Qingling Xu, Bin Shao, Zheyi Sun, Zihao Gao, Zhicheng Xie, Jun Hu
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A high CO<jats:sub>2</jats:sub> conversion efficiency of 27.4% and C<jats:sub>2</jats:sub>‐C<jats:sub>4</jats:sub><jats:sup>=</jats:sup> yield of 15.3% with excellent stability for 200 h are achieved on optimized CoO<jats:sub><jats:italic>x</jats:italic></jats:sub>/ZnGa<jats:sub>2</jats:sub>O<jats:sub>4</jats:sub>–2.5/SAPO‐34 through the oxide–zeolite (OX‐ZEO) bifunctional tandem route. The well‐controlled Co‐O‐Zn oxide–oxide interface in CoO<jats:sub><jats:italic>x</jats:italic></jats:sub>/ZnGa<jats:sub>2</jats:sub>O<jats:sub>4</jats:sub> facilitates the bidentate adsorption of CO<jats:sub>2</jats:sub>, enabling the exposed C atom to be attracted by spilled‐over H* from the heterolytic cleavage on adjacent Zn‐O. Accordingly, the preferentially produced HCOO* leads to effective CO<jats:sub>2</jats:sub> conversion and selective generation of methanol precursor. Therefore, this oxide–oxide interfacial engineering offers a promising strategy for achieving highly efficient CO<jats:sub>2</jats:sub>‐to‐C<jats:sub>2</jats:sub>‐C<jats:sub>4</jats:sub><jats:sup>=</jats:sup> through OX‐ZEO route.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"64 1","pages":""},"PeriodicalIF":4.0000,"publicationDate":"2025-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Co‐O‐Zn interface engineering for boosting CO2 hydrogenation to light olefins\",\"authors\":\"Qingling Xu, Bin Shao, Zheyi Sun, Zihao Gao, Zhicheng Xie, Jun Hu\",\"doi\":\"10.1002/aic.70106\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The carbon dioxide (CO<jats:sub>2</jats:sub>) hydrogenation to light olefins (CO<jats:sub>2</jats:sub>‐to‐C<jats:sub>2</jats:sub>‐C<jats:sub>4</jats:sub><jats:sup>=</jats:sup>) represents a promising approach for its high‐value utilization but faces the crucial challenges of low CO<jats:sub>2</jats:sub> conversion efficiency and olefin selectivity. Herein, we develop an oxide–oxide interface engineering strategy to boost CO<jats:sub>2</jats:sub>‐to‐C<jats:sub>2</jats:sub>‐C<jats:sub>4</jats:sub><jats:sup>=</jats:sup>. A high CO<jats:sub>2</jats:sub> conversion efficiency of 27.4% and C<jats:sub>2</jats:sub>‐C<jats:sub>4</jats:sub><jats:sup>=</jats:sup> yield of 15.3% with excellent stability for 200 h are achieved on optimized CoO<jats:sub><jats:italic>x</jats:italic></jats:sub>/ZnGa<jats:sub>2</jats:sub>O<jats:sub>4</jats:sub>–2.5/SAPO‐34 through the oxide–zeolite (OX‐ZEO) bifunctional tandem route. The well‐controlled Co‐O‐Zn oxide–oxide interface in CoO<jats:sub><jats:italic>x</jats:italic></jats:sub>/ZnGa<jats:sub>2</jats:sub>O<jats:sub>4</jats:sub> facilitates the bidentate adsorption of CO<jats:sub>2</jats:sub>, enabling the exposed C atom to be attracted by spilled‐over H* from the heterolytic cleavage on adjacent Zn‐O. 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引用次数: 0
摘要
二氧化碳(CO2)加氢制轻烯烃(CO2 - to - C2 - C4=)是一种有前途的高价值利用方法,但面临着低CO2转化效率和烯烃选择性的关键挑战。在此,我们开发了一种氧化物-氧化物界面工程策略来提高CO2 - to - C2 - C4=。优化后的CoOx/ ZnGa2O4-2.5 /SAPO - 34催化剂通过氧化物-沸石(OX - ZEO)双功能串联途径,CO2转化率为27.4%,C2 - C4=产率为15.3%,稳定性为200 h。CoOx/ZnGa2O4中的Co - O - Zn氧化物界面控制良好,有利于CO2的双齿吸附,使暴露的C原子被相邻Zn - O上的异裂解理溢出的H*所吸引。因此,优先生成的HCOO*导致了有效的CO2转化和甲醇前驱体的选择性生成。因此,这种氧化物-氧化物界面工程为通过OX - ZEO途径实现高效的CO2 - to - C2 - C4=提供了一种有前途的策略。
Co‐O‐Zn interface engineering for boosting CO2 hydrogenation to light olefins
The carbon dioxide (CO2) hydrogenation to light olefins (CO2‐to‐C2‐C4=) represents a promising approach for its high‐value utilization but faces the crucial challenges of low CO2 conversion efficiency and olefin selectivity. Herein, we develop an oxide–oxide interface engineering strategy to boost CO2‐to‐C2‐C4=. A high CO2 conversion efficiency of 27.4% and C2‐C4= yield of 15.3% with excellent stability for 200 h are achieved on optimized CoOx/ZnGa2O4–2.5/SAPO‐34 through the oxide–zeolite (OX‐ZEO) bifunctional tandem route. The well‐controlled Co‐O‐Zn oxide–oxide interface in CoOx/ZnGa2O4 facilitates the bidentate adsorption of CO2, enabling the exposed C atom to be attracted by spilled‐over H* from the heterolytic cleavage on adjacent Zn‐O. Accordingly, the preferentially produced HCOO* leads to effective CO2 conversion and selective generation of methanol precursor. Therefore, this oxide–oxide interfacial engineering offers a promising strategy for achieving highly efficient CO2‐to‐C2‐C4= through OX‐ZEO route.
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