Catalysis LettersPub Date : 2024-09-19DOI: 10.1007/s10562-024-04800-0
Vanjari Pallavi, Reddi Kamesh, K. Yamuna Rani
{"title":"In Silico Models for Prediction of Methanol Yield in CO2 Hydrogenation Reaction Using Cu-Based Catalysts","authors":"Vanjari Pallavi, Reddi Kamesh, K. Yamuna Rani","doi":"10.1007/s10562-024-04800-0","DOIUrl":"10.1007/s10562-024-04800-0","url":null,"abstract":"<p>CO<sub>2</sub> hydrogenation to methanol is instrumental in mitigating carbon emissions and providing a renewable source of clean fuel, methanol. Though Cu-based catalysts proved to be economical and efficient catalysts for this reaction, it has the disadvantage of low catalyst efficiency and sintering. In this study, we developed different six machine learning (ML) models for the prediction of methanol yield (%) from CO<sub>2</sub> hydrogenation for Cu-based catalysts. The gradient boost random trees model outperformed other ML models with accuracy R<sup>2</sup> and RMSE of 0.96, 0.71 on train data and 0.75, 1.75 on test data. Pressure, metal:support ratio, active metal composition, GHSV and reaction temperature were found to be influential parameters for optimization of methanol yield. The prediction capability of this model is also validated based on unseen experimental data with varied input parameters and the predictions are good enough with R<sup>2</sup> and RMSE of 0.9 and 1.14. Therefore, this model can be regarded as a valuable solution to guide experimental design without actual experimentation for Cu-based catalysts.</p>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142518386","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Modification of Pt/SiO2 with Mg(OH)2 Improves Xylose to Xylulose Isomerization","authors":"Wenxuan Li, Ming Chen, Yuanbo Song, Mengyu Jin, Dongsu Bi, Yalei Zhang, Zheng Shen","doi":"10.1007/s10562-024-04824-6","DOIUrl":"10.1007/s10562-024-04824-6","url":null,"abstract":"<div><p>Sugar compounds are an important part of biomass resources, and their catalytic conversion can prepare a series of platform compounds, such as lactic acid and polyols. One of the key steps is the isomerization of aldoses to ketoses. However, finding a simple method to efficiently convert aldoses to ketoses remains a great challenge. Herein, we report a core–shell structured catalyst, Pt/SiO<sub>2</sub>@Mg(OH)<sub>2</sub>, for the efficient conversion of xylose as well as the further conversion of xylose to xylulose. Xylose, a five-carbon sugar unit with the highest content in biomass, was used as the object of study to determine the optimal reaction conditions in the aqueous system by adjusting the loading amount of Mg(OH)<sub>2</sub>, catalyst addition, reaction temperature, and reaction time: In the optimum aqueous conditions, the yield of xylulose was 23.61%. We also investigated the effect of solvent effects on the hydrothermal reaction and determined the optimal solvent ratio, the yield of xylulose reached 31.74% at H<sub>2</sub>O:MeOH (8:2). We anticipate that this research result can provide a theoretical basis and reference for the industrialized production of subsequent sugar isomerization.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142254120","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Catalysis LettersPub Date : 2024-09-17DOI: 10.1007/s10562-024-04826-4
Venkata D. B. C. Dasireddy, Balaga Viswanadham, Blaz Likozar, Jignesh Valand
{"title":"CO-Free Fuel Processing of Water Gas Shift Feedstocks: Effect of Support on CuMn Spinel Performance","authors":"Venkata D. B. C. Dasireddy, Balaga Viswanadham, Blaz Likozar, Jignesh Valand","doi":"10.1007/s10562-024-04826-4","DOIUrl":"10.1007/s10562-024-04826-4","url":null,"abstract":"<div><p>Cleaning up carbon monoxide (CO) in water gas shift feedstocks is crucial for fuel cell applications. The catalytic transformation of CO in hydrogen-rich feeds poses a significant challenge in environmental catalysis. To address this issue, a range of Cu–Mn-based monometallic and bimetallic catalysts with diverse supports (such as alumina, silica, zirconia, and titania) were employed. Temperature programming techniques were utilised to observe the reduction and oxidation behaviours of these catalysts. The investigation involved testing CO oxidation at various