Molecular Catalysis最新文献

Photoinduced pinacol coupling of carbon-carbon bonds via triethoxysilane or Hantzsch Ester

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-04-03 DOI: 10.1016/j.mcat.2025.115088

Jianhua Liu, Gelan Wang, Chen Chen, Xiangrong Zhou, Peihe Li

{"title":"Photoinduced pinacol coupling of carbon-carbon bonds via triethoxysilane or Hantzsch Ester","authors":"Jianhua Liu, Gelan Wang, Chen Chen, Xiangrong Zhou, Peihe Li","doi":"10.1016/j.mcat.2025.115088","DOIUrl":"10.1016/j.mcat.2025.115088","url":null,"abstract":"<div><div>The photocatalytic reductive coupling of carbon-carbon bonds via pinacol coupling represents a significant transformation in organic synthesis chemistry. Several elegant studies have reported the use of metal or organic photocatalysts in this process, but these often lead to trace metal residues or involve intricate operational procedures. Herein, we report a photoinduced pinacol coupling of carbon-carbon bonds from ketones, achieved under photocatalyst-free conditions using triethoxysilane or Hantzsch ester as the reductant. In the model reaction employing benzophenone as substrate and triethoxysilane as the reductant, the corresponding pinacol product was obtained in 96 % yield under 370 nm LED light irradiation. Similarly, when Hantzsch ester served as the reductant, the pinacol product was obtained in 95 % yield under 423 nm LED light irradiation. The substrate scope demonstrated that six substrates yielded the corresponding products with yields ranging from 40 % to 96 %. Notably, when acetophenone, a substrate with minimal steric hindrance, was used under the established conditions, only 1-phenylethanol was produced. This work introduces two practical methods for the synthesis of carbon-carbon coupling intermediates through pinacol coupling of benzophenone-derived substrates, positioning these methodologies as promising candidates for various applications.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"579 ","pages":"Article 115088"},"PeriodicalIF":3.9,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143760052","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

Lean methane catalytic combustion using Pd/ZSM-5 catalysts prepared by ammonia evaporation method

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-04-03 DOI: 10.1016/j.mcat.2025.115092

Songquan Tang , Wenzhi Li , Jingting Jin , Xin Zhang , Zilong Shen , Yunfan Gui

{"title":"Lean methane catalytic combustion using Pd/ZSM-5 catalysts prepared by ammonia evaporation method","authors":"Songquan Tang , Wenzhi Li , Jingting Jin , Xin Zhang , Zilong Shen , Yunfan Gui","doi":"10.1016/j.mcat.2025.115092","DOIUrl":"10.1016/j.mcat.2025.115092","url":null,"abstract":"<div><div>Catalytic combustion of lean methane is an effective measure to alleviate the greenhouse effect, which posing extensive demands for catalysts with appreciable reactivity and thermal stability. Herein, the reactivity and thermal stability of Pd/ZSM-5 catalysts prepared by ammonia evaporation and impregnation were tested. Experimental results indicated that the catalyst prepared by the ammonia evaporation method exhibited higher catalytic activity than that prepared by the impregnation method with similar Pd loadings. Especially, when the palladium loading is 0.1 %, the methane conversion of Pd/ZSM-5 prepared by AE method maintained at 80 % for 12 h at 550 °C while the methane conversion of Pd/ZSM-5 prepared by IM method decreased from 70 % to 20 % within 12 h at 550 °C. Through characterization, it was found that the elevated reactivity originated from the high dispersion of palladium due to the boosted interaction between palladium species and ZSM-5 support. These findings on the preparation of Pd catalysts <em>via</em> ammonia evaporation offer a practical reference for catalyst preparation environment adjustment, active species anchoring, and support-metal interactions, thus providing a promising blueprint for the design of future methane catalytic combustion materials.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"579 ","pages":"Article 115092"},"PeriodicalIF":3.9,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143760050","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

Direct coupling of CH4 and CO2 to acetic acid over Pd/LDH catalyst by stepwise technique

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-04-03 DOI: 10.1016/j.mcat.2025.115084

