{"title":"HDPE热解挥发物在Ni催化剂上的氧化蒸汽重整:载体(Al2O3、ZrO2、SiO2)和促进剂(CeO2、La2O3)对催化剂性能的影响","authors":"Mayra Alejandra Suarez , Laura Santamaria , Gartzen Lopez , Enara Fernandez , Martin Olazar , Maider Amutio , Maite Artetxe","doi":"10.1016/S1872-2067(24)60222-6","DOIUrl":null,"url":null,"abstract":"<div><div>High density polyethylene (HDPE) pyrolysis and in-line oxidative steam reforming was carried out in a two-step reaction system consisting of a conical spouted bed reactor and a fluidized bed reactor. Continuous plastic pyrolysis was conducted at 550 °C and the volatiles formed were fed in-line to the oxidative steam reforming step (space-time 3.12 g<sub>cat</sub> min g<sub>HDPE</sub><sup>−1</sup>; ER = 0.2 and steam/plastic = 3) operating at 700 °C. The influence Ni based reforming catalyst support (Al<sub>2</sub>O<sub>3</sub>, ZrO<sub>2</sub>, SiO<sub>2</sub>) and promoter (CeO<sub>2</sub>, La<sub>2</sub>O<sub>3</sub>) have on HDPE pyrolysis volatiles conversion and H<sub>2</sub> production was assessed. The catalysts were prepared by the wet impregnation and they were characterized by means of N<sub>2</sub> adsorption-desorption, X-ray fluorescence, temperature-programmed reduction and X-ray powder diffraction. A preliminary study on coke deposition and the deterioration of catalysts properties was carried out, by analyzing the tested catalysts through temperature programmed oxidation of coke, transmission electron microscopy, and N<sub>2</sub> adsorption-desorption. Among the supports tested, ZrO<sub>2</sub> showed the best performance, attaining conversion and H<sub>2</sub> production values of 92.2% and 12.8 wt%, respectively. Concerning promoted catalysts, they led to similar conversion values (around 90%), but significant differences were observed in H<sub>2</sub> production. Thus, higher H<sub>2</sub> productions were obtained on the Ni/La<sub>2</sub>O<sub>3</sub>-Al<sub>2</sub>O<sub>3</sub> catalyst (12.1 wt%) than on CeO<sub>2</sub> promoted catalysts due to La<sub>2</sub>O<sub>3</sub> capability for enhancing water adsorption on the catalyst surface.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"69 ","pages":"Pages 149-162"},"PeriodicalIF":17.2000,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Oxidative steam reforming of HDPE pyrolysis volatiles on Ni catalysts: Effect of the support (Al2O3, ZrO2, SiO2) and promoter (CeO2, La2O3) on the catalyst performance\",\"authors\":\"Mayra Alejandra Suarez , Laura Santamaria , Gartzen Lopez , Enara Fernandez , Martin Olazar , Maider Amutio , Maite Artetxe\",\"doi\":\"10.1016/S1872-2067(24)60222-6\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>High density polyethylene (HDPE) pyrolysis and in-line oxidative steam reforming was carried out in a two-step reaction system consisting of a conical spouted bed reactor and a fluidized bed reactor. Continuous plastic pyrolysis was conducted at 550 °C and the volatiles formed were fed in-line to the oxidative steam reforming step (space-time 3.12 g<sub>cat</sub> min g<sub>HDPE</sub><sup>−1</sup>; ER = 0.2 and steam/plastic = 3) operating at 700 °C. The influence Ni based reforming catalyst support (Al<sub>2</sub>O<sub>3</sub>, ZrO<sub>2</sub>, SiO<sub>2</sub>) and promoter (CeO<sub>2</sub>, La<sub>2</sub>O<sub>3</sub>) have on HDPE pyrolysis volatiles conversion and H<sub>2</sub> production was assessed. The catalysts were prepared by the wet impregnation and they were characterized by means of N<sub>2</sub> adsorption-desorption, X-ray fluorescence, temperature-programmed reduction and X-ray powder diffraction. A preliminary study on coke deposition and the deterioration of catalysts