temperatures over copper and manganese-based supported catalysts in the presence of H<sub>2</sub>O and CO<sub>2</sub> (simulating realistic conditions). A positive impact of H<sub>2</sub>O on catalytic performance was noted, whereas CO<sub>2</sub> had a suppressive effect. Furthermore, the specific support materials (Al<sub>2</sub>O<sub>3</sub>, SiO<sub>2</sub>, TiO<sub>2</sub>, and ZrO<sub>2</sub>) were studied to understand their roles in CO oxidation under realistic conditions. In the presence of water, alumina catalysts containing bimetallic metals (Cu–Mn) exhibited 100% CO conversion even at a lower temperature of 160 °C. Conversely, under the predominant influence of CO<sub>2</sub>, alumina catalyst (Cu–Mn) showed 55% CO conversion. The exceptional performance was attributed to CO preferential adsorption on highly active Cu–Mn sites and a small H<sub>2</sub>-oxidative atmosphere of the catalysts. The activity results highlighted the strong dependence of CO conversion on reaction temperatures, the presence of metals, and the types of supports. Overall, these findings suggest the potential use of these catalysts for H<sub>2</sub> purification under realistic conditions.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s10562-024-04826-4.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142254122","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Catalysis LettersPub Date : 2024-09-16DOI: 10.1007/s10562-024-04820-w
Longwei Cheng, Pan Wang, Quanxin Ye, Hongyu Zhao, Sheikh Muhammad Farhan, Tong Yan, Hailin Zhao
{"title":"Impact of M (M = Co, Cu, Fe, Zr) Doping on CeO2-Based Catalysts for Ammonia Selective Catalytic Oxidation at Low Temperatures","authors":"Longwei Cheng, Pan Wang, Quanxin Ye, Hongyu Zhao, Sheikh Muhammad Farhan, Tong Yan, Hailin Zhao","doi":"10.1007/s10562-024-04820-w","DOIUrl":"10.1007/s10562-024-04820-w","url":null,"abstract":"<div><p>Selective catalytic conversion of ammonia to nitrogen is an effective method for reducing ammonia emissions from both stationary and mobile sources. In this study, CeO<sub>2</sub>-based catalysts (M/CeO<sub>2</sub>, M = Co, Cu, Fe, Zr) were synthesized using the sol–gel method and subsequently tested on a simulated gas experimental platform to assess their performance in NH<sub>3</sub> selective catalytic oxidation (NH<sub>3</sub>-SCO). Results showed that Co/CeO<sub>2</sub> and Cu/CeO<sub>2</sub> catalysts exhibited high ammonia oxidation activity at respectively low temperatures, with T<sub>50</sub> 196.8 and 229.5 °C, and T<sub>90</sub> 239.2 and 292.1 °C. However, it was observed that while Co/CeO<sub>2</sub> displayed poor N<sub>2</sub> selectivity, Cu/CeO<sub>2</sub> demonstrated good N<sub>2</sub> selectivity. The superior catalytic performance of Cu/CeO<sub>2</sub> and Co/CeO<sub>2</sub> catalysts compared to Fe/CeO<sub>2</sub> and Zr/CeO<sub>2</sub> can be attributed to their distinct interactions with Ce. Subsequent characterization experiments were conducted to elucidate these interactions. BET and SEM analyses revealed that all M/CeO<sub>2</sub> catalysts possessed a typical mesoporous structure. XRD and XPS results indicated that the primary phase of each catalyst was CeO<sub>2</sub>, and the incorporation of M transition metals did not alter the cubic fluorite structure. The interaction between the M metal and Ce varied, impacting the Ce<sup>3+</sup> content on the catalyst surface, which in turn influenced oxygen species adsorption and ammonia oxidation activity. H<sub>2</sub>-TPR and Raman spectroscopy analyses demonstrated that M metal incorporation shifted the CeO<sub>2</sub> reduction peak, thereby altering reduction properties and affecting oxidation performance. In particular, the Co-metal composite shifted the reduction peak to a lower temperature, thereby enhancing the reduction properties and indirectly increasing oxidation activity.