{"title":"金-钙钛矿催化剂在一氧化碳氧化中的催化活性","authors":"Leboheng Mokoena, Gary Pattrick, Mike S Scurrell","doi":"10.1007/s13404-016-0180-x","DOIUrl":null,"url":null,"abstract":"<p>Perovskites (ABO<sub>3</sub> structures), which can be manipulated by partial substitution, are reported to be active supports for CO oxidation, but only at high temperatures, with no activity being shown for temperatures below 200?°C. In this study, these perovskites were investigated at low temperatures (below 100?°C) with improved activity found upon gold deposition. The presence of gold nanoparticles therefore significantly enhanced the catalytic activity, while the support itself was suspected to be involved in the reaction mechanism. A series of perovskites of the type ABO<sub>3</sub> (LaMnO<sub>3</sub>, LaFeO<sub>3</sub>, LaCoO<sub>3</sub>, and LaCuO<sub>3</sub>) were prepared using the citrate method, while the gold was deposited on them using the deposition-precipitation method. The supports were calcined at different temperatures for optimization. With the support calcined at 800?°C, the best catalyst was 1?wt% Au supported on LaFeO<sub>3</sub>. Calcium-doping of this system showed decreased surface area, poorer crystallinity, and a drop in catalytic activity relative to the Au-LaFeO<sub>3</sub>. In addition, Au-LaFeO<sub>3</sub> showed online stability over 21?h. Calcining the support improved the incorporation of gold nanoparticles into the perovskite lattice, resulting in superior catalytic activity. Nevertheless, at higher calcination temperatures, the catalytic activity of Au-CaTiO<sub>3</sub> was depressed while that of Au-LaFeO3 was enhanced. XPS revealed that in the active catalysts, both cationic and metallic gold coexisted, while in the inactive catalysts, the gold existed predominantly either as cationic or metallic gold.</p>","PeriodicalId":55086,"journal":{"name":"Gold Bulletin","volume":null,"pages":null},"PeriodicalIF":2.2000,"publicationDate":"2016-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://sci-hub-pdf.com/10.1007/s13404-016-0180-x","citationCount":"7","resultStr":"{\"title\":\"Catalytic activity of gold-perovskite catalysts in the oxidation of carbon monoxide\",\"authors\":\"Leboheng Mokoena, Gary Pattrick, Mike S Scurrell\",\"doi\":\"10.1007/s13404-016-0180-x\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Perovskites (ABO<sub>3</sub> structures), which can be manipulated by partial substitution, are reported to be active supports for CO oxidation, but only at high temperatures, with no activity being shown for temperatures below 200?°C. In this study, these perovskites were investigated at low temperatures (below 100?°C) with improved activity found upon gold deposition. The presence of gold nanoparticles therefore significantly enhanced the catalytic activity, while the support itself was suspected to be involved in the reaction mechanism. A series of perovskites of the type ABO<sub>3</sub> (LaMnO<sub>3</sub>, LaFeO<sub>3</sub>, LaCoO<sub>3</sub>, and LaCuO<sub>3</sub>) were prepared using the citrate method, while the gold was deposited on them using the deposition-precipitation method. The supports were calcined at different temperatures for optimization. With the support calcined at 800?°C, the best catalyst was 1?wt% Au supported on LaFeO<sub>3</sub>. Calcium-doping of this system showed decreased surface area, poorer crystallinity, and a drop in catalytic activity relative to the Au-LaFeO<sub>3</sub>. In addition, Au-LaFeO<sub>3</sub> showed online stability over 21?h. Calcining the support improved the incorporation of gold nanoparticles into the perovskite lattice, resulting in superior catalytic activity. Nevertheless, at higher calcination temperatures, the catalytic activity of Au-CaTiO<sub>3</sub> was depressed while that of Au-LaFeO3 was enhanced. XPS revealed that in the active catalysts, both cationic and metallic gold coexisted, while in the inactive catalysts, the gold existed predominantly either as cationic or metallic gold.</p>\",\"PeriodicalId\":55086,\"journal\":{\"name\":\"Gold Bulletin\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":2.2000,\"publicationDate\":\"2016-07-06\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://sci-hub-pdf.com/10.1007/s13404-016-0180-x\",\"citationCount\":\"7\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Gold Bulletin\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s13404-016-0180-x\",\"RegionNum\":4,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"Chemistry\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Gold Bulletin","FirstCategoryId":"5","ListUrlMain":"https://link.springer.com/article/10.1007/s13404-016-0180-x","RegionNum":4,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"Chemistry","Score":null,"Total":0}
Catalytic activity of gold-perovskite catalysts in the oxidation of carbon monoxide
Perovskites (ABO3 structures), which can be manipulated by partial substitution, are reported to be active supports for CO oxidation, but only at high temperatures, with no activity being shown for temperatures below 200?°C. In this study, these perovskites were investigated at low temperatures (below 100?°C) with improved activity found upon gold deposition. The presence of gold nanoparticles therefore significantly enhanced the catalytic activity, while the support itself was suspected to be involved in the reaction mechanism. A series of perovskites of the type ABO3 (LaMnO3, LaFeO3, LaCoO3, and LaCuO3) were prepared using the citrate method, while the gold was deposited on them using the deposition-precipitation method. The supports were calcined at different temperatures for optimization. With the support calcined at 800?°C, the best catalyst was 1?wt% Au supported on LaFeO3. Calcium-doping of this system showed decreased surface area, poorer crystallinity, and a drop in catalytic activity relative to the Au-LaFeO3. In addition, Au-LaFeO3 showed online stability over 21?h. Calcining the support improved the incorporation of gold nanoparticles into the perovskite lattice, resulting in superior catalytic activity. Nevertheless, at higher calcination temperatures, the catalytic activity of Au-CaTiO3 was depressed while that of Au-LaFeO3 was enhanced. XPS revealed that in the active catalysts, both cationic and metallic gold coexisted, while in the inactive catalysts, the gold existed predominantly either as cationic or metallic gold.
期刊介绍:
Gold Bulletin is the premier international peer reviewed journal on the latest science, technology and applications of gold. It includes papers on the latest research advances, state-of-the-art reviews, conference reports, book reviews and highlights of patents and scientific literature. Gold Bulletin does not publish manuscripts covering the snthesis of Gold nanoparticles in the presence of plant extracts or other nature-derived extracts. Gold Bulletin has been published over 40 years as a multidisciplinary journal read by chemists, physicists, engineers, metallurgists, materials scientists, biotechnologists, surface scientists, and nanotechnologists amongst others, both within industry and academia. Gold Bulletin is published in Association with the World Gold Council.