Regulation of the Heavy Fuel Oil modification process for Medium-Low temperature coal tar pitch aromatic depolymerization-recombination and design of the derived carbon microcrystalline structure

IF 6.2 2区 化学 Q1 CHEMISTRY, ANALYTICAL
Shuaichao Song , Yuan Lv , Junxia Cheng , Xiliang Wen , Wei Guan , Yaming Zhu , Xuefei Zhao
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Abstract

This research addresses the challenge of heterogeneous mosaic carbon structures encountered when directly thermally converting Medium-Low temperature coal tar pitch (MLP) to prepare high-performance carbon materials, by introducing Heavy Fuel Oil (HFO) as a molecular-level modification medium. Directed design of derived carbon microcrystalline structures is achieved by regulating the HFO blending ratio to induce selective depolymerization and reorganization of MLP's aromatic system during low-temperature copolymerization. Studies revealed that HFO, characterized by hydrogen-rich alkyl branches, is capable of efficiently extracting oxygen elements from MLP in low-temperature copolymerization and can guide the polymerization of substituent sites beyond the aromatic rings in the pitch, resulting in the formation of broader sheet-like molecular formations. As a result, there's a notable rise in the toluene-insoluble (TI) levels in the altered pitch to 7.39 %, accompanied by an average molecular weight of 1684 Da, an aromaticity index of 0.394, a branching index of 0.661, and an aromatic degree of 0.89. The altered pitch during thermal conversion-calcination, due to the creation of a uniform miscible/melt state and structural and compositional shifts, stabilizes pitch free radicals through hydrogen supply, leading to a combined effect of “depolymerization-stabilization”. The liquid-phase carbonization setting is significantly enhanced, leading to even breakdown and lamellar reorganization of the pitch. The derived pitch's optical microstructure has evolved from its initial mosaic form to a structured lamellar/fibrous form, concurrently diminishing carbon structural flaws. The derived carbon material's structural organization is greatly improved, achieving an ideal graphite microcrystal concentration of 72.90 %. The research accomplished precise alterations to the optical microstructure of pitch derived from MLP, paving the way for a novel technical route in MLP's high-value use and providing both theoretical groundwork and actionable advice for the regulated creation of high-efficiency carbon materials.
重质燃料油改性中低温煤沥青芳烃解聚-复合工艺调控及衍生碳微晶结构设计
本研究通过引入重质燃料油(HFO)作为分子级改性介质,解决了中低温煤沥青(MLP)直接热转化制备高性能碳材料时遇到的非均相马赛克碳结构的挑战。通过调节HFO共混比例,诱导MLP的芳香族体系在低温共聚过程中选择性解聚和重组,实现衍生碳微晶结构的定向设计。研究表明,以富氢烷基支链为特征的HFO在低温共聚时能够有效地从MLP中提取氧元素,并能引导沥青中芳香环以外取代基的聚合,从而形成更宽的片状分子结构。结果表明,改性沥青中甲苯不溶性(TI)含量显著提高至7.39 %,平均分子量为1684 Da,芳香指数为0.394,分支指数为0.661,芳香度为0.89。热转化-煅烧过程中沥青的改变,由于产生了均匀的混溶/熔融状态以及结构和成分的变化,通过氢供应稳定了沥青自由基,从而产生了“解聚-稳定”的综合效应。液相碳化设置显著增强,导致均匀的击穿和层状重组的沥青。衍生沥青的光学微观结构已经从最初的马赛克形式演变为有结构的片层/纤维形式,同时减少了碳结构缺陷。所得碳材料的结构组织得到了很大的改善,石墨微晶浓度达到了理想的72.90 %。该研究完成了对MLP衍生的沥青光学微观结构的精确改变,为MLP的高价值应用开辟了一条新的技术路线,并为高效碳材料的规范创造提供了理论基础和可行建议。
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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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