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超声波耦合废机油加氢改质非粮生物油制取“绿色柴油”

项目来源

国家自然科学基金(NSFC)

项目主持人

段培高

项目受资助机构

河南理工大学

立项年度

2017

立项时间

未公开

项目编号

21776063

项目级别

国家级

研究期限

未知 / 未知

受资助金额

64.00万元

学科

化学科学-化学工程与工业化学-资源、环境与生态化工

学科代码

B-B08-B0816

基金类别

面上项目

关键词

超声波 ; 加氢改质 ; 绿色柴油 ; 废机油 ; 非粮生物油 ; Ultrasound ; waste engine oil ; non-food bio-oil ; hydro-upgrading ; green diesel

参与者

王枫；闫卫红；张会菊；许玉平；焦佳丽；杨世坤；李世昌；谢龙飞

参与机构

南阳理工学院

项目标书摘要：传质阻力大、催化效果差、积碳严重是非粮生物油催化加氢改质制取“绿色柴油”面临的主要技术瓶颈。为此，本项目提出生物油催化加氢改质新途径——超声波耦合废机油加氢改质非粮生物油制取“绿色柴油”。拟在生物油催化加氢改质中引入超声波并以废机油为改质介质，利用超声波产生的冲击波和微射流实现沥青质的均匀分散，促进催化剂和生物油的有效接触，增强催化效果；利用废机油增强生物油和改质介质的互溶性，强化传质，减少积碳生成，得到产率高、品质好的改质油。通过本项目研究，确定生物油氢化改质的核心化学反应及其动力学，筛选出高效复合贵金属—钼基催化剂；明确催化脱氮脱氧脱硫催化反应动力学、催化剂失活机理及回收再生工艺；确立改质过程积碳成因及废机油中添加剂对脱氮、脱氧和脱硫以及积碳形成的影响机制；通过对超声波耦合废机油加氢改质生物油反应条件优化，摸清反应条件对改质油产率与元素组成的影响规律，形成定向调控技术。

Application Abstract: Large mass transfer resistance,poor catalytic effect of catalyst,and severe coke formation are the major technical bottlenecks in production of“green diesel encountered during catalytic hydro-upgrading of nonfood bio-oil”.In view of these issues,a new catalytic hydro-upgrading way of bio-oil is proposed-ultrasound coupling waste engine oil to hydro-upgrade non-food bio-oil for production of“green diesel”.The ultrasound is intended to be introduced during the catalytic hydro-upgrading process of bio-oil,and waste engine oil is used as upgrading medium.Using shock waves and cavitation microjet generated by ultrasound to achieve uniform dispersion of asphalt,which promote effective contact between catalyst and bio-oil and enhance the catalytic effect of catalyst.Using the waste engine oil to enhance mutual solubility of bio-oil and the upgrading media to intensify mass transfer and to reduce coke formation to obtain high yield,good quality of upgraded bio-oil.Through the study of this project,the core chemical reactions and their kinetics of hydrogenation of bio-oil were determined,high performance of noble metal-Mo based composite catalysts were selected;catalytic reaction kinetics,deactivation mechanism of the catalyst and recovery and regeneration process were elucidated;effect of reaction conditions on yield and elemental composition of upgraded bio-oil was studied through optimization of reaction conditions for hydrogenation of bio-oil through ultrasound coupling waste engine oil.

项目受资助省

河南省

项目结题报告(全文)

目前“人车争粮”的产业模式、高成本的生物质原料及其转化技术仍是制约生物液体燃料快速发展的瓶颈。筛选质优价廉的非粮生物质原料及其高效、科学的转换技术是实现生物液体燃料规模化发展的前提基础，同时对于保护生态环境、实现人类社会能源的可持续发展具有非常重要的意义。1)采用超声波对微藻水热液化生物油进行了预处理，并考察了声强、频率和时间对生物油理化性能的影响;2)研究了不同非粮生物质(微藻、浮萍、秸秆、市政污泥、油莎豆)和废弃轮胎的热解、水热液化、醇解行为，并对不同生物质原料热化学转化反应参数进行了优化，获得了产率高和品质好的粗生物油;3)采用微藻作为生物质原料，选用不同的催化剂进行了超临界水气化，气化所得氢气作为生物油加氢提质的氢源，实现原料利用的内循环;4)以微藻、秸秆为原料，通过不同的热化学转化方法制备生物油，然后对生物油进行加氢提质，降低粘度、脱除氮硫氧，提高生物油品质，或直接让生物质原料和废弃机油进行在线氢化热解，同时实现生物油制备及其在线提质，制备高品质车用型烃类燃料;5)将生物质液化、气化以及加氢提质过程中产生的废弃物进行了资源化利用研究，制备了高值化学品和碳材料;6)初步尝试了将生物质转化为高附加值化学品的研究。本项目在SCI期刊上发表备注项目号的研究论文40篇,SCI-2区以上33篇，总引用频次338次),1篇论文入选2018年度获河南省自然科学一等奖(优秀学术论文类);授权发明专利6项；培养博士研究生7名，其中留学生博士4名，培养硕士研究生13名；积极参加国际或全国性学术会议20次以上。2018年，入选河南省科技创新杰出青年、河南省高校科技创新团队、河南省学术技术带头人、盐城市科技创新创业领军人才称号、代言中国化学会元素周期表中的“钕”元素;2019年，入选美国化学会IECR 2019 Class of Influential Researchers(全球共计32人)、陕西省高层次人才;2021年，中国发明学会创业创新一等奖、第十二届发明创业奖·人物奖、产学研合作创新奖(个人)。

