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Rational design of CdS/NH2-UiO-66(Zr) nanocomposites via robust covalent linkages for photocatalytic coproduced H2 and organic compounds
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-11 DOI: 10.1016/j.mcat.2025.115017
Yuhuan Qin , Guoguo Yuan , Xiaowei Guo , Mingming Hao
{"title":"Rational design of CdS/NH2-UiO-66(Zr) nanocomposites via robust covalent linkages for photocatalytic coproduced H2 and organic compounds","authors":"Yuhuan Qin ,&nbsp;Guoguo Yuan ,&nbsp;Xiaowei Guo ,&nbsp;Mingming Hao","doi":"10.1016/j.mcat.2025.115017","DOIUrl":"10.1016/j.mcat.2025.115017","url":null,"abstract":"<div><div>Photocatalytic hydrogen (H<sub>2</sub>) evolution from organic substrates is an appealing process since H<sub>2</sub> and high-value chemicals can be simultaneously produced by harnessing solar radiation through the utilization of semiconductor photocatalysts. Herein, we report the preparation of CdS/NH<sub>2</sub>-UiO-66(Zr) nanocomposites, in which CdS quantum dots (QDs) are firmly immobilized on NH<sub>2</sub>-UiO-66(Zr) through a robust covalent assembly strategy. The resulting CdS/NH<sub>2</sub>-UiO-66(Zr) nanocomposites demonstrate remarkable performance in the coproduction of hydrobenzoin (HB) and H<sub>2</sub> from benzyl alcohol under visible-light irradiation, owing to the strong interfacial interaction. The significantly superior activity exhibited over the CdS/NH<sub>2</sub>-UiO-66(Zr) nanocomposites, when contrasted with that over a simple grinding of CdS and NH<sub>2</sub>-UiO-66(Zr), strikingly emphasizes the pivotal significance of rational interface engineering within photocatalytic systems. This work presents a green and sustainable approach for the synthesis of hydrobenzoins and paves the way for further exploration and optimization of semiconductor QDs/metal-organic frameworks nanocomposites.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 115017"},"PeriodicalIF":3.9,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143593793","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
NH3 synthesis via photo-assisted thermalcatalytic NO and H2O reduction by CO over Pd/TiO2: Synergistic effects of Pd and oxygen vacancies
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-10 DOI: 10.1016/j.mcat.2025.115008
Gang Cheng , Junhua Zou , Xinjie Song , Hongmei Tang , Qing Gong , Hongxian Liu , Wenxin Dai
{"title":"NH3 synthesis via photo-assisted thermalcatalytic NO and H2O reduction by CO over Pd/TiO2: Synergistic effects of Pd and oxygen vacancies","authors":"Gang Cheng ,&nbsp;Junhua Zou ,&nbsp;Xinjie Song ,&nbsp;Hongmei Tang ,&nbsp;Qing Gong ,&nbsp;Hongxian Liu ,&nbsp;Wenxin Dai","doi":"10.1016/j.mcat.2025.115008","DOIUrl":"10.1016/j.mcat.2025.115008","url":null,"abstract":"<div><div>Upcycling of NO into NH<sub>3</sub> provided a win-win strategy for NO purification and NH<sub>3</sub> production. In this work, we reported an approach for NH<sub>3</sub> production via photo-assisted thermalcatalytic NO and H<sub>2</sub>O reduction by CO at low temperature and atmospheric pressure. Herein, a Pd/TiO<sub>2</sub> model catalyst with electron-enriched Pd and oxygen vacancies dual active sites was applied. The results showed that full NO conversion was realized only at 120 °C, and a beyond 55.0% NH<sub>3</sub> selectivity could be obtained below 180 °C over Pd/TiO<sub>2</sub>. A series of collective spectroscopic and theoretical investigations revealed that CO adsorbed at Pd site and H<sub>2</sub>O dissociated at interfacial oxygen vacancies would first interact to <em>in situ</em> generate active *H species, and then NO also adsorbed at interfacial oxygen vacancies was gradually hydrogenated by *H to produce NH<sub>3</sub>. Light irradiation further reinforced this process by promoting oxygen vacancies formation and electron transfer for enhancing CO and NO activation and H<sub>2</sub>O dissociation. This work provides a valuable insight into NH<sub>3</sub> production via photothermal catalytic NO and H<sub>2</sub>O reduction by CO.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 115008"},"PeriodicalIF":3.9,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577726","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
