Molecular Catalysis最新文献_第2页

Theoretical insights into H2S desulfurization: Catalysis by binuclear cobalt phthalocyanine

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-11-29 DOI: 10.1016/j.mcat.2024.114734

Yang Wang , Bo Zhu , Liang Zhao , Bao-Li Li , Zhong-Min Su , Wei Guan

引用次数: 0

Role of “post-coordination interaction” boosted performance of rare-earth based MOFs derived catalyst for hydrogenation-alkylation cascade reaction

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-11-29 DOI: 10.1016/j.mcat.2024.114735

Danfeng Deng , Wenjing Song , Qiang Li , Weizuo Li , Xin Wang

{"title":"Role of “post-coordination interaction” boosted performance of rare-earth based MOFs derived catalyst for hydrogenation-alkylation cascade reaction","authors":"Danfeng Deng , Wenjing Song , Qiang Li , Weizuo Li , Xin Wang","doi":"10.1016/j.mcat.2024.114735","DOIUrl":"10.1016/j.mcat.2024.114735","url":null,"abstract":"<div><div>Post-coordination interactions (abbreviated as <em>PCI</em>) play an essential role in the synthesis and optimization of catalysts by influencing their coordination environment, stabilizing reaction intermediates, tuning activity, and allowing for dynamic behavior. In this work, a LaOCl incorporated into carbon-nitrogen supported metallic Co and CoFe alloy catalyst (termed as CF/L-CN-<em>PCI</em>) via <em>PCI</em> strategy has been synthesized. This catalyst was then utilized in a cascade reaction involving nitroarenes and benzyl alcohol. The developed CF/L-CN-<em>PCI</em> catalyst exhibits higher catalytic selectivity compared to CF/L-CN-<em>IWI</em> catalyst prepared by <em>IWI</em> method in cascade reactions. Additionally, this catalyst offers ease of separation and demonstrates good catalytic cycle stability. Various characterization techniques and control experiments were employed to validate the reasons for the enhanced catalytic performance and to investigate the key issues such as the rate-determining step during the reaction process. We hope that this catalyst preparation method can serve as a reference for the development of other superior catalysts and their application in different reactions.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"572 ","pages":"Article 114735"},"PeriodicalIF":3.9,"publicationDate":"2024-11-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142747907","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 vitro activation of recombinant pro-protein-glutaminases from Bacteroides helcogenes and Flavobacterium sp.

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-11-29 DOI: 10.1016/j.mcat.2024.114718

Gudrun Horstmann, Anja Luz, Julius Plomer, Eva Pross, Ines Seitl, Lucas Kettner, Lutz Fischer

{"title":"In vitro activation of recombinant pro-protein-glutaminases from Bacteroides helcogenes and Flavobacterium sp.","authors":"Gudrun Horstmann, Anja Luz, Julius Plomer, Eva Pross, Ines Seitl, Lucas Kettner, Lutz Fischer","doi":"10.1016/j.mcat.2024.114718","DOIUrl":"10.1016/j.mcat.2024.114718","url":null,"abstract":"<div><div>Protein-glutaminases (PGs) are extracellular enzymes and catalyze the deamidation of protein-bound glutamine residues in other proteins. This often increases the respective protein's solubility. Therefore, PGs are interesting for the food industry since protein-rich foods are trending. Microbial PGs are intracellularly produced in their inactive zymogenic pre-pro-form and subsequently activated after the secretion process, whereby the pre-pro-peptide sequence is cleaved off extracellularly by an endogenous peptidase. However, a former study showed that a recombinantly produced pro-PG from <em>Bacteroides helcogenes</em> (PGB) was surprisingly active, although the pro-peptide was still attached. In this study, the specific <em>in vitro</em> cleavage of the PGB pro-peptide by HRV-3C peptidase was investigated and led to a 16-fold activity increase compared to the non-cleaved pro-PGB. Alternatively, trypsin was used for activation (17.5-fold activity increase) and mass spectrometry analysis revealed that the pro-peptide was indeed cleaved in proximity to the putative native cleavage site. In addition, another formerly unknown PG from <em>Flavobacterium</em> sp. 316 (PGF) was recombinantly produced as pro-PGF in <em>E. coli</em>, partially purified, and biochemically characterized. Pro-PGF was almost inactive, but was activated similarly to pro-PGB through <em>in vitro</em> pro-peptide hydrolysis with trypsin. The mature PGF showed maximal specific activity of 123.7 nkat mg<sup>−1</sup> at 35 °C and pH 9.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"572 ","pages":"Article 114718"},"PeriodicalIF":3.9,"publicationDate":"2024-11-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142747908","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Unveiling the role of aniline as a Brønsted base in Rh-catalyzed C−H alkylation: Computational insights into amino-assisted outer-sphere CMD

