介质阻挡放电反应条件下生物油加氢提质机理分析

doi:10.3969/j.issn.1671-7775.2023.02.011

摘要
图/表
参考文献(19)
相关文章 (5)

全文: PDF (1794 KB) HTML (1 KB)
输出: BibTeX | EndNote (RIS)

摘要介质阻挡放电反应技术是实现温和反应条件下热敏性生物油加氢提质的有效途径.为解析介质阻挡放电条件下生物油各组分加氢反应途径及机理，在此前研究的基础上，以模型化合物配制的模拟生物油为研究对象进行了加氢试验及理论研究.结果表明：丁酸与丁醇主要通过酯化生成丁酸丁酯，羟基丙酮的加氢液相产物主要为异丁醛，糠醛主要通过加氢饱和生成糠醇，愈创木酚主要通过甲基断裂生成邻苯二酚以及进一步加氢得到环己烯；模型化合物丁酸、丁醇、糠醛、羟基丙酮、愈创木酚、乙酸乙酯和环己烷的转化率依次为82.86%、85.95%、82.05%、83.79%、51.70%、68.54%和13.03%，导致生物油腐蚀性及热稳定较差的酸类、醛类、酮类组分表现出较高的反应活性.

	服务

	把本文推荐给朋友
	加入我的书架
	加入引用管理器
	E-mail Alert
	RSS
	作者相关文章
	赵卫东1
	朱艳辉1
	戚小龙1
	王军锋2

关键词 ：生物油, 模型化合物, 介质阻挡放电, 加氢, 反应路径

Abstract：Dielectric barrier discharge reaction technology is an effective way to achieve the hydrogenation and upgrading of thermosensitive bio-oil under mild reaction conditions. To analyze the hydrogenation reaction pathway and mechanism of each component of bio-oil under the condition of dielectric barrier discharge, hydrogenation experiments and theoretical investigation on the simulated bio-oil prepared by model compounds were conducted based on the previous studies. The results show that butyric acid and butanol are mainly esterified to produce butyl butyrate, and the hydrogenation liquid product of hydroxyl acetone is mainly isobutyl aldehyde. Furfural is mainly saturated by hydrogenation to produce furfuryl alcohol, and the guaiacol is mainly broken by methyl to produce catechol and further hydrogenation to cyclohexene. The conversion rates of model compounds of butyric acid, butanol, furfural, hydroxyacetone, guaiacol, ethyl acetate and cyclohexane are 82.86%, 85.95%, 82.05%, 83.79%, 51.70%, 68.54% and 13.03%, respectively. Acid, aldehyde and ketone can lead bio-oil to poor corrosion and thermal stability and show high reactivity.

Key words： bio-oil model compound dielectric barrier discharge hydrogenation reaction path

收稿日期: 2021-03-09

基金资助:国家自然科学基金资助项目(51761145011)

作者简介: 赵卫东(1975—)，男，山东梁山人，副教授 (zhaowd@ujs.edu.cn)，主要从事低温等离子体技术的应用研究. 朱艳辉(1994—)，男，江西萍乡人，硕士研究生(18867317786@163.com)，主要从事生物质能的利用研究.

引用本文:

赵卫东1，朱艳辉1，戚小龙1，王军锋2. 介质阻挡放电反应条件下生物油加氢提质机理分析[J]. 江苏大学学报（自然科学版）, 2023, 44(2): 200-206. ZHAO Weidong1, ZHU Yanhui1, QI Xiaolong1, WANG Junfeng2. Mechanism analysis of bio-oil hydrogenation under condition of dielectric barrier discharge reaction[J]. Journal of Jiangsu University(Natural Science Eidtion) , 2023, 44(2): 200-206.

链接本文:

http://zzs.ujs.edu.cn/xbzkb/CN/10.3969/j.issn.1671-7775.2023.02.011 或 http://zzs.ujs.edu.cn/xbzkb/CN/Y2023/V44/I2/200

