{"title":"同步构建具有双缺陷的 Ni/CeO2/C 作为无氢条件下催化精制木质素油的双引擎","authors":"Yingbo Zhu, Yulong Ma, Yonggang Sun, Wenxin Ji, Liqiong Wang, Feng Lin, Yuanyuan Li, Hongqiang Xia","doi":"10.1021/acscatal.4c03228","DOIUrl":null,"url":null,"abstract":"The ambiguous structural defect types and sites of catalysts impede the investigation of structure–activity relationships at the atomic scale for catalytic transfer of hydrodeoxygenation of lignin and its derivatives. In this work, oxygen vacancies (O<sub>v</sub>) and carbon defects (C<sub>d</sub>) in Ni/CeO<sub>2</sub>/C catalysts were constructed by an in situ calcination atmosphere-induced engraving strategy. The dual defect embodied the chemical characteristics of heterogeneous frustrated Lewis pairs, and the synergy between O<sub>v</sub> and C<sub>d</sub> could effectively promote the adsorption and activation of isopropanol and the oxygen-containing substrate, which stimulated the production of more reactive H<sup>δ+</sup> and H<sup>δ−</sup>, anchored the methyl group. Efficient conversion of lignin oil was achieved without initial H<sub>2</sub> pressure, yielding 56% liquid product and 62.9% C<sub>6+</sub> cycloalkanol selectivity. The traditional hydrodeoxygenation was transformed into a solid–liquid two-phase catalytic transfer hydrodeoxygenation, which enhanced the mass transfer. This study developed a catalytic system for catalytic transfer hydrodeoxygenation and offered insights for the preparation of heterogeneous frustrated Lewis pairs.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":null,"pages":null},"PeriodicalIF":11.3000,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Synchronous Construction of Ni/CeO2/C with Double Defects as a Dual Engine for Catalytic Refinement of Lignin Oil Under Hydrogen-Free Condition\",\"authors\":\"Yingbo Zhu, Yulong Ma, Yonggang Sun, Wenxin Ji, Liqiong Wang, Feng Lin, Yuanyuan Li, Hongqiang Xia\",\"doi\":\"10.1021/acscatal.4c03228\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The ambiguous structural defect types and sites of catalysts impede the investigation of structure–activity relationships at the atomic scale for catalytic transfer of hydrodeoxygenation of lignin and its derivatives. In this work, oxygen vacancies (O<sub>v</sub>) and carbon defects (C<sub>d</sub>) in Ni/CeO<sub>2</sub>/C catalysts were constructed by an in situ calcination atmosphere-induced engraving strategy. The dual defect embodied the chemical characteristics of heterogeneous frustrated Lewis pairs, and the synergy between O<sub>v</sub> and C<sub>d</sub> could effectively promote the adsorption and activation of isopropanol and the oxygen-containing substrate, which stimulated the production of more reactive H<sup>δ+</sup> and H<sup>δ−</sup>, anchored the methyl group. Efficient conversion of lignin oil was achieved without initial H<sub>2</sub> pressure, yielding 56% liquid product and 62.9% C<sub>6+</sub> cycloalkanol selectivity. The traditional hydrodeoxygenation was transformed into a solid–liquid two-phase catalytic transfer hydrodeoxygenation, which enhanced the mass transfer. This study developed a catalytic system for catalytic transfer hydrodeoxygenation and offered insights for the preparation of heterogeneous frustrated Lewis pairs.\",\"PeriodicalId\":9,\"journal\":{\"name\":\"ACS Catalysis \",\"volume\":null,\"pages\":null},\"PeriodicalIF\":11.3000,\"publicationDate\":\"2024-11-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Catalysis \",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acscatal.4c03228\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Catalysis ","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acscatal.4c03228","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Synchronous Construction of Ni/CeO2/C with Double Defects as a Dual Engine for Catalytic Refinement of Lignin Oil Under Hydrogen-Free Condition
The ambiguous structural defect types and sites of catalysts impede the investigation of structure–activity relationships at the atomic scale for catalytic transfer of hydrodeoxygenation of lignin and its derivatives. In this work, oxygen vacancies (Ov) and carbon defects (Cd) in Ni/CeO2/C catalysts were constructed by an in situ calcination atmosphere-induced engraving strategy. The dual defect embodied the chemical characteristics of heterogeneous frustrated Lewis pairs, and the synergy between Ov and Cd could effectively promote the adsorption and activation of isopropanol and the oxygen-containing substrate, which stimulated the production of more reactive Hδ+ and Hδ−, anchored the methyl group. Efficient conversion of lignin oil was achieved without initial H2 pressure, yielding 56% liquid product and 62.9% C6+ cycloalkanol selectivity. The traditional hydrodeoxygenation was transformed into a solid–liquid two-phase catalytic transfer hydrodeoxygenation, which enhanced the mass transfer. This study developed a catalytic system for catalytic transfer hydrodeoxygenation and offered insights for the preparation of heterogeneous frustrated Lewis pairs.
期刊介绍:
ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels.
The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.