在MgO调控的NiO/SiO2催化剂上通过油酸催化热解生产绿色烃类

IF 6.2 2区 化学 Q1 CHEMISTRY, ANALYTICAL Journal of Analytical and Applied Pyrolysis Pub Date : 2025-03-01 Epub Date: 2024-12-12 DOI:10.1016/j.jaap.2024.106913
Meihua Fu , Shengzu Zhang , Jida Wang , Feng Shi , Yifei Chen , Liu Chengguo , Shunxiong Yang , Defa Hou , Yi Lu , Fulin Yang , Can Liu , Xu Lin , Zhifeng Zheng , Yunwu Zheng
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引用次数: 0

摘要

脂肪酸的选择性催化脱氧已被认为是一种很有前途的生产可持续燃料的方法。然而,有限的催化活性往往导致所需产物的选择性降低。本文合成了一系列具有mg修饰NiO界面的mgo促进NiO/SiO2催化剂,用于油酸催化脱氧制汽油级烃。详细的表征和实验表明,Ni0是活性相,可以提供活性H原子,通过解离H2促进C-C键的裂解和加氢脱氧;Mg的引入显著促进NiOx的良好分散和氧空位含量的增加,以吸附和活化羰基。值得注意的是,3 %-Mg促进的Ni- sio2催化剂表现出优异的催化活性,其转化率为100 %,烃类化合物收率和烯烃收率分别为96.83 %和54.58 %,通过脱水加氢过程对汽油馏分的选择性为70.25 %,这是由于优异的酸性位置、氧空位、织构性质以及Ni和Mg组分的均匀分布和协同促进作用。此外,焦炭沉积、活性物质还原和浸出是催化剂失活的合理原因,导致5次循环后烃类收率和烯烃选择性下降。这种深刻的认识为催化剂的合理设计提供了一个简单的策略,所开发的Mg/Ni-Si催化剂突出了从生物质衍生的含氧化合物生产绿色富烃燃料的巨大前景。
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Green hydrocarbon-range production via catalytic pyrolysis of oleic acid over MgO regulated NiO/SiO2 catalysts
Selective catalytic deoxygenation of fatty acids has been recognized as a promising approach for producing sustainable fuels. However, limited catalytic activity often results in reduced selectivity for desired products. Herein, a series of MgO-promoted NiO/SiO2 catalysts featuring Mg-decorated NiO interfaces was synthesized for oleic acid catalytic deoxygenation to gasoline-range hydrocarbon. Detailed characterization and experiment revealed that Ni0 species was the active phase which could provide active H atom to enhance C-C bond cracking and hydrodeoxygenation via dissociation H2, and Mg species introduction significant promoted NiOx species well-dispersion and enhanced oxygen vacancies content to adsorption and activate carbonyl group. Notably, 3 %-Mg promoted Ni-SiO2 catalyst exhibited superior catalytic activity with 100 % conversion rate, 96.83 % and 54.58 % yield of hydrocarbon compound and olefins yield and 70.25 % selectivity to gasoline-range fraction via dehydration-hydrogenation process due to excellent acidity site, oxygen vacancies, texture properties and well-distribution and synergistic promoting effect of Ni and Mg species. Furthermore, coke deposition, active species reduction and leaching was reasonable for catalyst deactivation, resulting in hydrocarbon yield and olefin selectivity decreasing after five cycling. This deep understanding provided a facile strategy for catalyst rational design and the developed Mg/Ni-Si catalysts highlighted a great prospect for produce green hydrocarbon-rich fuel from biomass-derived oxygen-containing compound.
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来源期刊
CiteScore
9.10
自引率
11.70%
发文量
340
审稿时长
44 days
期刊介绍: The Journal of Analytical and Applied Pyrolysis (JAAP) is devoted to the publication of papers dealing with innovative applications of pyrolysis processes, the characterization of products related to pyrolysis reactions, and investigations of reaction mechanism. To be considered by JAAP, a manuscript should present significant progress in these topics. The novelty must be satisfactorily argued in the cover letter. A manuscript with a cover letter to the editor not addressing the novelty is likely to be rejected without review.
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