{"title":"使用 InCeZrOX/H-ZSM-5-Si 双功能催化剂将二氧化碳转化为轻烯烃","authors":"Zheng Yuan, Xia Lv, Muhammad Irfan, Guofeng Zhao, Jichang Liu, Haitao Xu","doi":"10.1021/acs.iecr.4c01132","DOIUrl":null,"url":null,"abstract":"Carbon dioxide (CO<sub>2</sub>) conversion into light olefins (C<sub>2</sub><sup>=</sup>–C<sub>4</sub><sup>=</sup>) using green hydrogen is a desirable strategy to reduce CO<sub>2</sub> emissions and obtain valuable chemicals. Although ZSM-5-based bifunctional catalysts exhibit unique characteristics that render them suitable for various processes, they are rarely used for CO<sub>2</sub> conversion into C<sub>2</sub><sup>=</sup>–C<sub>4</sub><sup>=</sup>. Herein, an In<sub>0.9</sub>Ce<sub>1</sub>Zr<sub>4</sub>O<sub><i>X</i></sub>/H-ZSM-5-Si bifunctional catalyst composed of In<sub>0.9</sub>Ce<sub>1</sub>Zr<sub>4</sub>O<sub><i>X</i></sub> and tetraethyl orthosilicate (TEOS)-passivated H-ZSM-5-Si was prepared for CO<sub>2</sub> conversion into light olefins. CO<sub>2</sub> on In<sub>0.9</sub>Ce<sub>1</sub>Zr<sub>4</sub>O<sub><i>X</i></sub>/H-ZSM-5-Si exhibits a selectivity of 60.3% for C<sub>2</sub><sup>=</sup>–C<sub>4</sub><sup>=</sup>, 5.9% for CH<sub>4</sub>, and 17.2% for C<sub>5+</sub> in hydrocarbons. The CO selectivity in the total products is 63.6%. The doping of In and Ce increases the concentration of surface oxygen vacancies, thereby enhancing the adsorption of CO<sub>2</sub> and H<sub>2</sub>. The passivation of H-ZSM-5-Si by TEOS effectively reduces its acidity, promoting the generation of C<sub>2</sub><sup>=</sup>–C<sub>4</sub><sup>=</sup>.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":null,"pages":null},"PeriodicalIF":3.8000,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"CO2 Conversion into Light Olefins Using an InCeZrOX/H-ZSM-5-Si Bifunctional Catalyst\",\"authors\":\"Zheng Yuan, Xia Lv, Muhammad Irfan, Guofeng Zhao, Jichang Liu, Haitao Xu\",\"doi\":\"10.1021/acs.iecr.4c01132\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Carbon dioxide (CO<sub>2</sub>) conversion into light olefins (C<sub>2</sub><sup>=</sup>–C<sub>4</sub><sup>=</sup>) using green hydrogen is a desirable strategy to reduce CO<sub>2</sub> emissions and obtain valuable chemicals. Although ZSM-5-based bifunctional catalysts exhibit unique characteristics that render them suitable for various processes, they are rarely used for CO<sub>2</sub> conversion into C<sub>2</sub><sup>=</sup>–C<sub>4</sub><sup>=</sup>. Herein, an In<sub>0.9</sub>Ce<sub>1</sub>Zr<sub>4</sub>O<sub><i>X</i></sub>/H-ZSM-5-Si bifunctional catalyst composed of In<sub>0.9</sub>Ce<sub>1</sub>Zr<sub>4</sub>O<sub><i>X</i></sub> and tetraethyl orthosilicate (TEOS)-passivated H-ZSM-5-Si was prepared for CO<sub>2</sub> conversion into light olefins. CO<sub>2</sub> on In<sub>0.9</sub>Ce<sub>1</sub>Zr<sub>4</sub>O<sub><i>X</i></sub>/H-ZSM-5-Si exhibits a selectivity of 60.3% for C<sub>2</sub><sup>=</sup>–C<sub>4</sub><sup>=</sup>, 5.9% for CH<sub>4</sub>, and 17.2% for C<sub>5+</sub> in hydrocarbons. The CO selectivity in the total products is 63.6%. The doping of In and Ce increases the concentration of surface oxygen vacancies, thereby enhancing the adsorption of CO<sub>2</sub> and H<sub>2</sub>. The passivation of H-ZSM-5-Si by TEOS effectively reduces its acidity, promoting the generation of C<sub>2</sub><sup>=</sup>–C<sub>4</sub><sup>=</sup>.\",\"PeriodicalId\":39,\"journal\":{\"name\":\"Industrial & Engineering Chemistry Research\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":3.8000,\"publicationDate\":\"2024-07-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Industrial & Engineering Chemistry Research\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.iecr.4c01132\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Industrial & Engineering Chemistry Research","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1021/acs.iecr.4c01132","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
摘要
利用绿色氢气将二氧化碳(CO2)转化为轻烯烃(C2=-C4=)是减少二氧化碳排放和获得有价值化学品的理想策略。虽然基于 ZSM-5 的双功能催化剂具有独特的特性,使其适用于各种工艺,但很少用于将 CO2 转化为 C2=-C4=。 本文制备了一种 In0.9Ce1Zr4OX/H-ZSM-5-Si 双功能催化剂,该催化剂由 In0.9Ce1Zr4OX 和正硅酸四乙酯(TEOS)钝化的 H-ZSM-5-Si 组成,用于将 CO2 转化为轻质烯烃。In0.9Ce1Zr4OX/H-ZSM-5-Si 上的 CO2 对碳氢化合物中 C2=-C4= 的选择性为 60.3%,对 CH4 的选择性为 5.9%,对 C5+ 的选择性为 17.2%。总产物中 CO 的选择性为 63.6%。In 和 Ce 的掺杂增加了表面氧空位的浓度,从而增强了对 CO2 和 H2 的吸附。TEOS 对 H-ZSM-5-Si 的钝化可有效降低其酸度,促进 C2=-C4= 的生成。
CO2 Conversion into Light Olefins Using an InCeZrOX/H-ZSM-5-Si Bifunctional Catalyst
Carbon dioxide (CO2) conversion into light olefins (C2=–C4=) using green hydrogen is a desirable strategy to reduce CO2 emissions and obtain valuable chemicals. Although ZSM-5-based bifunctional catalysts exhibit unique characteristics that render them suitable for various processes, they are rarely used for CO2 conversion into C2=–C4=. Herein, an In0.9Ce1Zr4OX/H-ZSM-5-Si bifunctional catalyst composed of In0.9Ce1Zr4OX and tetraethyl orthosilicate (TEOS)-passivated H-ZSM-5-Si was prepared for CO2 conversion into light olefins. CO2 on In0.9Ce1Zr4OX/H-ZSM-5-Si exhibits a selectivity of 60.3% for C2=–C4=, 5.9% for CH4, and 17.2% for C5+ in hydrocarbons. The CO selectivity in the total products is 63.6%. The doping of In and Ce increases the concentration of surface oxygen vacancies, thereby enhancing the adsorption of CO2 and H2. The passivation of H-ZSM-5-Si by TEOS effectively reduces its acidity, promoting the generation of C2=–C4=.
期刊介绍:
ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.