Molecular Catalysis最新文献_第2页

Direct Z-scheme SnS₂/WTe₂ heterojunction for enhanced visible-light-driven water splitting performance based on DFT

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-03-25 DOI: 10.1016/j.mcat.2025.115048

Jie Li, Yongchao Liang, Xiaoxiao Li, Gongmin Wei, Zhihan Zhang, Qian Chen

{"title":"Direct Z-scheme SnS₂/WTe₂ heterojunction for enhanced visible-light-driven water splitting performance based on DFT","authors":"Jie Li, Yongchao Liang, Xiaoxiao Li, Gongmin Wei, Zhihan Zhang, Qian Chen","doi":"10.1016/j.mcat.2025.115048","DOIUrl":"10.1016/j.mcat.2025.115048","url":null,"abstract":"<div><div>The use of fossil fuels leads to environmental issues such as global warming and acid rain. Photocatalytic hydrogen production has become a trend towards solving this problem. However, the rapid recombination of photo-generated electrons and holes in single-component photocatalysts severely limits their photocatalytic performance. Van der Waals (vdW) heterojunctions can effectively suppress the carrier recombination rate. Therefore, this study constructs SnS₂/WTe₂ van der Waals heterojunctions via a vertical stacking approach and employs first-principles calculations to investigate their stability, electronic structure, optical properties, and photocatalytic mechanisms. The results demonstrate that the SnS₂/WTe₂ heterojunction exhibits structural stability, with the valence band maximum (VBM) and conduction band minimum (CBM) dominated by WTe₂ and SnS₂, respectively. The oxidation and reduction potentials of this heterojunction span the redox potential of water, enabling photocatalytic water splitting to proceed normally. Compared to the single-layer materials, the SnS<sub>2</sub>/WTe<sub>2</sub> heterojunction exhibits superior light absorption properties and refractive index. Furthermore, it achieves a hydrogen production efficiency of 9.39 % under AM1.5G solar flux. The application of biaxial strain further optimizes the electronic and optical properties of the SnS₂/WTe₂ heterojunction. The SnS₂/WTe₂ heterojunction exhibits efficient HER and OER performance based on Gibbs free energy calculations. This study provides a highly promising candidate material for the development of high-efficiency hydrogen evolution reaction catalysts.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"579 ","pages":"Article 115048"},"PeriodicalIF":3.9,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143697191","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

Distinctive pathways of single-atom and nanoparticle sites over Co-based catalysts for furfuryl alcohol hydrogenation

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-03-24 DOI: 10.1016/j.mcat.2025.115043

Fan Xue, Shangpu Zhuang, Jingyue Bi, Zhaoyang Fei, Xu Qiao

{"title":"Distinctive pathways of single-atom and nanoparticle sites over Co-based catalysts for furfuryl alcohol hydrogenation","authors":"Fan Xue, Shangpu Zhuang, Jingyue Bi, Zhaoyang Fei, Xu Qiao","doi":"10.1016/j.mcat.2025.115043","DOIUrl":"10.1016/j.mcat.2025.115043","url":null,"abstract":"<div><div>The targeted transformation of biomass resources into premium chemicals and biofuels stands out as a highly promising approach to mitigate greenhouse gas emissions and curb environmental pollution caused by excessive use of fossil fuels. The catalysts with diverse active sites are crucial to determine the products distribution of furan-containing bio-based feedstocks hydrogenation. Herein, Co<sub>1</sub>/NC and Co<sub>NPs</sub>/NC catalysts have been successfully prepared and demonstrated distinct reaction pathways in the selective hydrogenation of furfuryl alcohol (FOL). Notably, the Co<sub>1</sub>/NC catalyst showed 11.8 % FOL conversion within 1 h and both furan ring (C = C) and the C–OH could be hydrogenated over CoN<sub>4</sub> sites. In contrast, the Co nanoparticles were more inclined to facilitate the activation and cleavage of C–OH bond in FOL with 92.2 % selectivity of 2-methylfuran and its derivatives over Co<sub>NPs</sub>/NC catalyst. Although the temperature, H<sub>2</sub> pressure and solvents can affect products distribution, their impact differences also depended on the nature of the active sites. This work underscores the importance of a thorough understanding about the structure–activity relationship, which is crucial to systematic design suitable catalysts with tailored active sites for specific catalytic reactions.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"579 ","pages":"Article 115043"},"PeriodicalIF":3.9,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143686244","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

