Mo/N共掺杂zif -67基Co-Mo15@NC上东明褐煤两步级联降解研究

IF 7.5 1区 工程技术 Q2 ENERGY & FUELS Fuel Pub Date : 2025-07-01 Epub Date: 2025-02-21 DOI:10.1016/j.fuel.2025.134803
Guang-Hui Liu , Hao-Dong An , Han Wang , Ya-Jun Ma , Yan-Jun Li , Yu-Hong Kang , Jie Kang , Wei Zhao , Sheng-Kang Wang , Xian-Yong Wei
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引用次数: 0

摘要

采用Mo/N共掺杂原位热解策略制备了一种新型的zif -67基Co-Mo双金属协同催化剂,并将其应用于东明褐煤加氢裂化(H2活化)-醇解(溶剂活化)级联转化体系。Co-Mo15@NC含有丰富的空位/缺陷,可以区别激活H2和乙醇,促进褐煤衍生芳基醚选择性转化为高产芳烃或芳香单体。综合评价表明,该催化剂具有优良的性能。C-O具有解理活性和循环稳定性,且易于磁回收。中间体和产物分析表明,加氢裂化体系涉及H+、H·和不对称双原子活性氢(δ+H··Hδ-)的协同转移,乙醇分解体系涉及H+、H·、C2H5+和C2H5O·的协同转移。一段加氢裂化油(SP1C)富含烷烃和多环芳烃,总烃含量由67.7%增加到78.1%;二段乙醇裂解油(SP2C)富含烷烃、芳烃和酯类,含氧化合物总含量由66.7%增加到90.3%。采用基于H2和乙醇活化的两步级联降解策略,可得到富烃油和富o油两种类型的增值油。
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Two-step cascade degradation of Dongming lignite over Mo/N co-doped ZIF-67-based Co-Mo15@NC
A novel ZIF-67-based Co-Mo bimetallic synergistic catalyst was prepared via Mo/N co-doping in-situ pyrolysis strategy and used in the cascade conversion system of hydrocracking (H2 activation) and ethanolysis (solvent activation) of Dongming lignite. Co-Mo15@NC, rich in vacancies/defects, can differentially activate H2 and ethanol, promoting the selective conversion of lignite-derived aryl ethers into high-yield arenes or aromatic monomers. Comprehensive evaluation indicates that this catalyst exhibits excellent > C-O- cleavage activity and cyclic stability, and is easy to magnetic recovery. Analysis of intermediates and products shows that hydrocracking system involves the synergistic transfer of H+, H·, and asymmetric diatomic active hydrogen (δ+H···Hδ-), while ethanolysis system involves the synergistic transfer of H+, H·, C2H5+, and C2H5O·. Hydrocracking-derived oil (SP1C) from first-stage is rich in alkanes and polycyclic arenes, with the total content of hydrocarbons increasing from 67.7 to 78.1 %, while ethanolysis-derived oil (SP2C) from second-stage is rich in alkanols, arenols, and esters, with the total content of O-containing compounds increasing from 66.7 to 90.3 %. Two types of value-added oils, i.e., hydrocarbon-rich and O-rich oils, can be obtained by the two-step cascade degradation strategy based on H2 and ethanol activation.
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来源期刊
Fuel
Fuel 工程技术-工程:化工
CiteScore
12.80
自引率
20.30%
发文量
3506
审稿时长
64 days
期刊介绍: The exploration of energy sources remains a critical matter of study. For the past nine decades, fuel has consistently held the forefront in primary research efforts within the field of energy science. This area of investigation encompasses a wide range of subjects, with a particular emphasis on emerging concerns like environmental factors and pollution.
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