Qiang Guo , Yixiao Wu , Yongjun Liu , Shiqi Tao , Xiaoshuang Wang , Wei Huang

{"title":"Direct coupling of CH4 and CO2 to acetic acid over Pd/LDH catalyst by stepwise technique","authors":"Qiang Guo , Yixiao Wu , Yongjun Liu , Shiqi Tao , Xiaoshuang Wang , Wei Huang","doi":"10.1016/j.mcat.2025.115084","DOIUrl":"10.1016/j.mcat.2025.115084","url":null,"abstract":"<div><div>Directly convert CH<sub>4</sub> and CO<sub>2</sub> into acetic acid is a 100 % atomic efficiency reaction, but remains a great challenge under mild conditions. Herein, we report that acetic acid is generated as the sole liquid product by direct CH<sub>4</sub> and CO<sub>2</sub> coupling over Pd/LDH catalyst by two stepwise technique at 200 °C and atmospheric pressure. The formation of acetic acid is closely related to the surface Pd<sup>0</sup> content, as well as the number of medium-strong acid and medium-strong base on the catalyst surface. The results of <em>in-situ</em> DRIFTS experiments show that acetic acid is mainly formed by the coupling of CH<sub>3</sub>* and CO<sub>2</sub>* (CH<sub>3</sub>*+CO<sub>2</sub>*→CH<sub>3</sub>COO*+*), or via CH<em><sub>x</sub></em>* and COOH* coupling (CH<em><sub>x</sub></em>*+COOH*→CH<em><sub>x</sub></em>COOH*+*) to form acetate which then followed by hydrogenation reaction. In which CH<sub>3</sub>* is originated from CH<sub>4</sub> dehydrogenation step, and COOH* may be formed by the reduction of CO<sub>2</sub> on metallic Pd sites. This study provides a feasible approach for the construction of high selectivity catalytic materials for the direct co-conversion of CH<sub>4</sub> and CO<sub>2</sub> into acetic acid at low temperature.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"579 ","pages":"Article 115084"},"PeriodicalIF":3.9,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143760053","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

In-situ synthesis of NiMo@SAPO-11 under mild conditions for the hydrodeoxygenation of triolein

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-04-02 DOI: 10.1016/j.mcat.2025.115076

Dejiang Zheng, Lu Li, Shitao Yu

引用次数: 0

Mining and engineering of pyrroline-5-carboxylate reductase for biocatalytic production of l-pipecolic acid with self-sufficient cofactor recycling

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-04-02 DOI: 10.1016/j.mcat.2025.115081

Shaoshuai Zhu , Binhao Wang , Guochao Xu, Ye Ni

{"title":"Mining and engineering of pyrroline-5-carboxylate reductase for biocatalytic production of l-pipecolic acid with self-sufficient cofactor recycling","authors":"Shaoshuai Zhu , Binhao Wang , Guochao Xu, Ye Ni","doi":"10.1016/j.mcat.2025.115081","DOIUrl":"10.1016/j.mcat.2025.115081","url":null,"abstract":"<div><div><span>l</span>-pipecolic acid (<span>l</span>-PA) is an essential chiral intermediate for local anesthetics and macrolide antibiotics. To achieve more stable and cost-effective biosynthesis of <span>l</span>-PA from <span>l</span>-lysine (<span>l</span>-Lys), a cascade enzymatic pathway with self-sufficient cofactor recycling was developed, incorporating lysine-6-dehydrogenase (LysDH) and pyrroline-5-carboxylate reductase (P5CR). To overcome bottlenecks in the pathway, Ec-P5CR from <em>Enterococcus casseliflavus</em> was identified as a promising biocatalyst for enhancing <span>l</span>-PA production. For further improvement of <span>l</span>-PA yield, protein engineering was performed on Ec-P5CR. The resulting variant K261W, combined with Rp-LysDH from <em>Rhodobacter pomeroyi</em> DSS-3, achieved significantly enhanced yield of 93 % at 100 mM <span>l</span>-Lys, as well as an impressive yield of 83 % at 500 mM <span>l</span>-Lys. MD simulations revealed that improved hydride transfer efficiency was mainly responsible for the enhanced performance of K261W, leading to shorter distances between catalytic residues and substrates. This work paves the way for efficient and sustainable <span>l</span>-PA synthesis, showcasing the potential of enzyme optimization in industrial applications.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"579 ","pages":"Article 115081"},"PeriodicalIF":3.9,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143746394","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