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142254121","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Construction of SnO2@CrS2 Nanocuboids Via Solvothermal Synthesis for Photoelectrochemical OER/HER Performance in Alkaline and Acidic Media and Water Detoxification Behavior","authors":"Sidra Aslam, Basharat Ali, Misbah Mirza, Raheela Naz, Waseem Abbas, Muhammad Safdar","doi":"10.1007/s10562-024-04808-6","DOIUrl":"10.1007/s10562-024-04808-6","url":null,"abstract":"<div><p>The electrolytic division of water into hydrogen (H<sub>2</sub>) and oxygen (O<sub>2</sub>) presents a sustainable solution for meeting escalating demands in renewable energy sources. Yet, this process faces formidable challenges due to its energy-intensive nature. Our study introduces efficient electrocatalysts formed from chromium sulphide nanoparticles integrated with tin oxide via a straightforward solvothermal approach, enabling water splitting in both acidic and alkaline settings. The resulting SnO<sub>2</sub>@CrS<sub>2</sub> heterostructure exhibits notable performance by requiring lower overpotentials 142 and 99 mV for achieving a current density of 10 mA cm<sup>−2</sup> during the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in 1 M KOH, and 157 and 165 mV for OER and HER in 0.1 M HClO<sub>4</sub>, respectively. Correspondingly, Tafel slopes of 30 and 45 mVdec<sup>−1</sup> in 1.0 M KOH and 52 and 32 mVdec<sup>−1</sup> in 0.1 M HClO<sub>4</sub> were observed for OER and HER respectively. These catalysts display promising efficiency at reduced overpotentials, demonstrating exceptional performance for overall water splitting. This approach of integrating an active heterostructure through interfacial tuning offers a novel pathway for developing economically viable and efficient electrocatalyst systems crucial for water splitting and H<sub>2</sub> production.</p><h3>Graphical Abstract</h3><p>Graphical abstract of synthesized catalyst</p>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142254123","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Catalysis LettersPub Date : 2024-09-16DOI: 10.1007/s10562-024-04810-y
Snehal A. Jawale, Vijay Mahajan, Bhalchandra M. Bhanage
{"title":"Nanosized-Ni Doped on Montmorillonite Catalysed Suzuki–Miyaura Coupling Reactions","authors":"Snehal A. Jawale, Vijay Mahajan, Bhalchandra M. Bhanage","doi":"10.1007/s10562-024-04810-y","DOIUrl":"10.1007/s10562-024-04810-y","url":null,"abstract":"<div><p>This work reports the synthesis and characterization of Nanosized-Ni doped montmorillonite heterocatalyst and its application for Suzuki Miyaura cross coupling of aryl iodides with aryl boronic acids. The catalyst is highly selective and did not give any other byproducts. The reaction was complete within 24 h with > 98% yield. Nickel was uniformly dispersed on the catalyst with approximately 4.0 ± 2 nm clusters of Ni. The solvent, base, catalyst loading, and catalyst precursors were varied to obtain optimum reaction conditions for highest yield. The catalyst was recovered and reused for reactions demonstrating excellent recyclability with high yield. Ni doped montmorillonite catalyst is very effective for Suzuki Miyaura cross coupling reactions and can be used to replace expensive Pd-based catalysts with earth abundant and inexpensive Ni-based catalysts.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142254153","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Catalysis LettersPub Date : 2024-09-15DOI: 10.1007/s10562-024-04830-8
Kai Wang, Qing Chen, Haiyan Xie, Miao Wang, Xu Kong, Kaiyuan Cheng, Zhiliang Jin
{"title":"The Construction of Type II Cu2O/ZnFe2O4 Heterojunction Promoted the Photocatalytic Hydrogen Production Activity","authors":"Kai Wang, Qing Chen, Haiyan Xie, Miao Wang, Xu Kong, Kaiyuan Cheng, Zhiliang Jin","doi":"10.1007/s10562-024-04830-8","DOIUrl":"10.1007/s10562-024-04830-8","url":null,"abstract":"<div><p>Photocatalytic hydrogen production by semiconductors is an optimal path to achieve solar energy conversion. In this work, Cu<sub>2</sub>O/ZnFe<sub>2</sub>O<sub>4</sub> type II heterostructure is composed of ZnFe<sub>2</sub>O<sub>4</sub> nanoparticles loaded on the surface of Cu<sub>2</sub>O microspheres, the photocatalytic hydrogen evolution performance is studied. Under the irradiation 5 h of 5 w LED lamp, the hydrogen production of Cu<sub>2</sub>O/ZnFe<sub>2</sub>O<sub>4</sub> composites was 30.8 and 12.7 times higher than pure Cu<sub>2</sub>O and pure ZnFe<sub>2</sub>O<sub>4</sub>, respectively. In addition, after four cycles of experiments for 20 h, the hydrogen production is still maintained at 67.4% of the initial activity, indicating the relatively stable hydrogen evolution activity of the composite material. The electron transfer mechanism of the photocatalyst was confirmed through the utilization of density functional theory (DFT) and in-situ irradiation X-ray photoelectron spectroscopy. The effective interfacial contact between Cu<sub>2</sub>O and ZnFe<sub>2</sub>O<sub>4</sub> nanoparticles forms a type II heterojunction, which makes the effective separation of photogenerated charges, facilitates the reduction of protons to H<sub>2</sub>, and achieves efficient hydrogen production. This work presents a strategy for simple design and fabrication of highly efficient composite photocatalysts.