Molecular Catalysis最新文献

Hemin-functionalised conducting polymer as a unique host matrix for the electrochemical synthesis of benzothiazole derivatives: A sustainable approach hemin功能化导电聚合物作为电化学合成苯并噻唑衍生物的独特宿主基质：一种可持续的方法

IF 4.9 2区化学

Molecular Catalysis Pub Date : 2025-10-11 DOI: 10.1016/j.mcat.2025.115521

Krishnapriya Jayan , Anitha Varghese

{"title":"Hemin-functionalised conducting polymer as a unique host matrix for the electrochemical synthesis of benzothiazole derivatives: A sustainable approach","authors":"Krishnapriya Jayan , Anitha Varghese","doi":"10.1016/j.mcat.2025.115521","DOIUrl":"10.1016/j.mcat.2025.115521","url":null,"abstract":"<div><div>An electrocatalyst based on the non-toxic and biologically derived metalloporphyrin hemin, immobilized on poly 3,4-diaminobenzoic acid (PDABA) was utilized for the sustainable electrochemical synthesis of benzothiazole derivatives. Electrochemical and topographical attributes of the electrocatalyst were analyzed critically using a ferricyanide probe, electrochemical impedance spectroscopy (EIS), X-ray photoelectron spectroscopy (XPS), optical profilometry, FTIR, and FE-SEM techniques. The modified electrode was employed for the electrochemical synthesis of benzothiazole derivatives using various aromatic aldehydes and 2-aminothiophenol. The reactions were performed in a three-electrode system, at oxidation potentials derived from cyclic voltametric elucidations, using lithium perchlorate as the supporting electrolyte and ethanol as the solvent. The products obtained were crystallized, purified and confirmed with the help of 1H-NMR spectroscopy, showing yields ranging from 78-92 %. The hemin based heterogenous electrocatalyst enhances the efficacy of the reaction by reducing reaction time, and negating tedious work-up procedures, thereby making the method highly facile and environmentally benign.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"588 ","pages":"Article 115521"},"PeriodicalIF":4.9,"publicationDate":"2025-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145264646","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}

引用次数: 0

Gold versus palladium catalyzed cross-coupling reactions: a DFT mechanistic study on the chemoselective arylation of alkyl nitriles 金与钯催化的交叉偶联反应：烷基腈化学选择性芳基化的DFT机理研究

IF 4.9 2区化学

Molecular Catalysis Pub Date : 2025-10-11 DOI: 10.1016/j.mcat.2025.115524

Gaetano Galdi, Artur Brotons-Rufes, Chiara Costabile

引用次数: 0

Transition metal-anchored WS2 nanosheets as efficient electrocatalysts for hydrogen evolution reaction: A first-principles study 过渡金属锚定WS2纳米片作为析氢反应的高效电催化剂：第一线原理研究

IF 4.9 2区化学

Molecular Catalysis Pub Date : 2025-10-10 DOI: 10.1016/j.mcat.2025.115519

Rui Sun, Zhongxu Wang, Jingxiang Zhao

{"title":"Transition metal-anchored WS2 nanosheets as efficient electrocatalysts for hydrogen evolution reaction: A first-principles study","authors":"Rui Sun, Zhongxu Wang, Jingxiang Zhao","doi":"10.1016/j.mcat.2025.115519","DOIUrl":"10.1016/j.mcat.2025.115519","url":null,"abstract":"<div><div>The development of efficient, low-cost, and stable electrocatalysts remains a central challenge for sustainable hydrogen production. In this work, we systematically designed a series of single transition metal (TM) atoms (including Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zr, Nb, Mo, Ru, Rh, Pd, Ag, Hf, Ta, W, Os, Ir, Pt, and Au) anchored on a WS2 monolayer, and investigated their catalytic activity for the hydrogen evolution reaction (HER) using density functional theory (DFT) calculations. The comprehensive results reveal that TM atoms can effectively tune the electronic structure, electrical conductivity, and hydrogen adsorption behavior of WS2. In particular, Cr@WS2, Fe@WS2, Mo@WS2, and Ru@WS2 catalysts exhibit Gibbs free energies of hydrogen adsorption close to zero, indicating their promising HER activity. Further crystal orbital Hamilton population (COHP) analyses and Bader charge calculations demonstrate that the chemical bonding characteristics and charge transfer between the TM atoms and the WS2 substrate play a pivotal role in tuning adsorption strength and catalytic performance. This work provides a theoretical foundation for optimizing WS2-based single-atom catalysts and opens new avenues for the design of highly efficient HER electrocatalysts based on two-dimensional materials.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"588 ","pages":"Article 115519"},"PeriodicalIF":4.9,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145264643","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}

