{"title":"不同Cu前驱体CuCeY的有效活性位点与超深度吸附脱硫性能的关系","authors":"Jingjing Wang , Lihong Li , Zhihui Wen , Jinchuan Zhao , Xinjie Wei , Junjie Liao , Liping Chang , Kechang Xie","doi":"10.1016/j.fuproc.2023.107930","DOIUrl":null,"url":null,"abstract":"<div><p><span>Adsorption desulfurization processes employing </span>zeolites<span> as sorbents are considered to be prospective desulfurization methods owing to their cost-effectiveness.</span></p><p><span><span>Y zeolites modified with Cu and Ce have excellent adsorption capacity and selectivity for adsorption desulfurization. However, the effect of using different </span>metal precursors on the active sites of these sorbents and their adsorption desulfurization performance still remains ambiguous, which impedes the development of improved desulfurization adsorbents. Herein, Cu(NO</span><sub>3</sub>)<sub>2</sub>, Cu(Ac)<sub>2</sub>, and CuSO<sub>4</sub><span> were selected as Cu precursors to prepare a series of CuCeY from CeY zeolite. Desulfurization experimental results indicate that outstanding breakthrough adsorption capacities for thiophene (ca. 6.25 mg·g</span><sup>−1</sup>) with benzene as the solvent were achieved by the CuCeY<sub>A</sub>. The interaction between the Cu<img>Ce metals was beneficial for enhancing the electron transfer between Cu<sup>2+</sup>+Ce<sup>3+</sup>/Ce<sup>4+</sup>+Cu<sup>+</sup>. Moreover, using different copper precursors significantly changed the redox ability of the adsorbent surface. Changing the copper precursor also had a significant effect on the locations of Cu and Ce ions, and using Cu(Ac)<sub>2</sub> as a metal precursor facilitated the migration of Cu<sup>+</sup><span><span> (53.6%) and cerium species (35.9%) to the supercage. In situ infrared characterization showed that the </span>oligomerization of thiophene on CuCeY</span><sub>A</sub> was significantly restricted due to the lowest B acid content (11.85%) in the CuCeY<sub>A</sub>.</p></div>","PeriodicalId":326,"journal":{"name":"Fuel Processing Technology","volume":null,"pages":null},"PeriodicalIF":7.2000,"publicationDate":"2023-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Insight into the relationship between effective active sites and ultra-deep adsorption desulfurization performance of CuCeY with different Cu precursors\",\"authors\":\"Jingjing Wang , Lihong Li , Zhihui Wen , Jinchuan Zhao , Xinjie Wei , Junjie Liao , Liping Chang , Kechang Xie\",\"doi\":\"10.1016/j.fuproc.2023.107930\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p><span>Adsorption desulfurization processes employing </span>zeolites<span> as sorbents are considered to be prospective desulfurization methods owing to their cost-effectiveness.</span></p><p><span><span>Y zeolites modified with Cu and Ce have excellent adsorption capacity and selectivity for adsorption desulfurization. However, the effect of using different </span>metal precursors on the active sites of these sorbents and their adsorption desulfurization performance still remains ambiguous, which impedes the development of improved desulfurization adsorbents. Herein, Cu(NO</span><sub>3</sub>)<sub>2</sub>, Cu(Ac)<sub>2</sub>, and CuSO<sub>4</sub><span> were selected as Cu precursors to prepare a series of CuCeY from CeY zeolite. Desulfurization experimental results indicate that outstanding breakthrough adsorption capacities for thiophene (ca. 6.25 mg·g</span><sup>−1</sup>) with benzene as the solvent were achieved by the CuCeY<sub>A</sub>. The interaction between the Cu<img>Ce metals was beneficial for enhancing the electron transfer between Cu<sup>2+</sup>+Ce<sup>3+</sup>/Ce<sup>4+</sup>+Cu<sup>+</sup>. Moreover, using different copper precursors significantly changed the redox ability of the adsorbent surface. Changing the copper precursor also had a significant effect on the locations of Cu and Ce ions, and using Cu(Ac)<sub>2</sub> as a metal precursor facilitated the migration of Cu<sup>+</sup><span><span> (53.6%) and cerium species (35.9%) to the supercage. In situ infrared characterization showed that the </span>oligomerization of thiophene on CuCeY</span><sub>A</sub> was significantly restricted due to the lowest B acid content (11.85%) in the CuCeY<sub>A</sub>.</p></div>\",\"PeriodicalId\":326,\"journal\":{\"name\":\"Fuel Processing Technology\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":7.2000,\"publicationDate\":\"2023-11-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Fuel Processing Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0378382023002783\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Fuel Processing Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0378382023002783","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
Insight into the relationship between effective active sites and ultra-deep adsorption desulfurization performance of CuCeY with different Cu precursors
Adsorption desulfurization processes employing zeolites as sorbents are considered to be prospective desulfurization methods owing to their cost-effectiveness.
Y zeolites modified with Cu and Ce have excellent adsorption capacity and selectivity for adsorption desulfurization. However, the effect of using different metal precursors on the active sites of these sorbents and their adsorption desulfurization performance still remains ambiguous, which impedes the development of improved desulfurization adsorbents. Herein, Cu(NO3)2, Cu(Ac)2, and CuSO4 were selected as Cu precursors to prepare a series of CuCeY from CeY zeolite. Desulfurization experimental results indicate that outstanding breakthrough adsorption capacities for thiophene (ca. 6.25 mg·g−1) with benzene as the solvent were achieved by the CuCeYA. The interaction between the CuCe metals was beneficial for enhancing the electron transfer between Cu2++Ce3+/Ce4++Cu+. Moreover, using different copper precursors significantly changed the redox ability of the adsorbent surface. Changing the copper precursor also had a significant effect on the locations of Cu and Ce ions, and using Cu(Ac)2 as a metal precursor facilitated the migration of Cu+ (53.6%) and cerium species (35.9%) to the supercage. In situ infrared characterization showed that the oligomerization of thiophene on CuCeYA was significantly restricted due to the lowest B acid content (11.85%) in the CuCeYA.
期刊介绍:
Fuel Processing Technology (FPT) deals with the scientific and technological aspects of converting fossil and renewable resources to clean fuels, value-added chemicals, fuel-related advanced carbon materials and by-products. In addition to the traditional non-nuclear fossil fuels, biomass and wastes, papers on the integration of renewables such as solar and wind energy and energy storage into the fuel processing processes, as well as papers on the production and conversion of non-carbon-containing fuels such as hydrogen and ammonia, are also welcome. While chemical conversion is emphasized, papers on advanced physical conversion processes are also considered for publication in FPT. Papers on the fundamental aspects of fuel structure and properties will also be considered.