Molecular Catalysis最新文献_第2页

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

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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}

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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

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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}

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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

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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}

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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}

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Effect of the dielectric barrier discharge plasma on Cu-based catalysts supported on SiO2 for acetylene hydration

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-03-29 DOI: 10.1016/j.mcat.2025.115064

Yi Cui, Xiejie Chen, Jiaxuan Gao, Shui Liu, Denghao Wang, Caixia Xu

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Unlocking the positive effect of non-polar ZnO facets in ZrZnOx catalysts for CO2 hydrogenation

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-03-28 DOI: 10.1016/j.mcat.2025.115059

Xiaohong Guo, Liqiang Deng, Xiaoyue Wang, Yongjie Zhao, Zhifan Cao, Pengwei Li, Congming Li

{"title":"Unlocking the positive effect of non-polar ZnO facets in ZrZnOx catalysts for CO2 hydrogenation","authors":"Xiaohong Guo, Liqiang Deng, Xiaoyue Wang, Yongjie Zhao, Zhifan Cao, Pengwei Li, Congming Li","doi":"10.1016/j.mcat.2025.115059","DOIUrl":"10.1016/j.mcat.2025.115059","url":null,"abstract":"<div><div>A pivotal aspect in advancing ZrZnO<sub>x</sub> catalysts for CO<sub>2</sub> hydrogenation lies in the modulation of Zr-O-Zn active sites, with ZnO facets emerging as potential modulators of site activity. Whereas the beneficial influence of non-polar ZnO facets on ZrZnO<sub>x</sub> catalysts has been scarcely documented. Our investigation reveals that ZrZnO<sub>x</sub> catalysts exposed non-polar ZnO facets (ZrZnO-n) exhibit superior methanol selectivity (74 %) compared to those with randomly exposed ZnO facets (ZrZnO-r, 35 %). Characterization results demonstrate that it is ascribed to the formation of highly active Zr-O-Zn<sup>(2−δ)+</sup> sites on ZrZnO-n, which facilitate H<sub>2</sub> adsorption and dissociation. In situ spectroscopic studies and DFT calculations further substantiate this finding, demonstrating enhanced intermediates formation and more efficient hydrogenation processes. This research underscores the significance of ZnO facet engineering in the purposeful creation of efficient ZrZnO<sub>x</sub> catalysts for CO<sub>2</sub> hydrogenation.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"579 ","pages":"Article 115059"},"PeriodicalIF":3.9,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143715533","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}

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Integration of Computational Tools for Rational Design of (R)-ω-Transaminases with Enhanced Asymmetric Catalysis

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2025-03-28 DOI: 10.1016/j.mcat.2025.115078

Shujin Liu , Jingang Wang , Bo Yuan , Xin Meng , Ge Qu , Zhoutong Sun

{"title":"Integration of Computational Tools for Rational Design of (R)-ω-Transaminases with Enhanced Asymmetric Catalysis","authors":"Shujin Liu , Jingang Wang , Bo Yuan , Xin Meng , Ge Qu , Zhoutong Sun","doi":"10.1016/j.mcat.2025.115078","DOIUrl":"10.1016/j.mcat.2025.115078","url":null,"abstract":"<div><div>With the rapid development of genomics and high-throughput sequencing technologies, massive amounts of genetic sequence data have become available. However, identifying functional sequences with desired properties from these datasets remains a significant challenge. In biocatalysis, discovering catalysts with suitable stereoselectivity is crucial for asymmetric synthesis. In this study, we developed a streamlined method for the rational design of (<em>R</em>)-ω-transaminases ((<em>R</em>)-ω-TA) sequences. A library of 1620 candidate (<em>R</em>)-ω-TA sequences was generated by <em>in silico</em> DNA shuffling and ancestral sequence reconstruction techniques. After four rounds of machine learning-guided functional prediction and virtually screening, 85 novel TAs were annotated, with a sequence identity varying from 27.1 % to 69.7 %. In the examination of the substrate spectrum, each of the 85 novel TAs was able to catalyze at least three substrates among the tested ketones. Eventually, preparative-scale synthesis of (<em>R</em>)-N-Boc-3-piperidine was performed on a gram-scale. The newly designed TA G6-L164V exhibited a conversion of 98.1 % with a specific activity of 3.9 U/mg, and an enantiomeric excess (<em>ee</em>) > 99 % after 7 h in a 10 mL system containing 50 mM substrate. Our study provides a promising framework for protein sequence design and expands the toolbox of (<em>R</em>)-ω-TA in the synthesis of chiral amines.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"579 ","pages":"Article 115078"},"PeriodicalIF":3.9,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143715534","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}

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