引用次数: 0

Identifying the role of Pr oxide species in Ni-Pr/Al2O3 for dry reforming of methane Pr氧化物在Ni-Pr/Al2O3干重整甲烷中的作用

IF 4.9 2区化学

Molecular Catalysis Pub Date : 2025-10-10 DOI: 10.1016/j.mcat.2025.115528

Wenzheng Zhang , Huahua Zhao , Jian Yang , Huanling Song , Lingjun Chou

{"title":"Identifying the role of Pr oxide species in Ni-Pr/Al2O3 for dry reforming of methane","authors":"Wenzheng Zhang , Huahua Zhao , Jian Yang , Huanling Song , Lingjun Chou","doi":"10.1016/j.mcat.2025.115528","DOIUrl":"10.1016/j.mcat.2025.115528","url":null,"abstract":"<div><div>Ni-based catalysts are promising non-precious catalysts for dry reforming of methane (DRM), but their development is hindered by unavoidable coke formation and metal sintering. Herein, Pr-modified Ni/Al2O3 catalysts were prepared to investigate the role of Pr in the conventional Ni/Al2O3 catalyst during DRM. The XRD, XPS, and TEM results indicate that the Pr oxide species (Pr6O11) remain stable after H2 reduction and during DRM. The TG-DSC, CO2-TPD, CO2-TPSR, and O2-TPO results indicate a significant improvement in the adsorption and activation of CO2 by Pr oxide species, as well as the suppression of the formation of graphitic carbon species. In situ DRIFTS measurements reveal the oxygen-assisted CH4 activation and the rapid transformation of CO2 to carbonate species, which restrict the carbon deposition in DRM. By contrast, the unmodified Ni/Al2O3 catalyst shows inferior catalytic stability due to the higher amount and graphitization degree of coke species. This study demonstrates that the Pr oxide species can enhance the coke resistance of Ni-based catalysts during the DRM process.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"588 ","pages":"Article 115528"},"PeriodicalIF":4.9,"publicationDate":"2025-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145264645","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}

引用次数: 0

Hydrogen evolution using electropolymerized Nickel-Integrated Dipyrromethane as an electrocatalyst at neutral pH 中性pH下电聚合镍集成二吡咯甲烷的析氢研究

IF 4.9 2区化学

Molecular Catalysis Pub Date : 2025-10-10 DOI: 10.1016/j.mcat.2025.115526

Kumaresan Sudharsan , Thangaraj Keerthana , Baskaran Sarikalakshmi , Sekar Monisha , Samuthirakani AjithKumar , Venkatesh Soundharya , Sk. Jasimuddin , Palanisamy Kalimuthu

引用次数: 0

Ni–NbOx Bifunctional catalysts for selective hydrodeoxygenation of m-cresol to toluene 间甲酚选择性加氢脱氧制甲苯的Ni-NbOx双功能催化剂

IF 4.9 2区化学

Molecular Catalysis Pub Date : 2025-10-09 DOI: 10.1016/j.mcat.2025.115516

Camila A. Teles , Carmen Ciotonea , Ruben Palacio , Diana Lopez , Sébastien Royer , Frédéric Richard

{"title":"Ni–NbOx Bifunctional catalysts for selective hydrodeoxygenation of m-cresol to toluene","authors":"Camila A. Teles , Carmen Ciotonea , Ruben Palacio , Diana Lopez , Sébastien Royer , Frédéric Richard","doi":"10.1016/j.mcat.2025.115516","DOIUrl":"10.1016/j.mcat.2025.115516","url":null,"abstract":"<div><div>The catalytic performances of a series of Ni supported on mesoporous silica (SBA-15) and niobia, as well as Ni-NbOx dispersed on SBA-15 were evaluated for the hydrodeoxygenation (HDO) of m-cresol at 300°C under atmospheric pressure. Under the reaction conditions, hydrogenation and C-C hydrogenolysis pathways yielding only oxygenated products dominated over the monometallic Ni catalyst. In contrast, the Direct DeOxygenation pathway (DDO) leading to toluene was significantly promoted when Ni was in contact with oxophilic NbOx surface. Tuning the Ni-Nb ratio on silica revealed a remarkable enhancement of the DDO rate constant. Indeed, the kinetic rate constant determined over 5Ni5Nb/SBA was about 11 times higher than that measured on the catalyst containing only the Ni phase. This enhanced performance can be attributed to the formation of well-dispersed Ni–NbOx interfacial sites, where the hydrogenation capability of Ni associate with the oxophilic character of Nb⁵⁺/Nb⁴⁺ species allowing to a more efficient activation of the C-O bonding and promoting the DDO reaction pathway. These results offer valuable insights for the rational design of selective catalysts for the transformation of lignin-derived bio-oils into aromatic hydrocarbons.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"588 ","pages":"Article 115516"},"PeriodicalIF":4.9,"publicationDate":"2025-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145263800","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}

