Sinhamahapatra ,&nbsp;Suddhasatwa Basu","doi":"10.1016/j.jcat.2025.116012","DOIUrl":"10.1016/j.jcat.2025.116012","url":null,"abstract":"<div><div>Single-atom catalysts (SACs) have emerged as promising candidates for electrochemical conversion and storage applications due to their efficient atomic utilization and unique structure, wherein metal atoms are uniformly dispersed and anchored on a support material. This arrangement allows SACs to possess a high density of active sites, maximizing their exposure to reactants and consequently improving reaction rates and selectivity. In light of the growing global demand for renewable and sustainable energy sources, extensive research has been dedicated to designing and fabricating well-defined SAC-based electrocatalysts with optimized electronic structures and diverse compositions over the past decade. Given their exceptional activity and selectivity, particularly for small molecules or key intermediate conversions, the synergistic combination of SACs with nanoparticles (NPs) holds great potential for significantly enhancing performance in complex catalytic processes. In this mini-review, we provide a comprehensive overview of the various possibilities for the co-existence of SACs and nanoparticles, as well as the synthesis and characterization techniques employed in their preparation. Subsequently, we focus on the potential consequences of this co-existence, which has not been extensively explored in the literature, which can lead to improved selectivity towards desire products, thereby boosting the niche applications of these systems. We conclude by emphasizing the major challenges that need to be addressed and highlighting the emerging opportunities in the field of SAC-nanoparticle co-existence systems. By understanding and addressing these challenges, researchers can further advance the development and utilization of hybrid catalyst systems, thereby paving the way for the next generation of efficient and selective catalytic processes.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"445 ","pages":"Article 116012"},"PeriodicalIF":6.5,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418463","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}

{"title":"Visible light-induced radical cascade hydroaminoalkylation involving two distinct alkenes","authors":"Zhu-Ming Qian ,&nbsp;Qin Zhang ,&nbsp;Ya-Nan Zhao ,&nbsp;Zhi Guan ,&nbsp;Chu-Sheng Huang ,&nbsp;Yan-Hong He","doi":"10.1016/j.jcat.2025.116010","DOIUrl":"10.1016/j.jcat.2025.116010","url":null,"abstract":"<div><div>This paper describes a visible-light-mediated three-component dicarbofunctionalization of alkenes via a tandem radical addition reaction of two different alkenes triggered by aminoalkyl radicals derived from <em>N</em>-phenyl glycines. This method allows for one-pot skeletal assembly, providing efficient and straightforward access to structurally complex γ-amino sulfone derivatives directly from readily available and simple starting materials. Beyond the convenience of the one-pot protocol, this method also demonstrates broad substrate scope, excellent functional group compatibility, mild reaction conditions, and ease of scalability.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"445 ","pages":"Article 116010"},"PeriodicalIF":6.5,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418454","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}

{"title":"Photo-induced aerobic deborohydroxylation of organoboron compounds in 1,3-dioxolane at room temperature","authors":"Mingjing Deng ,&nbsp;Ke Liu ,&nbsp;Zhaolun Ma ,&nbsp;Qingsheng Qi ,&nbsp;Longyang Dian","doi":"10.1016/j.jcat.2025.116006","DOIUrl":"10.1016/j.jcat.2025.116006","url":null,"abstract":"<div><div>We report herein a simple and efficient light-induced aerobic oxidation of organoboron compounds to obtain phenols in an air atmosphere at room temperature, without the use of any photocatalyst, oxidant or other reagent. This protocol utilizes inexpensive and commercially available 1,3-dioxolane as both the solvent and electron donor to activate the molecular oxygen in the air under 365 nm light, enabling the aerobic oxidation to occur under mild reaction conditions. A wide range of sensitive functional groups are well tolerated, resulting in the corresponding phenols in moderate to good yields.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"445 ","pages":"Article 116006"},"PeriodicalIF":6.5,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418461","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}

