文献类型：期刊文献

英文题名：Synergistic enhancement of catalytic hydrodeoxygenation performance by oxygen vacancies and frustrated Lewis pairs

作者：Sun, Qing-Qing[1,2];Liu, Cong[2];Zhang, Guo-Qiang[2];Liu, Zhong-Qiu[1,2];Wang, Mei-Ying[2];Wang, Ai-Min[1,3];Liu, Yujing[2];Shen, Runpu[4];Ying, Anguo[2]

机构：[1]Yulin Univ, Sch Chem & Chem Engn, Yulin Key Lab Low Carbon Refining Utilizat Heavy C, Shaanxi Key Lab Low Metamorph Coal Clean Utilizat, Yulin 719000, Peoples R China;[2]Qufu Normal Univ, Sch Chem & Chem Engn, Key Lab Catalyt Convers & Clean Energy Univ Shando, Qufu 273165, Shandong, Peoples R China;[3]China Univ Min & Technol, Key Lab Coal Proc & Efficient Utilizat, Minist Educ, Xuzhou 221116, Jiangsu, Peoples R China;[4]Shaoxing Univ, Zhejiang Engn Res Ctr Fat Soluble Vitamin, Shaoxing 312000, Zhejiang, Peoples R China

年份：2025

卷号：382

外文期刊名：FUEL

收录：SCI-EXPANDED(收录号：WOS:001359902000001)、、EI(收录号：20244717379046)、Scopus(收录号：2-s2.0-85208953885)、WOS

基金：This work was supported by the National Natural Science Foundation of China (Grant Nos. 22108156; 22468051; 22278243; 42306235; 21978154), Youth Innovation Team Project of Shandong Provincial College (Grant No. 2022KJ180), Shandong Provincial Natural Science Foundation (Grant Nos. ZR2024MB020; ZR2024MB042; ZR2024MD122), Zhejiang Engineering Research Center of Fat-soluble Vitamin (Grant No. 202105), Technology Innovation Team of Shaanxi Province (Grant No. 2023-CX-TD-39), Scientific Research Project of Education Department of Shaanxi Provincial Government (Grant No. 22JC064), and Chinese Academy of Science Clean Energy Innovation Institute-Yulin University Joint Fund (Grant No. YLU-DNL Fund 2023001).

语种：英文

外文关键词：Ionic liquids; Capping effect; Frustrated Lewis pairs; Oxygen vacancies; Saturated cycloalkanes

外文摘要：The catalytic hydrodeoxygenation (CHDO) of lignin into saturated cycloalkanes not only enhances the efficient utilization of lignin but also reduces reliance on high-density liquid fuels (HDLFs), given the importance of saturated cycloalkanes as key constituents of HDLFs. The main challenge in lignin CHDO towards HDLFs is efficiently removing oxygen-atom while maintaining high selectivity for the desired saturated cycloalkanes. Herein, we report for the first time the fabrication of a Ni/N0.8-CeO2-500 composite with abundant oxygen vacancies (OVs) and adjacent frustrated Lewis pairs (FLPs), achieved through the capping effect of ionic liquids. The FLPs of N/Ce3+ within Ni/N0.8-CeO2-500, mediated by OVs, not only enhance the dispersion of Ni species but also effectively facilitate the conversion of H2 into active hydrogen (H*) through relay catalysis involving the Ni species. This integration, combining the oxygen atom-specific recognition of OVs with the adjacent FLPs of N/ Ce3+ for the tandem generation of H*, significantly promotes the adsorption/cleavage of C ar/alk-O-C alk bonds, oxygen-atom removal, and hydrogenation of aromatic rings, ultimately catalyzing the one-step production of saturated cycloalkanes. The synergistic catalytic interplay results in a remarkable yield of saturated cycloalkanes (up to 88.2 wt%) during the CHDO of Kraft lignin, representing the highest reported value under similar conditions to date. A combination of diverse characterizations, experimental analyses, and kinetic studies collectively reinforces the notion that in-situ N-doping of CeO2 increases the electron cloud density around Ce species, forming N-Ce delta+ entities that, at high temperatures, create OVs and adjacent FLPs of N-Ce3+, collectively enhancing lignin CHDO to yield saturated cycloalkanes.