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-11-28 DOI: 10.1016/j.mcat.2024.114715

Weirong Wu , Ju Peng , Xiaoqian He , Wenxuan Lin , Kangbao Zhong , Tao Zhang , Ruopeng Bai , Yu Lan

{"title":"Unveiling the role of aniline as a Brønsted base in Rh-catalyzed C−H alkylation: Computational insights into amino-assisted outer-sphere CMD","authors":"Weirong Wu , Ju Peng , Xiaoqian He , Wenxuan Lin , Kangbao Zhong , Tao Zhang , Ruopeng Bai , Yu Lan","doi":"10.1016/j.mcat.2024.114715","DOIUrl":"10.1016/j.mcat.2024.114715","url":null,"abstract":"<div><div>C−H bond cleavage is a key step for the formation of new C−Rh bond in Rh-catalyzed alkylation of aniline derivatives. Due to the inherent basicity of aniline, there is ongoing debate regarding its ability to act as a Brønsted base to assist C−H bond cleavage in these type reactions. In this report, we present computational evidence supporting an amino-assisted outer-sphere concerted metalation-deprotonation (CMD) mechanism. Here, the aniline acts as a Brønsted base to facilitate C−H bond cleavage without any direct interaction between the Rh and the aniline. This amino-assisted outer-sphere CMD pathway is found to be lower in energy compared with the inner-sphere CMD and other base-assisted C−H bond cleavage pathways, providing new insights into the mechanism of Rh-catalyzed C−H functionalization of aniline derivatives. Geometric analysis was conducted to elucidate details of the C−H bond cleavage process. This mechanistic study of C−H bond cleavage in Rh-catalyzed oxidative C−H alkylation of aniline derivatives with allyl alcohols is an important case study of the involvement of amino-assisted outer-sphere CMD in Rh catalysis. We anticipate that the novel amino-assisted outer-sphere CMD mode may extend to other C−H bond functionalization processes and explain the unique effectiveness of aniline in many instances.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"572 ","pages":"Article 114715"},"PeriodicalIF":3.9,"publicationDate":"2024-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142748006","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

Kinetic study of the double dehydration of sorbitol into isosorbide over commercial sulfonic acid resin 在商用磺酸树脂上将山梨醇双脱水成异山梨醇的动力学研究

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-11-26 DOI: 10.1016/j.mcat.2024.114716

Natthaphong Lertna , Supinya Nijpanich , Arthit Neramittagapong , Sutasinee Neramittagapong , Shawn C. Rood

{"title":"Kinetic study of the double dehydration of sorbitol into isosorbide over commercial sulfonic acid resin","authors":"Natthaphong Lertna , Supinya Nijpanich , Arthit Neramittagapong , Sutasinee Neramittagapong , Shawn C. Rood","doi":"10.1016/j.mcat.2024.114716","DOIUrl":"10.1016/j.mcat.2024.114716","url":null,"abstract":"<div><div>Biomass-derived chemicals show great promise as an alternative resource for the replacement of fossil fuel-derived chemicals. The double dehydration of sorbitol produces isosorbide, which is an important chemical building platform and a component in food, pharmaceuticals, and plasticizers. Homogeneous catalysts are used to perform this reaction due to their good performance, but they also exhibit some drawbacks. Therefore, in this study, the sulfonic acid resin Purolite CT269 was used as a heterogeneous catalyst to study isosorbide production. The reaction was carried out with a 4.43 wt.% catalyst loading, reaction temperature of 151 °C, and reaction time of 4 h under a vacuum. 100 % conversion of sorbitol was observed within 2 h, and an isosorbide yield of about 78 % was achieved after 4 h. The kinetics of the reaction were evaluated, the rate law followed a first-order reaction model, and the reaction rate depended on the concentration of reactant. The Langmuir–Hinshelwood–Hougen–Watson (LHHW) model was used to determine that the first dehydration was the rate-determining step of this reaction. The study also examined the deactivation of the catalyst using FE-SEM, N<sub>2</sub> adsorption/desorption, DSC, TGA, and XPS, confirming that changes to the catalytic properties after the reaction negatively impacted the performance of the sorbitol dehydration reaction. The catalytic performance and kinetic analysis were used to explain the mechanism of the double dehydration of sorbitol into isosorbide, providing essential information for catalyst and isosorbide production process design.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"572 ","pages":"Article 114716"},"PeriodicalIF":3.9,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142699043","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 and selective oxidation of methane into methanol over Cu/Fe-containing zeolites 在含铜/铁沸石上将甲烷直接和选择性氧化成甲醇