{"title":"Solvent-Free terminal alkyne hydrosilylation to β-(E)-vinylsilanes mediated by platinum(II) aminophosphine complexes","authors":"Hanna Stachowiak-Dłużyńska ,&nbsp;Marcin Gruszczyński ,&nbsp;Grzegorz Hreczycho","doi":"10.1016/j.jcat.2025.116027","DOIUrl":"10.1016/j.jcat.2025.116027","url":null,"abstract":"<div><div>This study presents a method for synthesizing β-(E)-vinylsilanes through the hydrosilylation of terminal alkynes with diverse secondary silanes, employing platinum(II) complexes with P,N-donor ligands. The method achieves selective hydrosilylation under solvent-free conditions, yielding up to 99% of alkenylhydrosilanes. It accommodates a wide range of aliphatic, aromatic, and heterocyclic alkynes, representing an advancement in platinum-based protocols by promoting mono-hydrosilylation with secondary silanes. The versatility of this approach is further demonstrated by subsequent transformations of β-(E)-vinylsilanes, indicating its broad applicability in organic synthesis and material chemistry.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"445 ","pages":"Article 116027"},"PeriodicalIF":6.5,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418462","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}

{"title":"Access to SCF3-containing N-fused quinolines via photo-induced domino radical trifluoromethylthiolation","authors":"Congjun Zhu,&nbsp;Yangyang Shen,&nbsp;Zilong Wang,&nbsp;Jie Xu,&nbsp;Wendong Fang,&nbsp;Haofang Tian,&nbsp;Jinjie Li,&nbsp;Tao Guo","doi":"10.1016/j.jcat.2025.116005","DOIUrl":"10.1016/j.jcat.2025.116005","url":null,"abstract":"<div><div>Radical trifluoromethylthiolation under mild photoredox conditions, show unique utility in the preparation of SCF₃-containing organic skeleton. Here, we report an unprecedented domino radical trifluoromethylthiolation upon photocatalysis. With the established protocol, a wide spectrum of SCF₃-containing N-fused quinolines has been rapidly synthesized. Preliminary mechanistic investigations, including several control experiments and photochemistry measurements, shed light on the catalytic radical reaction mechanism. Sequential evaluated the photophysical properties for selected products is presented, which further underlines the value of this work.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"445 ","pages":"Article 116005"},"PeriodicalIF":6.5,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418466","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}

{"title":"Thermosensitive four-arm star-shaped copolymers with phthalocyanine as core and porphyrin copolymer as arms was used as visible light photocatalyst","authors":"Shan Wu ,&nbsp;Jian Shi ,&nbsp;Qian Duan ,&nbsp;Ludan Shang ,&nbsp;Xiaodong Zhang ,&nbsp;Yuhan Duan","doi":"10.1016/j.jcat.2025.116009","DOIUrl":"10.1016/j.jcat.2025.116009","url":null,"abstract":"<div><div>Porphyrins and phthalocyanines are considered as visible light catalysts with great development potential due to their unique π-conjugated structure, strong visible light absorption and structural tunability. However, they are easy to aggregate and difficult to dissolve, and their application in the field of photocatalysis is limited. Based on the above problems, in this study, three four-arms star-shaped thermosensitive copolymers (PcZn-(PNIPAM_n-co-PUMPP_m)₄) photocatalysts with zinc phthalocyanine as the core and porphyrin thermosensitive copolymer as the arms was constructed by using RAFT polymerization technology and the ’core first’ route. The visible light catalytic activity of the prepared star-shaped copolymers was evaluated by using 1,5-dihydroxynaphthalene (DHN) and methylene blue (MB) as model pollutants. The three copolymers were found to be effective in oxidizing DHN to juglone and degrading MB. Among them, PcZn-(PNIPAM_33.5-co-PUMPP_1.6)₄ (P3) showed the highest DHN conversion efficiency (100.0 %), reaction yield (70.0 %) and MB degradation (96.9 %). ¹O₂ and O₂·^- are the main active substances in the visible photocatalytic process. Based on UV–vis absorption spectra, Fluorescence spectra, EIS Nyquist plots and transient photocurrents, it is confirmed that P3 has a wider range of visible light absorption, and there is effective energy and electron transfer between TTPcZn and UMPP units in P3, which makes it have higher catalytic activity. More importantly, the lower critical solution temperature (32.6 ∼ 32.9 °C) of P3 makes it possible to achieve homogeneous catalysis and heterogeneous recovery through simple temperature regulation in the catalytic process, which makes P3 have good reusability. This work paves a way for the construction of high-performance and recyclable visible polymer photocatalyst.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"445 ","pages":"Article 116009"},"PeriodicalIF":6.5,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418465","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}