Rare earth metal modified CaO catalysts Ln/CaO (Ln=La, Ce, Nd) for oxidative coupling methane: Revealing the interaction between metal oxide and carrier
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-10 DOI: 10.1016/j.mcat.2025.115014
Yanling Yu, Jingxuan Guo, Guizhu Zhang, Mingyi Wang, Junwen Wang
{"title":"Rare earth metal modified CaO catalysts Ln/CaO (Ln=La, Ce, Nd) for oxidative coupling methane: Revealing the interaction between metal oxide and carrier","authors":"Yanling Yu,&nbsp;Jingxuan Guo,&nbsp;Guizhu Zhang,&nbsp;Mingyi Wang,&nbsp;Junwen Wang","doi":"10.1016/j.mcat.2025.115014","DOIUrl":"10.1016/j.mcat.2025.115014","url":null,"abstract":"<div><div>Herein, a series of rare earth metal-modified alkaline earth metal oxide CaO Ln/CaO (Ln=La, Ce, Nd) catalysts were synthesized by sol-gel method and used for OCM reaction. Their reaction performance is not solely influenced by rare earth oxide and carrier CaO, but rather by their interaction. Specifically, the interaction between rare earth oxide and the CaO carrier can increase the surface basicity, the amount of strong basic sites and reactive oxygen species O<sub>2</sub><sup>-</sup>, thereby further enhancing the catalytic performance compared to rare earth oxide and the CaO carrier. In addition, the basicity of rare earth oxides affects the concentration of oxygen vacancies in the modified catalyst. The stronger the basicity of rare earth oxides, the more abundant the concentration of oxygen vacancies generated by their interaction with the carrier. The DFT calculation results indicate that the Ln/CaO (100) surface is conducive to the generation of O<sub>2</sub><sup>-</sup>, which easily activates methane to produce methyl radicals, and then desorb into the gas phase and couple to form C<sub>2</sub>H<sub>6</sub>.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 115014"},"PeriodicalIF":3.9,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577725","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
Aerobic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid by modification of the crystalline structure of MnO2 for catalytic purposes
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-10 DOI: 10.1016/j.mcat.2025.114995
Wenbo Liao , Shibo Yang , Yadong Liu , Qing Yin , Xing Tang , Lu Lin , Yong Sun
{"title":"Aerobic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid by modification of the crystalline structure of MnO2 for catalytic purposes","authors":"Wenbo Liao ,&nbsp;Shibo Yang ,&nbsp;Yadong Liu ,&nbsp;Qing Yin ,&nbsp;Xing Tang ,&nbsp;Lu Lin ,&nbsp;Yong Sun","doi":"10.1016/j.mcat.2025.114995","DOIUrl":"10.1016/j.mcat.2025.114995","url":null,"abstract":"<div><div>Investigating the various polymorphs of MnO<sub>2</sub> for the catalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is motivated by the pressing demand to engineer sustainable and proficient catalytic pathways. These pathways are essential for transforming renewable biomass into valuable chemicals, thereby facilitating the shift towards a circular economy and diminishing our dependence on fossil fuel-derived resources. Herein, three MnO<sub>2</sub> catalysts with different crystal structures were prepared for the efficient catalytic oxidation of HMF to FDCA. The results showed that α-MnO<sub>2</sub> exhibited higher oxidizing activity per unit specific surface area and an appreciably large specific surface area, however, its overall catalytic activity was found to be less than that of β-MnO<sub>2</sub>. XRD, SEM, and other characterizations suggest that the presence of smaller nanorods or amorphous particles with reduced crystallinity on the surface of the α-MnO<sub>2</sub> catalysts could be responsible for a decreased lattice oxygen content, thereby