Mechanistic insights and stereoselectivity in Ni(II)-catalyzed asymmetric [3 + 2]/[3 + 3] cycloaddition reactions of donor-acceptor cyclopropanes: A DFT study

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-03-24 DOI: 10.1016/j.mcat.2025.115034

Jiacheng Fan , Ran Fang , Yanyun Dong , Simeng Qi , Lizi Yang

{"title":"Mechanistic insights and stereoselectivity in Ni(II)-catalyzed asymmetric [3 + 2]/[3 + 3] cycloaddition reactions of donor-acceptor cyclopropanes: A DFT study","authors":"Jiacheng Fan , Ran Fang , Yanyun Dong , Simeng Qi , Lizi Yang","doi":"10.1016/j.mcat.2025.115034","DOIUrl":"10.1016/j.mcat.2025.115034","url":null,"abstract":"<div><div>Density functional theory (DFT) was employed to investigate the reaction mechanisms and stereoselectivity of Ni(II)-catalyzed nonracemic donor-acceptor cyclopropane (DAC) [3 + 2]/[3 + 3] cycloaddition reactions with imine, triazine, and nitrone substrates. The results indicate that the overall reaction for all three substrates consists of two main steps: (1) nucleophilic attack of the substrate on the nonracemic DAC, and (2) C-C cyclization of the resulting key intermediate to form either five- or six-membered rings. For imine and triazine, the most favorable reaction pathway involves direct nucleophilic attack followed by cyclization, while for nitrone, the reaction proceeds via racemization to form an alkene intermediate, which then undergoes cyclization. Computational analysis reveals that the of the diastereoselectivity nucleophilic attack step is primarily controlled by distortion energy, whereas the enantioselectivity of the cyclization step is governed by interaction energy. Global reactivity index (GRI) analysis shows that imine exhibits the highest nucleophilicity with the lowest activation energy, while nitrone displays the weakest nucleophilicity and the highest activation energy. This theoretical study provides new insights into predicting reaction pathways and rationalizing the selective features of related cyclization reactions.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"579 ","pages":"Article 115034"},"PeriodicalIF":3.9,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143686243","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

CdS quantum dots with sulfur defects for photoreforming plastics into valuable chemicals coupled with hydrogen production

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-03-24 DOI: 10.1016/j.mcat.2025.115049

Jiaxin Song , Cheng Rao , Zeshu Zhang , Xiangguang Yang , Yibo Zhang

{"title":"CdS quantum dots with sulfur defects for photoreforming plastics into valuable chemicals coupled with hydrogen production","authors":"Jiaxin Song , Cheng Rao , Zeshu Zhang , Xiangguang Yang , Yibo Zhang","doi":"10.1016/j.mcat.2025.115049","DOIUrl":"10.1016/j.mcat.2025.115049","url":null,"abstract":"<div><div>Photocatalytic reforming of plastics, involving converting plastics into valuable chemicals while producing hydrogen from water, is a promising green technology with sustainability potential. However, designing catalysts with optimized structures to further enhance efficiency remained a major challenge. In this study, a series of CdS Quantum dots (QDs) with different sulfur defect concentrations were synthesized by a one-step solvothermal method by adjusting the type of sulfur precursors. In the absence of co-catalysts, the optimal CdS-NS photocatalyst achieved reforming of polyethylene terephthalate (PET) into formate with 870 μmol <em>g</em><sup>−1</sup> h<sup>−1</sup> and acetate esters with 90 μmol <em>g</em><sup>−1</sup> h<sup>−1</sup>, while the hydrogen production rate reached 1771 μmol <em>g</em><sup>−1</sup> h<sup>−1</sup>. EPR spectra and other analyses confirmed the presence of abundant sulfur defects in the prepared CdS QDs and further demonstrated that the concentration of sulfur defects was closely related to photocatalytic performance. Suitable sulfur defects effectively modulated the electronic and band structure of CdS QDs, enhanced the oxidation capacity of photogenerated holes, reduced the recombination rate of charge carriers, and ultimately improved photocatalytic activity. This work provided an effective approach for designing efficient photocatalysts for the high-value recycling of plastic waste to achieve carbon neutrality.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"579 ","pages":"Article 115049"},"PeriodicalIF":3.9,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143686812","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

Zn-TiO2/AC photocatalysts for pollutants degradation from experimental and DFT studies