引用次数: 0

Tuning the structure and reactivity of zeolite-confined Pt catalysts by Ga incorporation for enhanced propane dehydrogenation 通过掺入Ga调整沸石型Pt催化剂的结构和反应性以促进丙烷脱氢

IF 4.9 2区化学

Molecular Catalysis Pub Date : 2025-10-09 DOI: 10.1016/j.mcat.2025.115518

Jianbing Wu , Ge Hua , Jihua Liu , Yifan Zhao , Hong Ma , Yongzhao Wang , Zhiwei Wu

{"title":"Tuning the structure and reactivity of zeolite-confined Pt catalysts by Ga incorporation for enhanced propane dehydrogenation","authors":"Jianbing Wu , Ge Hua , Jihua Liu , Yifan Zhao , Hong Ma , Yongzhao Wang , Zhiwei Wu","doi":"10.1016/j.mcat.2025.115518","DOIUrl":"10.1016/j.mcat.2025.115518","url":null,"abstract":"<div><div>Pt-based catalysts confined within silicalite-1 (S-1) zeolites offer promising selectivity for propane dehydrogenation (PDH), but their long-term stability remains limited due to metal sintering and coke deposition. In this study, a series of Pt@S-1 catalysts with systematically varied Ga contents were synthesized via ligand-assisted hydrothermal encapsulation of Pt and in situ Ga incorporation. Structural characterizations reveal that Ga is introduced as both framework (GaF) and extra-framework (GaEF) species. Under H2 treatment, GaEF partially transforms into either PtGa alloy nanoparticles and Gaδ+ species, leading to the formation of Pt-Gaδ+-H ensembles within the zeolite channels. These Ga-related species were associated with improved Pt dispersion, suppressed sintering, and reduced coke formation. The optimized catalyst, 1Pt24Ga@S-1, exhibited the most favorable PDH performance, achieving an initial propane conversion of 38.2 % and a propylene selectivity of 94.8 %. Under H2 co-feeding (C3H8:H2 = 1:1), it achieved a propylene production rate of 7.97 molC3H6·gPt-1·h-1. The deactivation constant decreased from 0.247 h-1 for the undoped catalyst to 0.086 h-1 with Ga incorporation, and further declined to 0.008 h-1 under H2, reflecting improved stability. These results suggest that Ga incorporation contributes to both structural and electronic modifications of confined Pt species, offering insights into the design of more stable and selective PDH catalysts.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"588 ","pages":"Article 115518"},"PeriodicalIF":4.9,"publicationDate":"2025-10-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145263801","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}

引用次数: 0

Support composition engineering of gold catalysts for efficient oxidative esterification of ethylene glycol 支持乙二醇高效氧化酯化金催化剂的组成工程

