Xiansong Xia, Liangqi Li, Lin Chen, Qi Yao, Miao Liu, Hai Lan
{"title":"以工业 Al2O3、SiO2、AC、TiO2-Al2O3 为支撑的 WVOx 催化气体-甘油脱水生成丙烯醛","authors":"Xiansong Xia, Liangqi Li, Lin Chen, Qi Yao, Miao Liu, Hai Lan","doi":"10.1007/s10562-024-04822-8","DOIUrl":null,"url":null,"abstract":"<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 data-test=\"abstract-sub-heading\">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>\n","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":null,"pages":null},"PeriodicalIF":2.3000,"publicationDate":"2024-09-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"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\":null,\"url\":null,\"abstract\":\"<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 data-test=\\\"abstract-sub-heading\\\">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>\\n\",\"PeriodicalId\":508,\"journal\":{\"name\":\"Catalysis Letters\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":2.3000,\"publicationDate\":\"2024-09-13\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Letters\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1007/s10562-024-04822-8\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Letters","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1007/s10562-024-04822-8","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
WVOx Supported on Industrial Al2O3, SiO2, AC, TiO2–Al2O3 for Catalytic Dehydration of Gas-Glycerol to Acrolein
WVOx bi-metal oxides supported on the cost-effective industrial mesoprous Al2O3, SiO2, active carbon (AC), and TiO2–Al2O3 with different specific surface areas (WVO/Al2O3, WVO/SiO2, WVO/AC, and WVO/TiO2–Al2O3) were designed and prepared through co-impregnation method for large-scale bio-glycerol dehydration to acrolein. The XRD, BET, SEM–EDS, XPS, and NH3-TPD characterization results revealed the WO3–VOx (V4+/V5+) species existed with better dispersion, lower molar ratio of V4+/V5+, and enhanced strength of surface acid sites on the developed mesoporous TiO2–Al2O3 in comparison with that on the mesoporous Al2O3, SiO2, and AC, demonstrating strong interaction of WO3–VOx species with the TiO2–Al2O3 support and accounting for the acrolein selectivity over catalysts following the order of WVO/TiO2–Al2O3 (75.8%) > WVO/AC (71.2%) > WVO/SiO2 (55.3%) > WVO/Al2O3 (42.8%). Over the WVO/TiO2–Al2O3, 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−1, and maintained an improved catalytic stability.
Graphical Abstract
The acrolein selectivity over the prepared catalysts followed the order of WVO/TiO2–Al2O3 > WVO/AC > WVO/SiO2 > WVO/Al2O3, Among them, the WVO/TiO2–Al2O3 catalyst demonstrated a low V4+/V5+ 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.
期刊介绍：
Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis.
The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.
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