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-03-23 DOI: 10.1016/j.mcat.2025.115037

Xiao Chu, Chen Chen, Ying Liang, Yuliang Chen, Yuliang Wu, Yijiang Liu, Rui Meng, Wenmin Wang, Weiwei Huang, Fei Yang, Xuesong Yi, Jun Cheng

{"title":"Zn-TiO2/AC photocatalysts for pollutants degradation from experimental and DFT studies","authors":"Xiao Chu, Chen Chen, Ying Liang, Yuliang Chen, Yuliang Wu, Yijiang Liu, Rui Meng, Wenmin Wang, Weiwei Huang, Fei Yang, Xuesong Yi, Jun Cheng","doi":"10.1016/j.mcat.2025.115037","DOIUrl":"10.1016/j.mcat.2025.115037","url":null,"abstract":"<div><div>The massive emission of dye wastewater has caused significant environmental problems. In this study, zinc-doped titanium dioxide loaded on biochar was synthesized by a simple solvothermal method to investigate its ability of degradation for dyes in photocatalytic process. The discussion focused on the impact of unactivated, acid-activated, and alkali-activated biochar on the properties of composites. Additionally, the composite catalysts underwent comprehensive physical and chemical characterization. The results showed that the particle size of Zn-TiO<sub>2<img></sub>OHAC increased significantly, which improved the sedimentation performance. Zn-TiO<sub>2<img></sub>OHAC demonstrated exceptional photocatalytic efficiency in the degradation of various pollutants such as Rhodamine B, Congo Red, Methyl Orange, and Methylene Blue. The better performance of the alkali-treated biochar-loaded composite catalysts was attributed to the fact that the alkali-treated biochar changed the electronic structure of the loaded materials and contained more carbon-oxygen functional groups, which was favorable for the separation of electrons and holes.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"579 ","pages":"Article 115037"},"PeriodicalIF":3.9,"publicationDate":"2025-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143686311","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

Construction of perylene diimide supramolecular polymers: Study of photocatalytic reduction conversion from sulfoxide to thioether

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-03-23 DOI: 10.1016/j.mcat.2025.115041

Yu-Song Bi , Cheng-Long Xin , Rong-Zhen Zhang , Hui Liu , Ling-Bao Xing

引用次数: 0

Morphology control of Ni(OH)2-TiO2 nanosheet array and its excellent electrochemical hydrogen evolution performance

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-03-23 DOI: 10.1016/j.mcat.2025.115042

Fen Qiao, Changshun Zheng, Jikang Zhao, Jiaxin Zhou, Genxiang Wang

{"title":"Morphology control of Ni(OH)2-TiO2 nanosheet array and its excellent electrochemical hydrogen evolution performance","authors":"Fen Qiao, Changshun Zheng, Jikang Zhao, Jiaxin Zhou, Genxiang Wang","doi":"10.1016/j.mcat.2025.115042","DOIUrl":"10.1016/j.mcat.2025.115042","url":null,"abstract":"<div><div>Aiming at the kinetic bottleneck of hydrogen evolution reaction in hydrogen production by electrolysis of water, Ni(OH)<sub>2</sub>-TiO<sub>2</sub> composites were successfully prepared on nickel foam (NF) substrate by two-step hydrothermal method. By adjusting the concentration of nickel source and reaction conditions, the composite catalysts with excellent morphology and structure were constructed. The Ni(OH)<sub>2</sub>-TiO<sub>2</sub> catalyst prepared under the optimized conditions has an overpotential of only 63 mV at the current density of 10 mA·cm<sup>−2</sup>, showing lower Tafel slope, higher double layer capacitance and excellent reaction kinetics. The results of density functional theory (DFT) revealed the phenomenon of charge transfer inside the composite and the influence of interface effect on the electron structure, and further confirmed that the electrons transfer from Ni(OH)<sub>2</sub> to TiO<sub>2</sub> optimized the charge distribution inside the composite, promoted the charge transfer at the interface, and reduced the activation energy of catalytic reaction.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"579 ","pages":"Article 115042"},"PeriodicalIF":3.9,"publicationDate":"2025-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143686310","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

Bimetallic oxide catalysis meets silanol-enhanced synergy: A winning combination for efficient CO2 fixation by cycloaddition with styrene oxide

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-03-22 DOI: 10.1016/j.mcat.2025.115029

Chaitra N. Mallannavar , S. Sujith , Shrinidhi D. Patil , Sanjeev P. Maradur , Ganapati V. Shanbhag