diminishing their catalytic activity. To validate this conjecture, this paper cites for the first time the application of a dilute nitric acid immersion treatment in the chemical industry to eliminate amorphous structures from catalysts. The α-MnO<sub>2</sub>-H<sup>+</sup> catalyst, prepared using this innovative method demonstrated exceptional activity in facilitating the conversion of HMF to FDCA under more stringent reaction conditions than any monometallic catalysts previously reported. According to the kinetic analysis of the reaction, it was established that the oxidation of 5-formyl-2-furancarboxylic acid (FFCA) to FDCA constitutes the rate-limiting step within the entire oxidation process. On this basis, FT-IR studies showed that the oxidation initiates at the -CHO terminus of HMF, leading to the formation of intermediates 5-hydroxymethylfurfurylacetic acid and 5-formylfurfurylacetic acid within the Mn<sup>4+</sup>/Mn<sup>3+</sup> redox cycle. In conclusion, the enhancement of catalytic activity by diluting nitric acid immersion treatment presents a promising avenue for further research and application in the field of green chemistry.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 114995"},"PeriodicalIF":3.9,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577727","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
Targeted acquisition furfural from xylose using sulfonic acid-functionalized organo-inorganic hybrid silica materials
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-10 DOI: 10.1016/j.mcat.2025.114996
Wenting Zou , Li Yang , Zidie Duan , Jianhua Wang , Shoulin Zhou , Dulin Yin , Qiong Xu , Xianxiang Liu
{"title":"Targeted acquisition furfural from xylose using sulfonic acid-functionalized organo-inorganic hybrid silica materials","authors":"Wenting Zou ,&nbsp;Li Yang ,&nbsp;Zidie Duan ,&nbsp;Jianhua Wang ,&nbsp;Shoulin Zhou ,&nbsp;Dulin Yin ,&nbsp;Qiong Xu ,&nbsp;Xianxiang Liu","doi":"10.1016/j.mcat.2025.114996","DOIUrl":"10.1016/j.mcat.2025.114996","url":null,"abstract":"<div><div>The catalytic dehydration of hemicellulose-derived xylose to furfural is a promising and appealing strategy for the effective utilization of biomass. A kind of sulfonic functionalized organic-inorganic hybrid silica materials (OIHMs-SO<sub>3</sub>H), using tetraethyl orthosilicate (TEOS) and 3-mercaptopropyltrimethoxysilane (MPTMS) as the starting precursors, were prepared via a sol-gel method which showed excellent catalytic performance for the dehydration of xylose to furfural. The microscopic structure, chemical composition and pore structure were ascertained by means of various characterization methods, such as SEM,FT-IR,TG-DTG,N<sub>2</sub> adsorption-desorption. 93.4 % conversion of xylose and 74.5 % selectivity of furfural was achieved under optimal conditions. More importantly, the catalysts displayed relatively high stability in five consecutive experimental cycles despite some acid sites covered by humus. In addition, the kinetics of reaction in this catalytic system were further investigated which demonstrated that the activation energy of xylose degradation (67.2 kJ/mol) was lower than that of xylose dehydration (122.8 kJ/mol) and furfural degradation (137.5 kJ/mol). All in all, this work provided an effective avenue for the synthesis of organic-inorganic hybrid silica materials applied to the conversion of xylose to furfural.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 114996"},"PeriodicalIF":3.9,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577023","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
Hydrothermal synthesis of calcium methoxide nano-catalyst for palm oil based biolubricant production
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-10 DOI: 10.1016/j.mcat.2025.115010
Lalita Attanatho , Amornrat Suemanotham , Yoothana Thanmongkhon , Wanchana Sisuthog , Paweesuda Natewong , Prasert Reubroycharoen , Songyoot Kaewmala , Natthawan Prasongthum