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-11-26 DOI: 10.1016/j.mcat.2024.114721

Yue Jiang , Tao Yu , Shanghong Zeng , Wenhao Luo

{"title":"Direct and selective oxidation of methane into methanol over Cu/Fe-containing zeolites","authors":"Yue Jiang , Tao Yu , Shanghong Zeng , Wenhao Luo","doi":"10.1016/j.mcat.2024.114721","DOIUrl":"10.1016/j.mcat.2024.114721","url":null,"abstract":"<div><div>Direct transformation of methane into methanol with high selectivity under mild conditions is one of the holy grails in catalysis. The major challenges arise from the high stability of the primary C-H bonds and the facile overoxidation of methanol. Among the numerous catalytic materials applied, Cu/Fe-containing zeolite catalysts have garnered considerable efforts and intensive investigation due to their significant advantages and distinctive potential in direct and selective oxidation of methane into methanol. In this Prospect, we present the recent progress of the application of Cu/Fe-containing zeolites as catalysts for the direct oxidation of methane into methanol. Furthermore, the state-of-the-art <em>ex</em>/<em>in situ</em> characterization techniques applied to understand the intrinsic active sites and reaction mechanisms for Cu/Fe-containing zeolites are also highlighted. Finally, the open challenges and opportunities regarding rational design of catalysts, the development of correlative <em>in situ</em>/<em>operando</em> characterization technologies and the feasible approaches by coupling with external energy resources or with other promising C-C coupling processes, are examined for inspiring future directions.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"571 ","pages":"Article 114721"},"PeriodicalIF":3.9,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723303","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

Oxidation of benzyl alcohol derivatives into carboxylic acids with a new Acetobacter malorum strain: boosting the productivity in a continuous flow system 利用新的恶性醋酸杆菌菌株将苯甲醇衍生物氧化成羧酸：提高连续流动系统的生产率

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-11-26 DOI: 10.1016/j.mcat.2024.114698

Luca Nespoli , Silvia Donzella , Emma Ribul Moro , Jair Mafezoli , Martina Letizia Contente , Diego Romano , Francesco Molinari

{"title":"Oxidation of benzyl alcohol derivatives into carboxylic acids with a new Acetobacter malorum strain: boosting the productivity in a continuous flow system","authors":"Luca Nespoli , Silvia Donzella , Emma Ribul Moro , Jair Mafezoli , Martina Letizia Contente , Diego Romano , Francesco Molinari","doi":"10.1016/j.mcat.2024.114698","DOIUrl":"10.1016/j.mcat.2024.114698","url":null,"abstract":"<div><div>The one-shot green oxidation of different benzyl alcohol derivatives into the corresponding carboxylic acids was achieved by using <em>Acetobacter malorum</em> DSM 112354, a newly isolated strain. Oxidation of benzyl alcohol was initially optimized considering productivity after 8 h as response parameter. Under optimized conditions, a set of <em>para-</em>substituted benzyl alcohols was tested, showing the great versatility of <em>Acetobacter malorum</em> DSM 112354 which was able to oxidize all the substrates albeit with different rates and conversions. The effect of the substituent position was subsequently studied using 2-(hydroxymethyl)phenol, 3-(hydroxymethyl)phenol, and 4-(hydroxymethyl)phenol as starting materials, showing that all the substrates were efficiently transformed (74-98% molar conversion in 2-24 h). Finally, the oxidation of 1,4-phenylenedimethanol gave 4-(hydroxymethyl)benzoic acid proceeded with excellent regioselectivity, since <3% of terephthalic acid was observed. This regioselective reaction was optimized using Ba-alginate immobilized cells of <em>Acetobacter malorum</em> DSM 112354 in a continuous multiphasic flow reactor. The process continuously run for 24 h allowed the obtainment of 0.65 g of HMBA using a 14.4 mL reactor. This intensification was associated with upgraded biocatalyst productivity (37.1 mmol<sub>P</sub>/g<sub>cells dry weight</sub>) and space-time yield (45.1 mg<sub>P</sub>/mL d).</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"571 ","pages":"Article 114698"},"PeriodicalIF":3.9,"publicationDate":"2024-11-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142723302","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