properties was carried out, by analyzing the tested catalysts through temperature programmed oxidation of coke, transmission electron microscopy, and N<sub>2</sub> adsorption-desorption. Among the supports tested, ZrO<sub>2</sub> showed the best performance, attaining conversion and H<sub>2</sub> production values of 92.2% and 12.8 wt%, respectively. Concerning promoted catalysts, they led to similar conversion values (around 90%), but significant differences were observed in H<sub>2</sub> production. Thus, higher H<sub>2</sub> productions were obtained on the Ni/La<sub>2</sub>O<sub>3</sub>-Al<sub>2</sub>O<sub>3</sub> catalyst (12.1 wt%) than on CeO<sub>2</sub> promoted catalysts due to La<sub>2</sub>O<sub>3</sub> capability for enhancing water adsorption on the catalyst surface.</div></div>\",\"PeriodicalId\":9832,\"journal\":{\"name\":\"Chinese Journal of Catalysis\",\"volume\":\"69 \",\"pages\":\"Pages 149-162\"},\"PeriodicalIF\":17.2000,\"publicationDate\":\"2025-02-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chinese Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1872206724602226\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2025/3/4 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chinese Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1872206724602226","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2025/3/4 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
引用次数: 0
摘要
在由锥形喷淋床反应器和流化床反应器组成的两步反应系统中对高密度聚乙烯(HDPE)进行了热解和在线氧化蒸汽重整。在550℃下连续进行塑料热解,形成的挥发物在线送入氧化蒸汽重整步骤(时空3.12 gcat min gHDPE−1;ER = 0.2,蒸汽/塑料= 3)在700°C下工作。考察了Ni基重整催化剂载体(Al2O3、ZrO2、SiO2)和促进剂(CeO2、La2O3)对HDPE热解挥发物转化和H2生成的影响。采用湿浸渍法制备了催化剂,并用N2吸附-解吸、x射线荧光、程序升温还原和x射线粉末衍射对催化剂进行了表征。通过程序升温氧化法、透射电镜法和N2吸附-脱附法对所测催化剂进行分析,对焦炭沉积和催化剂性能恶化进行了初步研究。其中,ZrO2表现最好,转化率为92.2%,产氢率为12.8%。对于促进催化剂,它们的转化率相似(约90%),但在H2产率方面存在显著差异。因此,在Ni/La2O3- al2o3催化剂上获得了比CeO2催化剂更高的H2产率(12.1%),这是由于La2O3增强了催化剂表面对水的吸附能力。
Oxidative steam reforming of HDPE pyrolysis volatiles on Ni catalysts: Effect of the support (Al2O3, ZrO2, SiO2) and promoter (CeO2, La2O3) on the catalyst performance
High density polyethylene (HDPE) pyrolysis and in-line oxidative steam reforming was carried out in a two-step reaction system consisting of a conical spouted bed reactor and a fluidized bed reactor. Continuous plastic pyrolysis was conducted at 550 °C and the volatiles formed were fed in-line to the oxidative steam reforming step (space-time 3.12 gcat min gHDPE−1; ER = 0.2 and steam/plastic = 3) operating at 700 °C. The influence Ni based reforming catalyst support (Al2O3, ZrO2, SiO2) and promoter (CeO2, La2O3) have on HDPE pyrolysis volatiles conversion and H2 production was assessed. The catalysts were prepared by the wet impregnation and they were characterized by means of N2 adsorption-desorption, X-ray fluorescence, temperature-programmed reduction and X-ray powder diffraction. A preliminary study on coke deposition and the deterioration of catalysts properties was carried out, by analyzing the tested catalysts through temperature programmed oxidation of coke, transmission electron microscopy, and N2 adsorption-desorption. Among the supports tested, ZrO2 showed the best performance, attaining conversion and H2 production values of 92.2% and 12.8 wt%, respectively. Concerning promoted catalysts, they led to similar conversion values (around 90%), but significant differences were observed in H2 production. Thus, higher H2 productions were obtained on the Ni/La2O3-Al2O3 catalyst (12.1 wt%) than on CeO2 promoted catalysts due to La2O3 capability for enhancing water adsorption on the catalyst surface.
期刊介绍:
The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.