Methane selective oxidation by Au nanoparticles supported on BETA zeolites using O2 as the oxidant

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-04-02 DOI: 10.1016/j.mcat.2025.115091

Ruoyan Wang, Qianqian Zhu, Zhuoyuan Chen, Wei Wang, Yanshuo Li, Zhenxin Zhang

引用次数: 0

MOFs derived acid-base regulation strategies of CuZnAl catalyst for boosting CO2 hydrogenation to methanol

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-04-02 DOI: 10.1016/j.mcat.2025.115089

Lu Ren , Bin Wang , Yueli Wen , Maohong Fan , Zhaoxiong Huang , Wenxuan Li , Wei Huang , Jing Li , Jianping Guo

{"title":"MOFs derived acid-base regulation strategies of CuZnAl catalyst for boosting CO2 hydrogenation to methanol","authors":"Lu Ren , Bin Wang , Yueli Wen , Maohong Fan , Zhaoxiong Huang , Wenxuan Li , Wei Huang , Jing Li , Jianping Guo","doi":"10.1016/j.mcat.2025.115089","DOIUrl":"10.1016/j.mcat.2025.115089","url":null,"abstract":"<div><div>Acid-base synergistic effect is crucial in adjusting the catalytic performance of CO<sub>2</sub> hydrogenation to methanol, an efficient CO<sub>2</sub> emission reduction and carbon recycle strategy. Two MOFs-derived catalysts (CZ-MIL, CA-ZIF) with opposite acid-base properties were tailored by using MIL-68 (Al) and ZIF-8 (Zn) as precursors, and the above two MOFs precursors were hybridized (C-ZAx) to control the acid-base property of the catalyst. C-ZA0.6 (molar ratio of MIL-68 (Al) to ZIF-8 (Zn)=0.6) exhibits a promising catalytic performance with CO<sub>2</sub> conversion of 8.9 %, methanol selectivity of 61.85 %, and STY of 117.02 mg mL<sup>−1</sup>·h<sup>−1</sup> at 4 MPa and 523 K. Combined with comprehensive analysis, it is found that methanol selectivity is closely related to weak acid sites arising from the residual skeleton of MIL-68. Acid-base synergy facilitates the hydrogenation of CO<sub>2</sub> to methanol. The basic sites are responsible for adsorbing and activating CO<sub>2</sub>, and the acidic site helps to stabilize CO* and facilitate the further hydrogenation to methanol. This work provides a new idea and feasible method for enhancing the catalytic performance of CO<sub>2</sub> hydrogenation to methanol.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"579 ","pages":"Article 115089"},"PeriodicalIF":3.9,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143746393","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

Bio-inspired Fe/Ti-MOF photocatalysts for efficient nitrogen fixation under mild conditions

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-04-01 DOI: 10.1016/j.mcat.2025.115063

Can Sun , Runze Guo , Zhexiao Zhu , Shouxin Zhu , Jingyi Qu , Zijie Fang , Xiaolu Xu , Jiahui Lin , Yangben Chen , Shijie Zhang , Hui Zheng

引用次数: 0

CuOx/CoOx tandem catalyst for effectively reducing nitrate to ammonia

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-04-01 DOI: 10.1016/j.mcat.2025.115056