{"title":"Ten recommendations for literature data generation for chemical process optimization in renewable feedstock conversion","authors":"Siddhant M. Lambor ,&nbsp;Dionisios G. Vlachos","doi":"10.1016/j.jcat.2025.116004","DOIUrl":"10.1016/j.jcat.2025.116004","url":null,"abstract":"<div><div>Process development of recyclable and renewable feedstocks entails intensive and tedious catalyst and solvent screening and multiparameter process exploration. The solid nature of these feedstocks necessitates highly time-consuming, batch experiments, leading to limited published datasets. Our ability to rapidly advance process development requires a systematic approach to the simultaneous optimization of catalysts, solvents, and processing conditions. One approach toward this goal is to harness and analyze accumulated literature data to develop performance-process correlations. With this goal, we study a prototype biomass reaction, the fructose dehydration to 5-hydroxymethyl furfural (HMF) over zeolite catalysts. We explore literature data to optimize the vast descriptor space of zeolite characteristics, solvents, and process conditions using correlation analysis. We assess the quality of reported literature data and identify where provenance is lacking. We develop apparent kinetic analysis to correlate performance with solvent and catalyst properties. We showcase that solvents and to an extent processing conditions dominate HMF yield; in contrast, zeolites play a secondary role for this chemistry. We provide ten recommendations for improving this methodology to extract further knowledge and improve process optimization.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"444 ","pages":"Article 116004"},"PeriodicalIF":6.5,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418464","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}

{"title":"Proton shuttle mediated by ionic liquid promotes aldol condensation","authors":"Tianhao Zhang ,&nbsp;Hanwen Yan ,&nbsp;Chong Zhang ,&nbsp;Yiqian Yang ,&nbsp;Jie Li ,&nbsp;Guoliang Zhang ,&nbsp;Junping Zhang ,&nbsp;Gang Wang ,&nbsp;Chunshan Li","doi":"10.1016/j.jcat.2025.116001","DOIUrl":"10.1016/j.jcat.2025.116001","url":null,"abstract":"<div><div>Effective strategy is intensively desired to construct efficient and durable catalytic system for mild aldol condensation between aldehydes, considering the profound significance in synthesis of high-valued <em>α</em>, <em>β</em>-unsaturated aldehydes. Although series of mild catalytic systems using secondary amine-based catalysts have been proposed, the compatibility of high catalytic selectivity and durability still troubles the researchers in this field. Here, we developed a protonated diethanolamine ionic liquid catalyzed mild aldol reaction system with reasonable regulation of ion pair strength and ionic cluster microenvironment based on the deep insights into proton shuttle effects to improve catalytic selectivity and durability for the probed methacrolein synthesis. The interplay between the cation and anion mediated proton shuttle was elucidated by detailed kinetics derived from <em>in situ</em> Raman spectroscopy and theoretical calculations. Further experimental and characterization facts combined with molecular dynamic simulations identify the weak interaction of cation–anion pair and metastable worm-like cluster microenvironment facilitate proton shuttle and thus improve catalytic performance and durability. Consequently, the formation rate of methacrolein was enhanced by one fold, while overall side reaction rates were reduced by 27.5% compared to the conventional <em>sec</em>-amine catalyst. Additionally, this strategy also exhibited significant promotion in catalytic activity, selectivity, and durability in synthesis of the other representative <em>α</em>, <em>β</em>-unsaturated aldehydes. These findings will offer reference for the construction and modulation of ionic liquid catalyzed mild aldol reaction system utilizing proton shuttle effects.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"444 ","pages":"Article 116001"},"PeriodicalIF":6.5,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143393982","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}

