在亚临界和超临界水中强化热解油泥和聚合物废料:使用基于镍钴的双金属催化剂生产低碳合成气和液态烃

IF 5.8 2区 化学 Q1 CHEMISTRY, ANALYTICAL
Richard Djimasbe , Mikhail A. Varfolomeev , Mohamed A. Abdelaal , Eduard A. Galiullin , Dmitry A. Feoktistov , Rustam R. Davletshin , Ameen A. Al-Muntaser , Muneer A. Suwaid , Dmitry A. Emelyanov , Aleksandr A. Rodionov , Almaz L. Zinnatullin , Alexey V. Vakhin , Irek I. Mukhamatdinov , Sergey A. Sitnov , Liliya K. Galiakhmetova , Konstantin Yu. Prochukhan
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引用次数: 0

摘要

塑料材料废料的积累、油泥的形成以及家庭用户和石油工业在自然界中的碳氢化合物泄漏,对环境构成了重大威胁,因此,研究新的有效技术以扩大废物回收利用的可能性至关重要。然而,本文的重点是基于 Al2O3 支持的 Ni-Co 合成双金属催化剂 (BMC),用于在亚临界和超临界水中热解聚乙烯 (PE)、聚对苯二甲酸乙二酯 (PET) 和油污泥 (OS) 样品,以生产燃料和低碳合成气。实验在间歇式反应器中进行,温度和压力范围为 350 - 410°C 和 213.7 - 268.9 巴,持续时间为 1 小时。分别采用 XRD、XRF、SEM-EDX、TGA、FTIR、GC-MS、GC 和 EPR 方法对 BMC 和热解产物进行了表征。研究结果表明,总气体(包括不饱和气体)的产量随热解温度的升高而增加,其组成为 C1-C4、C2=C4、H2、CO 和 CO2。在 380°C 的温度下,低密度聚乙烯和 PET-II 的热解在没有 BMC 的情况下,通过 PET 的二次裂解和脱羧,产生的 C2=C4、CO 和 CO2 分别达到 6.2、33.14 和 48.34 摩尔%。研究发现,PET 高温分解产生的液体产品的主要成分是苯甲酸和联苯,而且在没有 BMC 的情况下,苯甲酸本身会催化 CO2 的生成反应。因此,使用 BMC 后,CO 和 CO2 的生成速度分别降低了 2.80 倍和 3.5 倍,而 C1、H2 和 ΣC2-C4 的生成速度则分别提高到最高 45 摩尔百分率、24.63 摩尔百分率和 44.59 摩尔百分率。此外,在有 BMC 存在的 380°C 下,PE-I 的转化率高达 58.46 wt%,PE-IV 的液态烃转化率为 47.24 wt%。结果表明,大部分的 H2 来源基本上是基于水气变换反应和 Sabatier 反应。聚乙烯热解过程中约有 43-50% 的水,使用 BMC 的液体产品中仅检测到 0.4% 的十二碳二烯-1-醇和 5% 的癸二酸。总之,使用 BMC 在 SCW 水中热解样品有利于生产 H2 和 C1,同时减少 CO 和 CO2 的排放。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Enhanced pyrolysis of oil sludge and polymer waste in sub and supercritical water: Production of low-carbon syngas, and liquid hydrocarbons using bimetallic catalyst based on nickel-cobalt
Accumulation of waste of plastic materials, formation of the oil sludge and hydrocarbons spills from household users and petroleum industries processes in nature, constitute a major danger for the environment whence, research of new effective techniques to expand the possibilities of the wastes recycling, is crucial. However, this paper focuses on the synthesis of bimetallic catalyst (BMC) based on Ni-Co supported on Al2O3 for the pyrolysis of polyethylene (PE), polyethylene terephthalate (PET) and oil sludge (OS) samples in sub and supercritical water (sub- and SCW) for fuels and low carbon syngas production. Experiments were performed in a batch reactor at the temperatures and pressure ranges 350 – 410°C and 213.7 – 268.9 bars for 1 h. Characterization of the BMC and pyrolysis products was done by XRD, XRF, SEM-EDX, TGA, FTIR, GC-MS, GC and EPR methods, respectively. The findings reveal that the yield of the total gases, including unsaturated gases, increase with the pyrolysis temperature, and are composed by C1–C4, C2=C4, H2, CO and CO2. At a temperature of 380°C it is found that, the pyrolysis of the low density PE and that of PET-II, in the absence of BMC significantly generated the C2=C4, CO and CO2 up to 6.2, 33.14 and 48.34 mol.%, through a secondary cracking and decarboxylation of PET, respectively. It is found that, the composition of the resulting liquid product from pyrolysis of PET, is mostly composed of Benzoic acids, Biphenyl and that, the Benzoic acid catalyzes the reaction of CO2 formation itself, in the absence of BMC. Thus, use of BMC reduced the rate of CO and CO2 by 2.80 and 3.5 times while that of C1, H2 and ΣC2-C4 increased to maximal of 45 mol.%, 24.63 mol.% and 44.59 mol.%, respectively. Moreover, a high conversion rate of 58.46 wt% was achieved from the PE-I, and that of liquid hydrocarbons of 47.24 wt% observed for PE-IV, at 380°C in the presence of BMC. The results revealed that most of H2 source is essentially based on the water gas shift reaction and Sabatier's. Around 43–50 wt% of water was involved in the pyrolysis of PE, and that 0.4 % of Dodecadien-1-ol and 5 % of Decanedioic acid were detected only in the liquid product using the BMC. Overall, the use of BMC for pyrolysis of samples in SCW water is beneficial for the production of H2 and C1 with the reduction of CO and CO2 emissions.
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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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