{"title":"Hydrothermal synthesis of calcium methoxide nano-catalyst for palm oil based biolubricant production","authors":"Lalita Attanatho ,&nbsp;Amornrat Suemanotham ,&nbsp;Yoothana Thanmongkhon ,&nbsp;Wanchana Sisuthog ,&nbsp;Paweesuda Natewong ,&nbsp;Prasert Reubroycharoen ,&nbsp;Songyoot Kaewmala ,&nbsp;Natthawan Prasongthum","doi":"10.1016/j.mcat.2025.115010","DOIUrl":"10.1016/j.mcat.2025.115010","url":null,"abstract":"<div><div>The present work investigated the biolubricant production from palm oil-based methyl ester over calcium methoxide nanocatalyst. The hydrothermal method was employed in this work to prepare nano-calcium methoxide. The difference of hydrothermal synthesis time influenced on the catalytic characteristics and performances was studied. The catalytic activity showed a significant dependence on the catalyst's basic sites and particle size, achieving a palm oil methyl ester conversion of 78–89 % and a selectivity of 62–80 % for biolubricant production. The calcium methoxide with a hydrothermal synthesis time of 6 h exhibited superior catalytic activity to the other catalysts as a result of its small particle size and high basicity. Additionally, the calcium methoxide catalyst apparently showed good stability and reutilization, with palm oil methyl ester conversion of 85 % after use for 6 consecutive cycles. The physicochemical properties of the obtained biolubricant aligned closely the ISO VG 46 mineral oil, especially regarding viscosity and flash point. However, due to its high pour point, the obtained biolubricant may be most suitable for applications in tropical climates without winter conditions</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 115010"},"PeriodicalIF":3.9,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577024","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
Acidic photosensitizers promote the efficient photooxygenation of aromatic substrates catalyzed by anthraquinone-2-carboxylic acid through proton-coupled electron transfer and particle aggregation effect
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-10 DOI: 10.1016/j.mcat.2025.114955
Dabo Jiang , Weijie Zhou , Hongbo Peng , Yuncheng Xie , Shuting Liang , Tao Yang , Guangmei Xie , Bingbing Wang , Zaihui Fu , Anqun Su
{"title":"Acidic photosensitizers promote the efficient photooxygenation of aromatic substrates catalyzed by anthraquinone-2-carboxylic acid through proton-coupled electron transfer and particle aggregation effect","authors":"Dabo Jiang ,&nbsp;Weijie Zhou ,&nbsp;Hongbo Peng ,&nbsp;Yuncheng Xie ,&nbsp;Shuting Liang ,&nbsp;Tao Yang ,&nbsp;Guangmei Xie ,&nbsp;Bingbing Wang ,&nbsp;Zaihui Fu ,&nbsp;Anqun Su","doi":"10.1016/j.mcat.2025.114955","DOIUrl":"10.1016/j.mcat.2025.114955","url":null,"abstract":"<div><div>This article reports that acidic photosensitizers can significantly enhance the photooxidation of aromatic substrates catalyzed by anthraquinone-2-carboxylic acid (AQ-COOH) through proton-coupled electron transfer and particle aggregation effects, and PhSO<sub>3</sub>H exhibits the best improvement effect for the photooxidation of toluene. Under ambient conditions and visible light irradiation, 41.9 % toluene conversion and 49.0 % benzoic acid (BC) selectivity can be achieved. The introduction of benzenesulfonic acid (PhSO<sub>3</sub>H) can enhance the conversion of toluene to 70.1 % and significantly improve the BC selectivity, which likely originates from the particle aggregation and proton-coupled electron transfer (PCET) effect caused by the π-π interaction between AQ-COOH, PhSO<sub>3</sub>H and aromatic substrates. The PCET mechanism was successfully established by introducing PhSO<sub>3</sub>H into the AQ-COOH-based photooxidation system, resulting in efficient photooxidation of diverse aromatic substrates. The primary photo-generated active species involved in the photooxidation of toluene are superoxide free radicals (O<sub>2</sub><sup>·−</sup>), photogenerated electrons (e<sup>−</sup>), oxygen vacancies (h<sup>+</sup>) and singlet oxygen (<sup>1</sup>O<sub>2</sub>), according to quenching experiments and EPR spectrum characterizations. The current photooxidation methodology exemplifies the O<sub>2</sub>-based selective oxidation of inert hydrocarbons under mild circumstances, aligning with the principles of green chemistry.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 114955"},"PeriodicalIF":3.9,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577728","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