Photo-assisted highly efficient electrocatalytic N2 fixation on nonmetal-metal dual atom catalysts through the reversable evolution of active center 通过活性中心的可逆演化，在非金属-金属双原子催化剂上实现光助高效电催化固定 N2

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-11-25 DOI: 10.1016/j.mcat.2024.114712

Zhaolong Xu , Yi Ding , Song Lu , Tiancun Liu , Hailing Liu , Yong Wu , Yafei Zhao , Zhixin Yu

{"title":"Photo-assisted highly efficient electrocatalytic N2 fixation on nonmetal-metal dual atom catalysts through the reversable evolution of active center","authors":"Zhaolong Xu , Yi Ding , Song Lu , Tiancun Liu , Hailing Liu , Yong Wu , Yafei Zhao , Zhixin Yu","doi":"10.1016/j.mcat.2024.114712","DOIUrl":"10.1016/j.mcat.2024.114712","url":null,"abstract":"<div><div>The electrocatalytic reduction naturally abundant dinitrogen (N<sub>2</sub>) to ammonia (NH<sub>3</sub>) offers a promising alternative to the harsh Haber–Bosch process. However, developing catalysts for high-performance electrocatalytic N<sub>2</sub> reduction reaction (NRR) remains a significant challenge. In this study, density functional theory (DFT) calculations were employed to investigate boron-transition metal atom pairs (B–TM) supported on graphitic carbon nitride (g-C<sub>6</sub>N<sub>6</sub>) as dual-atom catalysts for photo-assisted electrocatalysis of NRR. It was demonstrated that B–TM atom pair can be successfully embedded on g-C<sub>6</sub>N<sub>6</sub>. Among the considered B–TM@g-C<sub>6</sub>N<sub>6</sub> catalysts, B–Os@g-C<sub>6</sub>N<sub>6</sub> exhibits exceptional catalytic activity for NRR via a consecutive mechanism, with the lowest overpotential of 0.21 V, outperforming the efficiency of widely used noble catalysts. Notably, both B and Os atoms directly participate in N<sub>2</sub> activation through σ-donation and π*-backdonation mechanism. Furthermore, the adsorption of intermediates can induce the reversable evolution of the active center, accelerating the NRR. Therefore, these novel characteristics endow B–Os dual atom catalyst with excellent NRR performance. Importantly, B–Os@g-C<sub>6</sub>N<sub>6</sub> also shows suitable band edges and high capability of visible-light absorption, which can assist N<sub>2</sub> conversion under visible-light irradiation. This work offers new insights and ideas for designing nonmetal-metal atom pair as dual atom catalyst for the photo-assisted electrocatalytic reduction of N<sub>2</sub> to NH<sub>3</sub>.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"571 ","pages":"Article 114712"},"PeriodicalIF":3.9,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142700278","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

First-principles investigation of novel direct-Z ZnS/ZrS2 heterojunction: Electronic properties and photocatalytic potential 新型直接-Z ZnS/ZrS2 异质结的第一性原理研究：电子特性和光催化潜力

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-11-25 DOI: 10.1016/j.mcat.2024.114713

