Boosting bio-lipids deoxygenation via tunable metal-support interaction in nickel/ceria-based catalysts
Boosting bio-lipids deoxygenation via tunable metal-support interaction in nickel/ceria-based catalysts
复制标题
通过镍/二氧化铈基催化剂中可调节金属-载体相互作用促进生物脂质脱氧
DOI：
10.1016/j.fuel.2022.124027
复制
发表时间：
2022
期刊：
影响因子：
7.4
通讯作者：
Yuejin Liu
中科院分区：
文献类型：
--
作者：
Lin Fu（付琳）;Zhaoxin Liu;Xin Li（黎新）;Yongfei Li;Houyi Yang;Yuejin Liu
镍催化剂在生物油脂脱氧过程中，由于金属烧结和结焦等原因，通常会发生快速失活。本文采用蒸发诱导自组装（EISA）法、湿浸法（WI）和共沉淀法（CP）制备了一系列Ni/CeO 2-Al 2 O3催化剂，分别命名为NiCeAl-EISA、NiCeAl-WI和NiCeAl-CP。采用BET、XRD、H_2-TPR、HR-TEM、FT-IR、O_2-TPD、NH_3-TPD、RPR、Py-FTIR、XPS和原位XPS等手段对催化剂的孔隙率和表面性质进行了系统的研究。NiCeAl-EISA催化剂在月桂酸甲酯完全转化时的正C11产率为92.2%，并且有效地脱氧不同的FAME，产生相应的烷烃产率为97.8%（n-C9）、96.4%（n-C13）、94.3%（n-C15）和92.9%（n-C17）。NiCeAl-EISA、NiCeAl-WI和NiCeAl-CP催化剂的TOF分别计算为426-719、241-343和148-243 h-1。小桐子油和废食用油也被转化为液体烷烃（C13-18），总收率分别为95.4%和93.7%。与NiCeAl-WI和NiCeAl-CP催化剂相比，NiCeAl-EISA催化剂具有上级催化活性，连续运行11次后，n-C11收率仍保持在92.2%。这种催化剂活性和稳定性的显著提高与Ni/CeO 2-Al 2 O3催化剂的可调SMSI密切相关，该SMSI易于形成丰富的氧空位和界面位（Niδ+-OV-CeOx）。这抑制了强烈的Ni-Al相互作用，从而暴露出更多活性和稳健的Ni位点，以促进R-COOH → R-CHO还原，从而产生更多的烷烃。Ni-Al相互作用的减弱也降低了催化剂的强酸性，从而抑制了焦炭的生成，同时抑制了烃类的C-C键断裂。
Ni-catalysts usually experienced quick deactivation during bio-lipids deoxygenation due to metal sintering and coke. Here we prepared a series of Ni/CeO2-Al2O3catalysts, denoted as NiCeAl-EISA, NiCeAl-WI and NiCeAl-CP, prepared by evaporation-induced self-assembly (EISA), wetness impregnation (WI), co-precipitation (CP) methods, respectively, aiming at tuning metal-support interaction (MSI) in Ni/CeO2-Al2O3catalysts for the deoxygenation of bio-lipids to hydrocarbons. The porosity and surface properties of the catalysts are systematically studied by BET, XRD, H2-TPR, HR-TEM, FT-IR, O2-TPD, NH3-TPD, RPR, Py-FTIR, XPS and in situ XPS. The NiCeAl-EISA catalyst afforded 92.2% n-C11yield at full methyl laurate conversion, and efficiently deoxygenated different FAMEs, yielding corresponding alkanes yields of 97.8% (n-C9), 96.4% (n-C13), 94.3% (n-C15) and 92.9% (n-C17). The TOFs were calculated as 426–719, 241–343 and 148–243 h−1for NiCeAl-EISA, NiCeAl-WI and NiCeAl-CP catalysts, respectively. Jatropha oil and waste cooking oil were also converted into liquid alkanes (C13-18) with a total yield of 95.4% and 93.7%, respectively. The NiCeAl-EISA catalyst exhibits superior catalytic activity and remained stable with 92.2% n-C11yield after 11 consecutive runs, as compared with NiCeAl-WI and NiCeAl-CP. This significant increase in catalyst activity and stability is closely correlated with the tunable SMSI of Ni/CeO2-Al2O3catalyst, which facilely forms abundant oxygen vacancies and interfacial sites (Niδ+-OV-CeOx). This suppresses strong Ni-Al interaction, thus exposing more active and robust Ni sites to promote R-COOH → R-CHO reduction to produce more alkanes. The weakened Ni-Al interaction also reduces the strong acidity and consequently inhibits the coke formation and simultaneously restrains C–C bond cleavage of hydrocarbons.
登录
查看更多内容
影响因子：
7.4
作者：
Norshakirah Ahmad Rashidi;Elnida Mustapha;Yeow Yean Theng;N. A. Razak;Najihah Abdul Bar;Khairul Basyar Baharudin;D. Derawi
通讯作者：
Norshakirah Ahmad Rashidi;Elnida Mustapha;Yeow Yean Theng;N. A. Razak;Najihah Abdul Bar;Khairul Basyar Baharudin;D. Derawi
影响因子：
12.9
作者：
de Souza, Priscilla M.;Rabelo-Neto, Raimundo C.;Noronha, Fabio B.
通讯作者：
Noronha, Fabio B.
影响因子：
5.3
作者：
Hui Xin;Wenjun Zhou;Keyao Zhou;Xiangze Du;Dan Li;Changwei Hu
通讯作者：
Hui Xin;Wenjun Zhou;Keyao Zhou;Xiangze Du;Dan Li;Changwei Hu
影响因子：
7.7
作者：
Zhifei Hao;Guoquan Liu;Nan Ma;He Zhang;Yi Li;Yuguo Xia;Dongpeng Zhang;Sihui Zhan
通讯作者：
Zhifei Hao;Guoquan Liu;Nan Ma;He Zhang;Yi Li;Yuguo Xia;Dongpeng Zhang;Sihui Zhan
影响因子：
22.1
作者：
Weiqing Zheng;Jian Zhang;Q. Ge;Hengyong Xu;Wenzhao Li
通讯作者：
Weiqing Zheng;Jian Zhang;Q. Ge;Hengyong Xu;Wenzhao Li