Crystal phase tailored TiO2 for photocatalytic ciprofloxacin (CIP) elimination: Performances, degradation pathways, and toxicity assessment
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-08 DOI: 10.1016/j.mcat.2025.115000
Bingwen Hu , Minjun Jiang , Zhipan Wen , Yubo Song , Gang Cheng
{"title":"Crystal phase tailored TiO2 for photocatalytic ciprofloxacin (CIP) elimination: Performances, degradation pathways, and toxicity assessment","authors":"Bingwen Hu ,&nbsp;Minjun Jiang ,&nbsp;Zhipan Wen ,&nbsp;Yubo Song ,&nbsp;Gang Cheng","doi":"10.1016/j.mcat.2025.115000","DOIUrl":"10.1016/j.mcat.2025.115000","url":null,"abstract":"<div><div>Environmental residues of antibiotic molecules adversely affecting human health and ecological safety. TiO<sub>2</sub>-intervened photocatalytic technology had been praised as a common method for green and efficient degradation of antibiotics. In this work, TiO<sub>2</sub> with different ratios of anatase/rutile crystal phases were synthesized by calcining as-prepared H<sub>2</sub>Ti<sub>5</sub>O<sub>11</sub> at different temperatures. The degradation experiments showed that complete removal of ciprofloxacin (CIP) solution was achieved upon the heterophase TiO<sub>2</sub> with anatase/rutile=92:8. The degradation intermediates and possible degradation pathways of ciprofloxacin were determined by high resolution liquid mass spectrometry (HRMS). The toxic effects of CIP on aquatic organisms during the degradation process was predicted by the ECOSAR program. The monitored pea seedlings growth process showed that the degradation of CIP by heterophase TiO<sub>2</sub> was a friendly process and had almost no negative impact on the environment. This work provided a reference for the tailoring of crystal phase TiO<sub>2</sub> and the toxicity assessment of the degradation process of the ciprofloxacin antibiotic.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 115000"},"PeriodicalIF":3.9,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577026","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
Ni-Mn-Al catalysts obtained from layered double hydroxides for CO2 hydrogenation
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-08 DOI: 10.1016/j.mcat.2025.114965
Joana Mara Polycarpo , Mattheus Torquato , Fatima Maria Zanon Zotin , Maria do Carmo Rangel , Arnaldo da Costa Faro Jr. , Luz Amparo Palacio
{"title":"Ni-Mn-Al catalysts obtained from layered double hydroxides for CO2 hydrogenation","authors":"Joana Mara Polycarpo ,&nbsp;Mattheus Torquato ,&nbsp;Fatima Maria Zanon Zotin ,&nbsp;Maria do Carmo Rangel ,&nbsp;Arnaldo da Costa Faro Jr. ,&nbsp;Luz Amparo Palacio","doi":"10.1016/j.mcat.2025.114965","DOIUrl":"10.1016/j.mcat.2025.114965","url":null,"abstract":"<div><div>It is widely agreed among researchers that global warming is directly linked to increased concentrations of carbon dioxide (CO<sub>2</sub>) in the atmosphere. As such, technologies aimed at reducing CO<sub>2</sub> emissions have been extensively studied. In this study, bimetallic (Ni-Mn, Ni-Al, Mn-Al) and trimetallic (Ni-Mn-Al) precursors were synthesized by a coprecipitation method to obtain layered double hydroxides (LDH). Preparation of the studied catalysts is easily scalable, due to the relative simplicity and reproducibility of LDH synthesis. The effects of pH and molar proportion of the metals on their physical and chemical properties were evaluated. After calcination and in-situ reduction, the oxides were evaluated as catalysts in the CO<sub>2</sub> hydrogenation