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超声辅助使用绿色合成的对苯二甲酸铝[MIL-53(Al)]对模拟燃料进行一锅法氧化脱硫

Ultrasounds assisted one-pot oxidative desulfurization of model fuel using green synthesized aluminum terephthalate [MIL-53(Al)].

作者信息

Metawea Rodaina, Farag Hassan A, El-Ashtoukhy El-Sayed, El-Latif Mona M Abd, El-Sayed Eman M

机构信息

Alexandria Petroleum Company, Alexandria, Egypt.

Chemical Engineering Department, Faculty of Engineering, Alexandria University, Alexandria, Egypt.

出版信息

Sci Rep. 2023 Aug 22;13(1):13728. doi: 10.1038/s41598-023-40955-3.

DOI:10.1038/s41598-023-40955-3
PMID:37608052
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10444795/
Abstract

Oxidative desulfurization (ODS) is considered to be one of the most promising desulfurization processes as it is energy-efficient and requires mild operating conditions. In this study, a novel green synthesized Al- based metal-organic framework with high surface area has been synthesized hydrothermally using waste polyethylene terephthalate bottles (PET) as a source of terephthalic acid as an organic linker. The prepared Al based MOF have been characterized using Fourier transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), scanning electron microscope (SEM) and transmission electron microscopy (TEM). The catalytic activity of the prepared Al-MOF was evaluated in the oxidative desulfurization (ODS) of both modeled and real crude oil samples. The different operating parameters (temperature, time, catalyst dose, oxidant loading and sonication) on the ODS performance have been optimized. The optimal conditions for maximum removal of thiophene from modeled oil samples were found to be 30 min, 0.5 g of catalyst and 1:3 oil to oxidant ratio. Under the optimized conditions, sulfur removal in real oil samples obtained from Alexandria petroleum company was 90%. The results revealed that, the presented approach is credited to cost-effectiveness, environmental benignity, and ease of preparation, predicting great prospects for desulfurization of fuel oils on a commercial level.

摘要

氧化脱硫(ODS)被认为是最具前景的脱硫工艺之一,因为它节能且操作条件温和。在本研究中,以废弃聚对苯二甲酸乙二酯瓶(PET)作为对苯二甲酸的来源作为有机连接体,通过水热法合成了一种具有高比表面积的新型绿色合成铝基金属有机框架材料。所制备的铝基金属有机框架材料已通过傅里叶变换红外光谱(FTIR)、X射线衍射(XRD)、扫描电子显微镜(SEM)和透射电子显微镜(TEM)进行了表征。在模拟原油样品和实际原油样品的氧化脱硫(ODS)中评估了所制备的铝基金属有机框架材料的催化活性。对氧化脱硫性能的不同操作参数(温度、时间、催化剂用量、氧化剂负载量和超声处理)进行了优化。发现从模拟油样中最大程度去除噻吩的最佳条件为30分钟、0.5克催化剂以及油与氧化剂的比例为1:3。在优化条件下,从亚历山大石油公司获得的实际油样中的硫去除率为90%。结果表明,所提出的方法具有成本效益、环境友好且易于制备的特点,预示着在商业层面上对燃料油进行脱硫具有广阔前景。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c8c4/10444795/d9b591e61246/41598_2023_40955_Fig8_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c8c4/10444795/aef33f8d3769/41598_2023_40955_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c8c4/10444795/e51f0c7e7981/41598_2023_40955_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c8c4/10444795/eb2455d6633b/41598_2023_40955_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c8c4/10444795/622de66f00cd/41598_2023_40955_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c8c4/10444795/c24493cf5e8e/41598_2023_40955_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c8c4/10444795/d9b591e61246/41598_2023_40955_Fig8_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c8c4/10444795/aef33f8d3769/41598_2023_40955_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c8c4/10444795/e51f0c7e7981/41598_2023_40955_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c8c4/10444795/eb2455d6633b/41598_2023_40955_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c8c4/10444795/622de66f00cd/41598_2023_40955_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c8c4/10444795/c24493cf5e8e/41598_2023_40955_Fig6_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c8c4/10444795/d9b591e61246/41598_2023_40955_Fig8_HTML.jpg

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本文引用的文献

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RSC Adv. 2018 Apr 12;8(25):13714-13721. doi: 10.1039/c8ra01542b. eCollection 2018 Apr 11.
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Study on ultrasound-assisted oxidative desulfurization for crude oil.超声辅助氧化脱硫技术在原油中的应用研究。
Ultrason Sonochem. 2020 May;63:104946. doi: 10.1016/j.ultsonch.2019.104946. Epub 2019 Dec 26.
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Ultrasound-assisted oxidative desulfurization process of liquid fuel by phosphotungstic acid encapsulated in a interpenetrating amine-functionalized Zn(II)-based MOF as catalyst.
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Ultrason Sonochem. 2017 Jan;34:713-720. doi: 10.1016/j.ultsonch.2016.07.006. Epub 2016 Jul 15.
4
The metal-organic framework MIL-53(Al) constructed from multiple metal sources: alumina, aluminum hydroxide, and boehmite.由多种金属源构建的金属有机框架MIL-53(Al):氧化铝、氢氧化铝和勃姆石。
Chemistry. 2015 Apr 27;21(18):6913-20. doi: 10.1002/chem.201406531. Epub 2015 Mar 10.