［1］	KAN T, STREZOV V, EVANS T J. Lignocellulosic bio-mass pyrolysis: a review of product properties and effects of pyrolysis parameters[J]. Renewable & Sustainable Energy Reviews, 2016, 57(28): 1126-1140.
［2］	ZULKANIA A, YASHA N Z, RACHMAN S A, et al. In situ pyrolysis of pine flowers to produce bio-oil: effect of temperature and catalyst treatment[J]. Materials Science Forum, 2020, 981: 185-189.
［3］	牛淼淼, 杨佳耀, 李尚, 等. 生物质热解制生物油及其提质研究现状[J]. 生物质化学工程, 2018, 52(5):55-61.
	NIU M M, YANG J Y, LI S, et al. Review on biomass pyrolysis for bio-oil and upgrading research[J]. Biomass Chemical Engineering, 2018, 52(5):55-61. (in Chinese)
［4］	HANSEN S, MIRKOUEI A, DIAZ L A. A comprehensive state-of-technology review for upgrading bio-oil to renewable or blended hydrocarbon fuels[J]. Renewable and Sustainable Energy Reviews, 2020, 118:109548-109562.
［5］	GOLLAKOTA A R K, REDDY M, SUBRAMANYAM M D, et al. A review on the upgradation techniques of pyrolysis oil[J]. Renewable and Sustainable Energy Reviews, 2016, 58: 1543-1568.
［6］	张小虎，张随平，张世刚.生物油催化加氢综述[J].广州化学，2019,47（17）：45-48.
	ZHANG X H, ZHANG S P, ZHANG S G. Review of bio-oil catalytic hydrogenation[J]. Guangzhou Chemical Industry, 2019,47（17）：45-48. (in Chinese)
［7］	LI X P, CHEN G Y, LIU C X, et al. Hydrodeoxyge-nation of lignin-derived bio-oil using molecular sieves supported metal catalysts: a critical review[J]. Rene-wable & Sustainable Energy Reviews, 2017, 71: 296-308.
［8］	LIU L N, WANG Q, SONG J W, et al. Dry reforming of model biomass pyrolysis products to syngas by dielectric barrier discharge plasma[J]. International Journal of Hydrogen Energy, 2018, 43(22): 10281-10293.
［9］	TAGHVAEI H, RAHIMPOUR M R. Catalytic hydro-deoxygenation of bio-oil using in situ generated hydrogen in plasma reactor: effects of allumina supported catalysts and plasma parameters[J]. Process Safety and Environmental Protection, 2018, 121:221-228.
[10]	ZHAO W D, ZHANG X Y, HUANG J Q, et al. Hydrogenation of bio-oil via gas-liquid two-phase discharge reaction system[J]. Process Safety and Environmental Protection, 2018, 118: 167-177.
[11]	XIU S N, SHAHBAZI A. Bio-oil production and upgrading research: a review[J]. Renewable and Sustainable Energy Reviews, 2012, 16(7): 4406-4414.
[12]	ISAHAK W N R W, HISHAM M W M, YARMO M A, et al. A review on bio-oil production from biomass by using pyrolysis method[J]. Renewable & Sustainable Energy Reviews, 2012, 16(8): 5910-5923.
[13]	张潇尹. 基于介质阻挡放电反应技术的生物柴油选择性加氢提质试验研究[D]. 镇江: 江苏大学, 2019.
[14]	OLIVEIRA R R, ROCHA A B. Acrylic acid hydro-deoxygenation reaction mechanism over molybdenum carbide studied by DFT calculations[J]. Journal of Mole-cular Modeling, 2019, 25(10): 309-319.
[15]	ARORA S, GUPTA N, SINGH V. Improved Pd/Ru metal supported Graphene oxide nano-catalysts for hydrodeoxygenation (HDO) of vanillyl alcohol, vanillin and lignin[J]. Green Chemistry, 2020, 22(6):2018-2027.
[16]	JENKINS R W, MOORE C M, SEMELSBERGER T A, et al. Heterogeneous ketone hydrodeoxygenation for the production of fuels and feedstocks from biomass[J]. ChemCatChem, 2017,9(14):2807-2815.
[17]	CHEN W, LUO Z Y, YU C J, et al. Catalytic transformations of acids, aldehydes, and phenols in bio-oil to alcohols and esters[J]. Fuel, 2014, 135(1): 55-62.
[18]	邱泽刚, 尹婵娟, 李志勤, 等. 酚类加氢脱氧催化剂研究进展[J]. 化工进展, 2019, 38(8): 3658-3669.
	QIU Z G, YIN C J, LI Z Q, et al. Recent advances in hydrodeoxygenation catalysts for phenols[J]. Chemical Industry and Engineering Progress, 2019, 38(8): 3658-3669. (in Chinese)
[19]	BEHTASH S, LU J M, WALKER E, et al. Solvent effects in the liquid phase hydrodeoxygenation of methyl propionate over a Pd(111) catalyst model[J]. Journal of Catalysis, 2016, 333: 171-183.