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  • 1.Hydrothermal gasification of microalgae over nickel catalysts for production of hydrogen-rich fuel gas: Effect of zeolite supports

    • 关键词：
    • Microalgae; Supercritical water gasification; Ni/zeolites; Hydrogen;Fuel gas;SUPERCRITICAL WATER GASIFICATION; BIOMASS GASIFICATION; METHANE
    • Xie, Long-Fei;Duan, Pei-Gao;Jiao, Jia-Li;Xu, Yu-Ping
    • 《6th International Conference on Energy, Engineering and EnvironmentalEngineering 》
    • 2019年
    • AUG 25-26, 2018
    • Beijing, PEOPLES R CHINA
    • 会议

    A series of Ni catalysts with different zeolites were prepared by wet impregnation method and used to catalyze supercritical water gasification (SCWG) of microalgae for production of hydrogen-rich fuel gas under conditions of 430 degrees C, 60 min, p(H2O) = 0.162 g/cm(3), 2 g/g Ni/zeolites. Compared with noncatalytic SCWG, the presence of Ni/zeolite could increase the hydrogen gasification efficiency and carbon gasification efficiency by promoting water-gas shift and steam reforming reactions which are mainly affected by the amount of strong acid sites and Ni, respectively. The highest carbon gasification efficiency (CGE) and hydrogen gasification efficiency (HGE) of 23.61% and 23.55% were achieved with Ni/HY (Na2O, 0.8%). The gaseous produced mainly consisted of H-2 and CO2. The H-2 content in the gaseous products varied from 27.15 to 40.51% depending on the Ni/zeolites and increased with increasing the SiO2/Al2O3 molar ratio of HZSM-5, which is 2.3-3.6 times higher than that of produced without catalyst. The H-2 yield varied between 2.57 and 3.61 mmol/g depending on the Ni/zeolites and increased from 2.19 to 5.61 mmol/g with increasing the SiO2/Al2O3 molar ratio from 50:1 to 170:1, which is 3.6-7.8 times higher than that of produced without catalyst. Coke formation, surface area loss, and sintering of Ni could decrease the activity of the Ni/zeolites. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

    ...

  • 2.Hydrothermal gasification of microalgae over nickel catalysts for production of hydrogen-rich fuel gas: Effect of zeolite supports

    • 关键词：
    • Microalgae; Supercritical water gasification; Ni/zeolites; Hydrogen;Fuel gas;SUPERCRITICAL WATER GASIFICATION; BIOMASS GASIFICATION; METHANE
    • Xie, Long-Fei;Duan, Pei-Gao;Jiao, Jia-Li;Xu, Yu-Ping
    • 《6th International Conference on Energy, Engineering and EnvironmentalEngineering 》
    • 2019年
    • AUG 25-26, 2018
    • Beijing, PEOPLES R CHINA
    • 会议

    A series of Ni catalysts with different zeolites were prepared by wet impregnation method and used to catalyze supercritical water gasification (SCWG) of microalgae for production of hydrogen-rich fuel gas under conditions of 430 degrees C, 60 min, p(H2O) = 0.162 g/cm(3), 2 g/g Ni/zeolites. Compared with noncatalytic SCWG, the presence of Ni/zeolite could increase the hydrogen gasification efficiency and carbon gasification efficiency by promoting water-gas shift and steam reforming reactions which are mainly affected by the amount of strong acid sites and Ni, respectively. The highest carbon gasification efficiency (CGE) and hydrogen gasification efficiency (HGE) of 23.61% and 23.55% were achieved with Ni/HY (Na2O, 0.8%). The gaseous produced mainly consisted of H-2 and CO2. The H-2 content in the gaseous products varied from 27.15 to 40.51% depending on the Ni/zeolites and increased with increasing the SiO2/Al2O3 molar ratio of HZSM-5, which is 2.3-3.6 times higher than that of produced without catalyst. The H-2 yield varied between 2.57 and 3.61 mmol/g depending on the Ni/zeolites and increased from 2.19 to 5.61 mmol/g with increasing the SiO2/Al2O3 molar ratio from 50:1 to 170:1, which is 3.6-7.8 times higher than that of produced without catalyst. Coke formation, surface area loss, and sintering of Ni could decrease the activity of the Ni/zeolites. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

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