Xingzhong Luo , Qingyi Feng , Biyi Wang , Hongxiang Deng , Chuanpeng Ge , Chi He , Bo Li

{"title":"First-principles investigation of novel direct-Z ZnS/ZrS2 heterojunction: Electronic properties and photocatalytic potential","authors":"Xingzhong Luo , Qingyi Feng , Biyi Wang , Hongxiang Deng , Chuanpeng Ge , Chi He , Bo Li","doi":"10.1016/j.mcat.2024.114713","DOIUrl":"10.1016/j.mcat.2024.114713","url":null,"abstract":"<div><div>The potential of ZnS/ZrS<sub>2</sub> heterojunction as a high-efficiency photocatalyst is studied by first-principles calculations in this work. The calculated results show that the ZnS/ZrS<sub>2</sub> heterojunction processes a 1.64 eV narrow direct band gap to enhance visible light absorption and a favorable staggered band alignment conducive to efficient charge separation. The internal electric field between ZnS and ZrS<sub>2</sub> blocks the transfer channels of carriers which confines electrons in ZnS layer and holes in ZrS<sub>2</sub> layer to facilitate redox reaction. Thus, the overall water splitting can be achieved in Z-scheme. The catalytic activity of redox reaction on the surface of ZnS/ZrS<sub>2</sub> heterojunction is demonstrated through the analysis of Gibbs free energy. The probable adsorption site for the OER and HER process is the top-site of Zr atom and S atom, respectively. The 1.78 and 2.43 eV external potential endows the heterojunction with the conducive to the HER and OER, respectively. The catalytic efficiency is guaranteed by a 29.64% STH efficiency. Notably, 32.58% efficiency can be achieved, due to compressive strain induced band gap reduction and visible-light optical absorption enhancement. These findings suggest that the ZnS/ZrS<sub>2</sub> heterojunction has great potential as a photocatalytic material.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"571 ","pages":"Article 114713"},"PeriodicalIF":3.9,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142700274","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

Enhanced activity for producing CO2-based polyols enabled by Zn-Co DMC/c-CTA catalytic system 利用 Zn-Co DMC/c-CTA 催化系统提高生产二氧化碳基多元醇的活性

IF 3.9 2区化学

Molecular Catalysis Pub Date : 2024-11-25 DOI: 10.1016/j.mcat.2024.114693

Tao Liu, Youcai Zhu, Yue Mu, Xindi Feng, Zhen Liu

{"title":"Enhanced activity for producing CO2-based polyols enabled by Zn-Co DMC/c-CTA catalytic system","authors":"Tao Liu, Youcai Zhu, Yue Mu, Xindi Feng, Zhen Liu","doi":"10.1016/j.mcat.2024.114693","DOIUrl":"10.1016/j.mcat.2024.114693","url":null,"abstract":"<div><div>CO<sub>2</sub>-based polyols have a unique terminal hydroxyl group structure that makes them suitable for the production of high-performance polyurethane foams. Zn-Co double metal cyanides (DMC) are an important class of catalysts for the copolymerization reaction of CO<sub>2</sub> with propylene oxide (PO). In the DMC-catalyzed CO<sub>2</sub>/PO copolymerization to produce CO<sub>2</sub>-based polyols, the crucial role of chain transfer agents (CTAs) is emphasized. In this work, a high-performance composite CTA (c-CTA) was successfully developed by investigating various dicarboxylic acids and polypropylene glycol (PPG-400) as CTAs. This system combines the high reaction rate of the DMC/PPG-400 system with the high CO<sub>2</sub> insertion rate of the DMC/sebacic acid (SA) system, achieving 2-3 times higher activity than that of single CTA (PPG-400 or SA), reaching 0.5 kg/g. The molecular characteristics of the CO<sub>2</sub>-based polyols synthesized by different DMC/CTAs systems were analyzed by FTIR and <sup>1</sup>H NMR. The reasons for the high catalytic activity of the DMC/c-CTA system were elucidated by analyzing the hydrogen bond distribution in each DMC/CTA systems. Overall, this work provides a theoretical guidance for the development of novel CO<sub>2</sub>-based materials with high industrial application value.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"571 ","pages":"Article 114693"},"PeriodicalIF":3.9,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142700276","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