{"title":"Insights into the catalytic synthesis of 2,5-hexanedione from the novel biomass-derived platform compound 5-chloromethylfurfural using NiMo@HZSM-5 catalyst","authors":"Shibo Yang ,&nbsp;Wenbo Liao ,&nbsp;Hangwei Qin ,&nbsp;Tong Sun ,&nbsp;Yadong Liu ,&nbsp;Xiaokai Li ,&nbsp;Wenlong Jia ,&nbsp;Xing Tang ,&nbsp;Lu Lin ,&nbsp;Yong Sun","doi":"10.1016/j.jcat.2025.116000","DOIUrl":"10.1016/j.jcat.2025.116000","url":null,"abstract":"<div><div>Currently, there exists a significant deficiency of reports addressing the direct synthesis of 2,5-hexanedione (HD) from biomass a derivatives 5-Chloromethylfurfural (CMF). The in-situ generation of hydrochloric acid during the hydrogenation process of CMF necessitates catalysts with exceptional acid resistance, which has compelled previous studies to rely on noble-metal catalysts—an approach that poses challenges for scaling up HD production. Herein, this study presents the inaugural report of a non-noble metal nickel-based alloy catalyst synthesized through a straightforward wet impregnation method, which facilitates the efficient catalytic hydrogenation of CMF to produce HD under mild conditions. The results demonstrate that complete conversion of CMF was achieved and an 81.6 % yield of HD was obtained under optimal reaction conditions. In addition, the reaction pathway for synthesizing HD from CMF was elucidated based on the reaction kinetics and gas chromatography-mass spectrometry analysis, accompanied by an in-depth investigation into the reaction mechanism. The molybdenum was incorporated into the catalyst to form alloy components, which significantly enhanced the stability and acid resistance of the catalyst, thereby improving its catalytic performance. This study presents a novel approach for non-noble metal alloy catalysts to efficiently facilitate the conversion of biomass derivatives into downstream chemicals in an acidic environment.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"444 ","pages":"Article 116000"},"PeriodicalIF":6.5,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143393954","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}

{"title":"Positive shift of the d-Band center in Cu nanoparticles facilitates electrocatalytic hydrogenation of furfural under mild pH conditions","authors":"Huabin Lian ,&nbsp;Riming Hu ,&nbsp;Lin Zheng ,&nbsp;Daowei Gao ,&nbsp;Shuai Wang ,&nbsp;Rongyao Wang ,&nbsp;Bin Wang ,&nbsp;Guozhu Chen","doi":"10.1016/j.jcat.2025.116003","DOIUrl":"10.1016/j.jcat.2025.116003","url":null,"abstract":"<div><div>The electrocatalytic reduction of biomass-derived furfural represents a sustainable pathway for the production of furfuryl alcohol and 2-methylfuran, serving respectively as value-added chemicals and biofuels. However, the production of these high-value-added products under mild conditions is hampered by low Faradaic efficiency. In this study, we develop a strategy to establish strong metal-support interactions, enabling Cu/NC (nitrogen-doped carbon) catalysts to efficiently produce value-added products under mild conditions. Specifically, we prepare a cost-effective NC support with highly dispersed ultrafine nano-Cu particles of approximately 1 nm in diameter. Under mild pH conditions, our comparative experiments show that the Faradaic efficiency for value-added products (furfuryl alcohol and 2-methylfuran) is nearly four times higher than that of commercial foam copper. We elucidate the influence of nitrogen-doped supports on the behavior of the supported metal Cu. Comprehensive in-situ infrared reflection absorption spectroscopy characterization and DFT theoretical calculations reveal a positive shift in the d-band center of the Cu 3d orbitals. This shift enhances the adsorption of furfural C1=O1 bonds on the Cu/NC catalyst and improves its capacity to bind active hydrogen, thereby increasing the Faradaic efficiency of the value-added products. Our findings advance theoretical understanding and providing practical insights for electrocatalytic hydrogenation of furfural under mild pH conditions.</div></div>","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"444 ","pages":"Article 116003"},"PeriodicalIF":6.5,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385449","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}