IF 4.9 2区化学

Molecular Catalysis Pub Date : 2025-10-07 DOI: 10.1016/j.mcat.2025.115522

Tingting Ge , Xiaorui Liu , Ziyan Jia , Chao Liu , Jiahui Huang

{"title":"Support composition engineering of gold catalysts for efficient oxidative esterification of ethylene glycol","authors":"Tingting Ge , Xiaorui Liu , Ziyan Jia , Chao Liu , Jiahui Huang","doi":"10.1016/j.mcat.2025.115522","DOIUrl":"10.1016/j.mcat.2025.115522","url":null,"abstract":"<div><div>To address the overcapacity in coal-to-ethylene glycol production, developing eco-friendly process to convert ethylene glycol into high-value-added chemicals is an important topic in current industrial research. In this work, we prepared a multi-component metal oxide-supported Au catalyst through a simple physical mixing and impregnation strategy, and investigated the influence of the support composition on the catalyst activity. Among all tested catalysts, Au/NbZnAlOx exhibited the optimal catalytic performance, achieving a selectivity of 95 % for methyl glycolate, while maintaining good stability (>90 % selectivity) after five cycles. The characterization of XRD, XPS, TPD and ATR-IR indicated that the incorporation of 10 wt% ZnO and 10 wt% Al2O3 into Nb2O5 effectively modulates the balanced distribution of acid-base sites on the catalyst surface and the substrate adsorption capacity. Meanwhile, NbZnAlOx support endowed Au nanoparticles highest electron density, promoting the activation of O2, thereby enhancing the catalytic activity. Kinetic studies revealed a remarkable reduction in activation energy from 77 kJ mol-1 to 24 kJ mol-1 upon ZnO/Al2O3 incorporation into Nb2O5. These findings provide insights into designing multi-component oxide-supported gold catalysts and highlight the critical importance of support composition in optimizing selective oxidation reactions.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"588 ","pages":"Article 115522"},"PeriodicalIF":4.9,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145264642","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}

引用次数: 0

Formate-driven chemoenzymatic oxyfunctionalization of inert C(sp3)-H bonds on unspecific peroxygenase-CLEAs immobilized RhIII-complex functionalized hierarchical covalent organic frameworks 非特异性过氧酶- cleas固定化rhiii -配合物功能化分层共价有机框架上惰性C(sp3)-H键的甲酸驱动化学酶氧化功能化

IF 4.9 2区化学

Molecular Catalysis Pub Date : 2025-10-06 DOI: 10.1016/j.mcat.2025.115525

Fei Huang , Qian Zhang , Hao Li , Yunting Liu , Guanhua Liu , Li Ma , Liya Zhou , Ying He , Xiaoyang Yue , Yanjun Jiang

{"title":"Formate-driven chemoenzymatic oxyfunctionalization of inert C(sp3)-H bonds on unspecific peroxygenase-CLEAs immobilized RhIII-complex functionalized hierarchical covalent organic frameworks","authors":"Fei Huang , Qian Zhang , Hao Li , Yunting Liu , Guanhua Liu , Li Ma , Liya Zhou , Ying He , Xiaoyang Yue , Yanjun Jiang","doi":"10.1016/j.mcat.2025.115525","DOIUrl":"10.1016/j.mcat.2025.115525","url":null,"abstract":"<div><div>Heme peroxygenases demonstrate exceptional catalytic efficiency for incorporating oxygen into inert C(sp3)-H bonds using only H2O2 as both oxygen source and electron donor, representing a fundamental challenge in synthetic chemistry. However, their practical utility is severely limited by oxidative inactivation caused by exogenous H2O2. To overcome this critical limitation, herein, we develop an innovative formate-driven chemoenzymatic cascade system. Our approach employs an unspecific peroxygenase from Agrocybe aegerita (AaeUPO) co-immobilized with a RhIII-complex within a hierarchical covalent organic framework (AaeUPO@Rh-macroCOF) to achieve efficient C(sp3)-H oxyfunctionalization. This system operates through an elegant tandem mechanism: (1) the Rh-complex catalyzes O2 reduction to generate H2O2 using formate as a safe hydrogen donor; and (2) the in situ produced H2O2 subsequently activates the immobilized AaeUPO for selective C(sp3)-H oxyfunctionalization. Notably, this integrated system addresses the longstanding stability issues of peroxygenase while maintaining highly catalytic efficiency. Furthermore, we demonstrate the broad substrate scope of this sustainable platform, highlighting its versatility for green synthesis applications.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"588 ","pages":"Article 115525"},"PeriodicalIF":4.9,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145263799","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}

引用次数: 0

Visible light catalyzed synthesis of quinazolinone compounds from benzyl alcohol/styrene and 2-aminobenzamide 可见光催化苯甲醇/苯乙烯和2-氨基苯甲酰胺合成喹唑啉酮化合物

IF 4.9 2区化学

Molecular Catalysis Pub Date : 2025-10-04 DOI: 10.1016/j.mcat.2025.115512

Guofang Jiang, Aixin Wang, Sheng Huang, Zongbo Xie, Zhanggao Le

引用次数: 0