{"title":"Bimetallic oxide catalysis meets silanol-enhanced synergy: A winning combination for efficient CO2 fixation by cycloaddition with styrene oxide","authors":"Chaitra N. Mallannavar , S. Sujith , Shrinidhi D. Patil , Sanjeev P. Maradur , Ganapati V. Shanbhag","doi":"10.1016/j.mcat.2025.115029","DOIUrl":"10.1016/j.mcat.2025.115029","url":null,"abstract":"<div><div>The bimetallic oxide dispersed on silanol rich SBA-15-OH was designed for the synthesis of cyclic carbonates from epoxides and CO<sub>2</sub>. The SBA-15-OH was synthesized via desilication and active metals were loaded by sol-gel method. Pure Sn-Ni oxide with a low surface area and lesser activity was modified by dispersing it on a high surface area SBA-15-OH. The different characterization techniques such as XRD, N<sub>2</sub>-sorption, CO<sub>2</sub> and NH<sub>3</sub>-TPD, H<sub>2</sub>-TPR, SEM-EDX, TEM and XPS confirmed that the surface silanol group acts as anchoring site for the enhanced metal oxide-support interaction. Supported Sn-Ni oxide exhibited 16-fold better activity than pure Sn-Ni oxide, due to improved dispersion, which enhances the accessibility of reactants to the catalytic sites. Under the optimized reaction conditions 10Sn5Ni/SBA-15-OH gave 92.9 % styrene oxide conversion and 84.3 % selectivity for styrene carbonate. The catalyst is recyclable and the flexibility of the catalyst is tested for different epoxides with CO<sub>2.</sub></div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"579 ","pages":"Article 115029"},"PeriodicalIF":3.9,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143686314","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

Bifunctional catalysts based on 2-amino-1,10-phenanthroline-containing podands for cyclic carbonates synthesis from CO2 and epoxides under mild conditions

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-03-22 DOI: 10.1016/j.mcat.2025.115019

Violetta A. Ionova , Artem N. Fakhrutdinov , Daniil I. Gusev , Anton S. Abel , Alexei D. Averin , Irina P. Beletskaya

{"title":"Bifunctional catalysts based on 2-amino-1,10-phenanthroline-containing podands for cyclic carbonates synthesis from CO2 and epoxides under mild conditions","authors":"Violetta A. Ionova , Artem N. Fakhrutdinov , Daniil I. Gusev , Anton S. Abel , Alexei D. Averin , Irina P. Beletskaya","doi":"10.1016/j.mcat.2025.115019","DOIUrl":"10.1016/j.mcat.2025.115019","url":null,"abstract":"<div><div>A new series of polytopic ligands based on 1,10-phenanthroline and polyoxadiamines has been synthesized through S<sub>N</sub>Ar amination between 2-chloro-1,10-phenanthroline and diamines of various structures. The obtained podands were investigated as polytopic ligands for potassium and zinc ions in the industrially important reaction of cyclic carbonates synthesis from CO<sub>2</sub> and epoxides under mild conditions (p(CO<sub>2</sub>) = 1 atm., T = 60–80 °C). The advantage of 1,11-diamino-3,6,9-trioxaundecane functionalized by 1,10-phenanthroline units compared to the diamine itself is demonstrated. It is revealed that heteroarylated 1,11-diamino-3,6,9-trioxaundecane can be used as a catalyst in the presence of KI (2 mol.%) with a low loading of the ligand (0.2 mol.%) instead of the usually employed 5–10 mol.% for unfunctionalized podands. Under these reaction conditions mono-substituted cyclic carbonates of various structures have been synthesized in excellent preparative yields ranging from 87 to 99%. Coordination of two Zn(II) ions to both 1,10-phenanthroline moieties has been shown to provide additional enhancement of catalytic activity. The catalysts demonstrate excellent stability and can be reused at least in 6 cycles.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"579 ","pages":"Article 115019"},"PeriodicalIF":3.9,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143686306","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

Fabrication of excellent bifunctional electrocatalyst FeNi-LDH@L-NiCoP using ZIF as a sacrifice template for alkaline electrolysis of water

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-03-22 DOI: 10.1016/j.mcat.2025.115052

Boxuan Zhang , Jinxing Cui , Zhifang Li , Changlong Yang , Weiwei Dong , Ke Li

引用次数: 0