V. I. Sobolev, A. N. Chernov, G. A. Zenkovets, A. V. Selivanova, E. Yu. Gerasimov, A. A. Shutilov, A. S. Gorbunova, V. V. Kaichev, K. Yu. Koltunov
{"title":"Catalytic Activity of Gallium Oxide in Propane Dehydrogenation: Effect of Support and Influence of Lanthanum Doping","authors":"V. I. Sobolev, A. N. Chernov, G. A. Zenkovets, A. V. Selivanova, E. Yu. Gerasimov, A. A. Shutilov, A. S. Gorbunova, V. V. Kaichev, K. Yu. Koltunov","doi":"10.1134/S0023158425600105","DOIUrl":null,"url":null,"abstract":"<p>Catalytic nonoxidative propane dehydrogenation (PDH) is the purposeful and most economical route to propylene production. The development of new PDH catalysts that can compete with existing commercial platinum and chromium catalysts is a major challenge for the progress of this technology. In the present study, GaO<sub><i>x</i></sub>-based catalysts (Ga<sub>2</sub>O<sub>3</sub> in bulk form or deposited on oxide supports such as SiO<sub>2</sub>, Al<sub>2</sub>O<sub>3</sub>, TiO<sub>2</sub>, and ZrO<sub>2</sub>) were prepared and their catalytic performance in the PDH was examined. It was shown that the activity of the catalysts depends on the support selected. The best results have been obtained with gallium oxide supported on alumina. The catalytic properties of this material were further improved by doping with lanthanum. PDH reaction catalyzed by La–Ga/Al<sub>2</sub>O<sub>3</sub> at 600°C at a gas hourly space velocity (GHSV) of 7500 mL h<sup>−1</sup> <span>\\({\\text{g}}_{{{\\text{cat}}}}^{{ - 1}}\\)</span> (propane/N<sub>2</sub> = 1/10) provided ca. 30% propane conversion with 95% propylene selectivity. The effect of the La-doping on the properties of bulk and supported Ga<sub>2</sub>O<sub>3</sub> were therefore studied by XRD, Raman and ATR-FTIR spectroscopies, HR-TEM, and low-temperature nitrogen adsorption techniques, which showed that La-doping contributes significantly to dispersion of gallium, diminishes crystallinity of the alumina support and increases the specific surface area of the catalyst.</p>","PeriodicalId":682,"journal":{"name":"Kinetics and Catalysis","volume":"66 3","pages":"286 - 296"},"PeriodicalIF":1.4000,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Kinetics and Catalysis","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1134/S0023158425600105","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q4","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Catalytic nonoxidative propane dehydrogenation (PDH) is the purposeful and most economical route to propylene production. The development of new PDH catalysts that can compete with existing commercial platinum and chromium catalysts is a major challenge for the progress of this technology. In the present study, GaOx-based catalysts (Ga2O3 in bulk form or deposited on oxide supports such as SiO2, Al2O3, TiO2, and ZrO2) were prepared and their catalytic performance in the PDH was examined. It was shown that the activity of the catalysts depends on the support selected. The best results have been obtained with gallium oxide supported on alumina. The catalytic properties of this material were further improved by doping with lanthanum. PDH reaction catalyzed by La–Ga/Al2O3 at 600°C at a gas hourly space velocity (GHSV) of 7500 mL h−1\({\text{g}}_{{{\text{cat}}}}^{{ - 1}}\) (propane/N2 = 1/10) provided ca. 30% propane conversion with 95% propylene selectivity. The effect of the La-doping on the properties of bulk and supported Ga2O3 were therefore studied by XRD, Raman and ATR-FTIR spectroscopies, HR-TEM, and low-temperature nitrogen adsorption techniques, which showed that La-doping contributes significantly to dispersion of gallium, diminishes crystallinity of the alumina support and increases the specific surface area of the catalyst.
催化非氧化丙烷脱氢(PDH)是生产丙烯的一种有目的和最经济的途径。开发新的PDH催化剂,以与现有的商业铂和铬催化剂竞争,是该技术进步的主要挑战。在本研究中,制备了基于gaox的催化剂(散装形式的Ga2O3或沉积在SiO2, Al2O3, TiO2和ZrO2等氧化物载体上),并测试了它们在PDH中的催化性能。结果表明,催化剂的活性取决于载体的选择。氧化铝负载氧化镓的效果最好。镧的掺入进一步提高了材料的催化性能。La-Ga /Al2O3在600℃下,气体小时空速(GHSV)为7500 mL h−1 \({\text{g}}_{{{\text{cat}}}}^{{ - 1}}\)(丙烷/N2 = 1/10)催化PDH反应% propane conversion with 95% propylene selectivity. The effect of the La-doping on the properties of bulk and supported Ga2O3 were therefore studied by XRD, Raman and ATR-FTIR spectroscopies, HR-TEM, and low-temperature nitrogen adsorption techniques, which showed that La-doping contributes significantly to dispersion of gallium, diminishes crystallinity of the alumina support and increases the specific surface area of the catalyst.
期刊介绍:
Kinetics and Catalysis Russian is a periodical that publishes theoretical and experimental works on homogeneous and heterogeneous kinetics and catalysis. Other topics include the mechanism and kinetics of noncatalytic processes in gaseous, liquid, and solid phases, quantum chemical calculations in kinetics and catalysis, methods of studying catalytic processes and catalysts, the chemistry of catalysts and adsorbent surfaces, the structure and physicochemical properties of catalysts, preparation and poisoning of catalysts, macrokinetics, and computer simulations in catalysis. The journal also publishes review articles on contemporary problems in kinetics and catalysis. The journal welcomes manuscripts from all countries in the English or Russian language.