</p><h3>Graphical Abstract</h3>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142254156","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Catalysis LettersPub Date : 2024-09-14DOI: 10.1007/s10562-024-04821-9
Shan Zhu, Yue Zhao, Fengxiang Ma, Feng Zhu, Wei Liu, Jun Cao, Yumei Song, Jinyu Ding, Peijin Du
{"title":"SF6 Photoconversion Triggered by Oxygen-Deficient ZnO Atomic Layers Under Mild Conditions","authors":"Shan Zhu, Yue Zhao, Fengxiang Ma, Feng Zhu, Wei Liu, Jun Cao, Yumei Song, Jinyu Ding, Peijin Du","doi":"10.1007/s10562-024-04821-9","DOIUrl":"10.1007/s10562-024-04821-9","url":null,"abstract":"<div><p>The majority of reaction conditions employed in SF<sub>6</sub> conversion research are characterized by elevated temperatures and pressures, resulting in a considerable expenditure of energy. The transformation of SF<sub>6</sub> under mild conditions represents a viable methodology at this time. It has been demonstrated that the conditions required for the photoconversion of SF<sub>6</sub> are relatively mild. Furthermore, the defect engineering of catalysts has been shown to be an effective strategy for enhancing the photocatalytic performance of photocatalysis. Thus, we utilized two-dimensional materials as a model for our research. These materials have active sites that are highly dense and uniform, allowing us to thoroughly examine how defects affect the SF<sub>6</sub> photoconversion process. By synthesizing ZnO atomic layers with oxygen vacancies and confirming their presence using various techniques, we found that these vacancies enhanced light absorption and promoted the separation of charge carriers. These results suggest that the oxygen-deficient ZnO atomic layers have superior SF<sub>6</sub> photoconversion performance compared to the pristine ZnO atomic layers. Overall, the findings of this study indicate that the incorporation of defects in photocatalysts is a crucial strategy for optimizing pivotal photocatalytic processes and enhancing the efficacy of SF<sub>6</sub> photoconversion.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div><p>We initially built clear models of two-dimensional atomic layers with defect concentrations, and hence directly disclose the defect type and distribution at atomic level. As a prototype, defective ZnO nanosheets with atomic thickness are successfully synthesized. Also, we use defective ZnO atomic layers to achieve light conversion of SF<sub>6</sub> under mild conditions, which provides a new path to solve the environmental pollution of perfluorinated compounds.</p></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142254154","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Catalysis LettersPub Date : 2024-09-14DOI: 10.1007/s10562-024-04804-w
Siwen Zhang, Haiming Gu, Shanhui Zhao
{"title":"Catalytic Decomposition of Toluene over Fe2O3 Nanocluster During Chemical Looping Gasification (CLG): ReaxFF MD Approach","authors":"Siwen Zhang, Haiming Gu, Shanhui Zhao","doi":"10.1007/s10562-024-04804-w","DOIUrl":"10.1007/s10562-024-04804-w","url":null,"abstract":"<div><p>Chemical looping gasification (CLG) is an effective technology for efficient utilization of coal, biomass and other fuels. In this work, the detailed mechanism of catalytic decomposition during CLG for toluene, a tar model compound, was studied by using reactive force field molecular dynamics (ReaxFF MD) method. Results show that toluene hardly decomposes at temperature lower than 2000 K. Improving temperature could significantly improve decomposition efficiency but also enhances the polymerization to produce PAHs and soot precursor, with largest molecule