reaction, which is a possible alternative to the abatement of global warming. It was concluded that Mn increased the specific surface area of the oxides and the content of basic sites in the catalyst, as well as facilitated the onset of the materials reduction. The most active catalyst, obtained at lower pH, had only 6 mol% Mn and showed CO<sub>2</sub> conversion and CH<sub>4</sub> selectivity equal to 82 % and 100 % at 350 °C, respectively. It was also stable during 16 h on stream, at the temperature of maximum conversion. At low temperatures, this catalyst was one of the best reported in the literature, with CO<sub>2</sub> conversion and CH<sub>4</sub> selectivity of 40 % and 100 % at 225 °C, respectively. Additionally, 50 % conversion was achieved at 248 °C (T<sub>50</sub>). At temperatures higher than 400 °C, the reverse water gas shift reaction, which competes with methanation, was inhibited in solids with higher Mn contents (≥ 40 mol%).</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 114965"},"PeriodicalIF":3.9,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577025","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
Soot oxidation performance of Cs-V-based non-noble catalyst used for diesel particulate filter and its regeneration performance by La doping
IF 3.9 2区 化学
Molecular Catalysis Pub Date : 2025-03-07 DOI: 10.1016/j.mcat.2025.114998
Yunhua Zhang, Yaoxin Xu, Sen Zheng, Diming Lou, Liang Fang
{"title":"Soot oxidation performance of Cs-V-based non-noble catalyst used for diesel particulate filter and its regeneration performance by La doping","authors":"Yunhua Zhang,&nbsp;Yaoxin Xu,&nbsp;Sen Zheng,&nbsp;Diming Lou,&nbsp;Liang Fang","doi":"10.1016/j.mcat.2025.114998","DOIUrl":"10.1016/j.mcat.2025.114998","url":null,"abstract":"<div><div>The catalytic diesel particulate filter (CDPF) has consistently been a standard setup for diesel engines. This research introduces and enhances a non-noble metal catalyst, Cs-V, by doping with the rare-earth element La for the CDPF. The impact of La doping on the Cs-V-based soot oxidation catalyst was quantitatively studied using physical and chemical analysis, activity testing, and density functional theory (DFT) techniques. Findings indicated that introducing La into the Cs-V-based non-noble metal catalyst led to an increase in both the surface area and pore volume by 41 % and 18.4 %, respectively. The addition of La enhanced both the clustering and spatial distribution of catalyst particles, positively impacting absorption and catalytic activity. Doping with La significantly increased the chances of oxygen adsorption and dissociation activation in catalytic processes, enhancing the chance of soot-oxidation, lowering the activation energy to 62.1 kJ/mol, and decreasing T<sub>10</sub>(the temperature at which the conversion rate of soot begins to reach 10 %), T<sub>90</sub>(the temperature at which the conversion rate of soot reaches 90 %), and, T<sub>m</sub>(the peak temperature at which the conversion rate of soot reaches) by 70.2 °C, 66.9 °C, and 69.1 °C respectively in contrast to their un-doped counterparts, while concurrently, La doping led to an average 4.5 % boost in the CDPF regeneration effectiveness. DFT simulation indicated that La doping can weaken the bonding between O atoms, lengthen the bond length between V atoms and solid O<sub>asd</sub> within the crystal cell, shorten the bond length between V atoms and solid O<sub>asd</sub> with C<sub>4</sub> molecules, increase the electronegativity of the configuration O<sub>asd</sub>, and make the chemical bonds formed by V*-O* more inclined towards ionic bonds, these changes promote the desorption of -CO<sub>x</sub> groups during soot-oxidation.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"578 ","pages":"Article 114998"},"PeriodicalIF":3.9,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143563448","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
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