Li Xing , Yuhong Wang , Ke Lin , Wei Liu , Rui Cao , Lei Song

{"title":"CuOx/CoOx tandem catalyst for effectively reducing nitrate to ammonia","authors":"Li Xing , Yuhong Wang , Ke Lin , Wei Liu , Rui Cao , Lei Song","doi":"10.1016/j.mcat.2025.115056","DOIUrl":"10.1016/j.mcat.2025.115056","url":null,"abstract":"<div><div>Electrocatalytic nitrate reduction reaction (NO<sub>3</sub>RR) offers a promising alternative to the Haber–Bosch process but requires efficient NH<sub>4</sub><sup>+</sup> electrocatalysts with enhanced performance and selectivity. Although copper-based catalysts have been extensively researched and employed in electrocatalytic NO<sub>3</sub>RR, the robust adsorption of intermediates and poor hydrolytic association activity of the catalysts result in reduced ammonia selectivity and interference of competing reactions. This study describes a nanoscale CuOx and CoOx coupling catalyst (CuOx/CoOx) with the most suitable ratio and tandem structure. Efficient and highly selective elimination of NO<sub>3</sub><sup>−</sup> was accomplished through the tandem catalysis of two oxides. Efficient and notably selective elimination of NO<sub>3</sub><sup>−</sup> was accomplished through the tandem catalysis of the two oxides. The CuOx/CoOx tandem catalyst achieved a NH<sub>4</sub><sup>+</sup> selectivity of 90.1 %, NH<sub>4</sub><sup>+</sup> Faraday efficiency of 95.3 % at a NO<sub>3</sub><sup>−</sup> concentration of 400 mg/L with a cathodic potential of −0.58 V vs. RHE, and showed desirable stability, attributed to the twin lively website synergy and oxygen vacancy defects of the catalyst.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"579 ","pages":"Article 115056"},"PeriodicalIF":3.9,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143746392","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

Effect of NH3-assisted Cu-modified NaX catalysts on acid-base property and their synergy in side chain alkylation of toluene with methanol

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-03-31 DOI: 10.1016/j.mcat.2025.115065

Faraz Ahmad , Yueli Wen , Muhammad Zeeshan , Bin Wang , Samia Kausar , El Gharrabi Mohamed , Wei Huang

{"title":"Effect of NH3-assisted Cu-modified NaX catalysts on acid-base property and their synergy in side chain alkylation of toluene with methanol","authors":"Faraz Ahmad , Yueli Wen , Muhammad Zeeshan , Bin Wang , Samia Kausar , El Gharrabi Mohamed , Wei Huang","doi":"10.1016/j.mcat.2025.115065","DOIUrl":"10.1016/j.mcat.2025.115065","url":null,"abstract":"<div><div>Achieving an optimal acid-base synergy and uniform dispersion of active sites on catalyst surface is essential for high catalytic performance in the side chain alkylation of toluene with methanol (SATM). Herein, we report that ammonium (NH₃) treatment of Cu-modified NaX zeolite catalysts effectively modulates acid-base properties and enhances the dispersion of Cu active sites across the catalyst surface. A series of Cu-modified catalysts were prepared with and without NH₃ treatment and further modified with NaOH to evaluate their synergistic effects. Comprehensive characterization techniques, including Scanning Electron Microscopy (SEM), HAADF-STEM and EDS, Pyridine FTIR, Temperature-Programmed Desorption of NH₃ (TPD-NH₃), X-ray Photoelectron Spectroscopy (XPS O <em>1</em> s), and regression analysis, were used to correlate catalyst structure, and acid-base property and nature of acid sites with catalytic performance. Results reveal that NH₃ incorporation into the Cu-modified NaX framework significantly enhances catalytic efficiency by tuning acid-base properties and promoting a homogeneous distribution of Cu active sites. Notably, the 3Cu-4Na-N catalyst achieved a superior yield of ethylbenzene and styrene production, reaching 84.9 %, compared to 64.3 % for the 3Cu-4Na catalyst under identical conditions. Methanol conversion reached 97.7 %, with the catalyst demonstrating robust stability over 168 h of operation. Additionally, 3Cu-4Na-N catalyst exhibited the highest turnover frequency (TOF) reaching 27.3 h<sup>-1</sup>, confirming its superior intrinsic activity. This study highlights the critical role of NH₃ in advancing Cu-NaX catalysts for SATM and provides a promising strategy for optimizing catalytic performance through controlled acid-base interactions and active site dispersion.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"579 ","pages":"Article 115065"},"PeriodicalIF":3.9,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143746390","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