weight of 2175 (C<sub>177</sub>H<sub>51</sub>, 3000 K, 400 ps). Fe<sub>2</sub>O<sub>3</sub> nanocluster, as oxygen carrier, could improve the decomposition efficiency of toluene and reduce the decomposition temperature. At 2000 K and 200 ps, the catalytic conversion of toluene reaches 60%. A large amount of H<sub>2</sub>, CO, C<sub>2</sub>H<sub>2</sub> and other small molecular gases are generated during the catalytic decomposition of toluene. At 3000 K, the yield of H<sub>2</sub>, CO and C<sub>2</sub>H<sub>2</sub> reached 132 %mole, 117 %mole and 40 %mole of toluene, respectively. Meanwhile, polymerization reactions are largely inhibited by Fe<sub>2</sub>O<sub>3</sub> nanocluster and the largest molecule is C<sub>20</sub>H<sub>9</sub>O, the weight of which is much lower than soot precursor in thermal decomposition. Kinetic results show that the activated energy of catalytic decomposition is about 74 kJ/mole, which is much lower than thermal decomposition (382 kJ/mole). Detailed reaction mechanism reveals that lattice oxygen on Fe<sub>2</sub>O<sub>3</sub> nanocluster act as the active sites, which enhance the decomposition of toluene.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142269078","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Catalysis LettersPub Date : 2024-09-13DOI: 10.1007/s10562-024-04822-8
Xiansong Xia, Liangqi Li, Lin Chen, Qi Yao, Miao Liu, Hai Lan
{"title":"WVOx Supported on Industrial Al2O3, SiO2, AC, TiO2–Al2O3 for Catalytic Dehydration of Gas-Glycerol to Acrolein","authors":"Xiansong Xia, Liangqi Li, Lin Chen, Qi Yao, Miao Liu, Hai Lan","doi":"10.1007/s10562-024-04822-8","DOIUrl":"10.1007/s10562-024-04822-8","url":null,"abstract":"<div><p>WVO<sub>x</sub> bi-metal oxides supported on the cost-effective industrial mesoprous Al<sub>2</sub>O<sub>3</sub>, SiO<sub>2</sub>, active carbon (AC), and TiO<sub>2</sub>–Al<sub>2</sub>O<sub>3</sub> with different specific surface areas (WVO/Al<sub>2</sub>O<sub>3</sub>, WVO/SiO<sub>2</sub>, WVO/AC, and WVO/TiO<sub>2</sub>–Al<sub>2</sub>O<sub>3</sub>) were designed and prepared through co-impregnation method for large-scale bio-glycerol dehydration to acrolein. The XRD, BET, SEM–EDS, XPS, and NH<sub>3</sub>-TPD characterization results revealed the WO<sub>3</sub>–VO<sub>x</sub> (V<sup>4+</sup>/V<sup>5+</sup>) species existed with better dispersion, lower molar ratio of V<sup>4+</sup>/V<sup>5+</sup>, and enhanced strength of surface acid sites on the developed mesoporous TiO<sub>2</sub>–Al<sub>2</sub>O<sub>3</sub> in comparison with that on the mesoporous Al<sub>2</sub>O<sub>3</sub>, SiO<sub>2</sub>, and AC, demonstrating strong interaction of WO<sub>3</sub>–VO<sub>x</sub> species with the TiO<sub>2</sub>–Al<sub>2</sub>O<sub>3</sub> support and accounting for the acrolein selectivity over catalysts following the order of WVO/TiO<sub>2</sub>–Al<sub>2</sub>O<sub>3</sub> (75.8%) > WVO/AC (71.2%) > WVO/SiO<sub>2</sub> (55.3%) > WVO/Al<sub>2</sub>O<sub>3</sub> (42.8%). Over the WVO/TiO<sub>2</sub>–Al<sub>2</sub>O<sub>3</sub>, gas-glycerol conversion reached above 97.0% with acrolein selectivity of about 75.0% under the gas hourly space velocity (GHSV) of 120–360 h<sup>−1</sup>, and maintained an improved catalytic stability.</p><h3>Graphical Abstract</h3><p>The acrolein selectivity over the prepared catalysts followed the order of WVO/TiO<sub>2</sub>–Al<sub>2</sub>O<sub>3</sub> > WVO/AC > WVO/SiO<sub>2</sub> > WVO/Al<sub>2</sub>O<sub>3</sub>, Among them, the WVO/TiO<sub>2</sub>–Al<sub>2</sub>O<sub>3</sub> catalyst demonstrated a low V<sup>4+</sup>/V<sup>5+</sup> ratio, surface acid sites, and exceptional catalytic performance with a gas-glycerol conversion rate of 97.2% and an acrolein selectivity of 75.8%. Even after continuous reaction for 16 h, both gas-glycerol conversion and acrolein selectivity remained above 75% and 90%, respectively. This study presents a remarkable advancement in the development of industrial catalysts with outstanding performance in terms of efficiency, stability, and cost-effectiveness. Moreover, this catalyst shows great promise for its utilization in acrolein synthesis via glycerol dehydration.</p>\u0000<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142175669","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}