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生物油及其衍生物催化重整制氢研究进展

李果 张安东 万震 李志合 王绍庆 李宁 张鹏

李果, 张安东, 万震, 李志合, 王绍庆, 李宁, 张鹏. 生物油及其衍生物催化重整制氢研究进展[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2022061
引用本文: 李果, 张安东, 万震, 李志合, 王绍庆, 李宁, 张鹏. 生物油及其衍生物催化重整制氢研究进展[J]. 燃料化学学报. doi: 10.19906/j.cnki.JFCT.2022061
LI Guo, ZHANG An-dong, WAN Zhen, LI Zhi-he, WANG Shao-qing, LI Ning, ZHANG Peng. Research progress on catalytic reforming of bio-oil and its derivatives for hydrogen production[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2022061
Citation: LI Guo, ZHANG An-dong, WAN Zhen, LI Zhi-he, WANG Shao-qing, LI Ning, ZHANG Peng. Research progress on catalytic reforming of bio-oil and its derivatives for hydrogen production[J]. Journal of Fuel Chemistry and Technology. doi: 10.19906/j.cnki.JFCT.2022061

生物油及其衍生物催化重整制氢研究进展

doi: 10.19906/j.cnki.JFCT.2022061
基金项目: 国家重点研发计划(2019YFD1100602),国家自然科学基金(52176192),山东省自然科学基金(ZR2021ME035,ZR2021QE132)资助
详细信息
    通讯作者:

    Tel:18678191880,E-mail:lizhihe@sdut.edu.cn

  • 中图分类号: TK6

Research progress on catalytic reforming of bio-oil and its derivatives for hydrogen production

Funds: The project was supported by National key research and development program (2019YFD1100602), National Natural Science Foundation of China (52176192) and Shandong Provincial Natural Science Foundation (ZR2021ME035,ZR2021QE132).
  • 摘要: 氢气作为最理想的清洁能源之一,在石油、化工、冶金、石化、食品和化肥工业等行业中发挥着重要作用。生物油水蒸气催化重整制氢作为一种具有发展前景且经济可行的绿色制氢技术,近些年来受到了研究者广泛关注。本文对近年来该领域的研究进展进行综述,重点分析了生物油(生物原油、水相生物油以及重质生物油/焦油)、生物油模型化合物(羧酸类、醇类、酚类等)和其他生物油衍生物的催化重整产氢过程,包括其在重整反应机理、重整工艺以及催化剂等方面的研究进展。对多种混合模化物以及真实生物油催化重整反应机理的深入探究是目前研究的主要难点,研制节能、高效的催化重整反应器以及开发稳定、高活性的重整催化剂是目前乃至今后生物油催化重整制氢领域研究和推广的重点。
  • 图  1  生物原油(左)、水相生物油(中)以及重质生物油(右)

    Figure  1  Biocrude oil (left), aqueous bio-oil (middle) and heavy bio-oil (right)

    图  2  水相生物油原位汽化-催化重整制氢(a)固定床/(b)流化床反应装置[22]

    Figure  2  In-situ vaporization-catalytic reforming of aqueous bio-oil for hydrogen production (a) fixed bed/ (b) fluidized bed reactor

    图  3  共沉淀法制备钛改性催化剂催化乙酸反应机理(下)[38]

    Figure  3  Mechanism of titanium-modified catalyst prepared by co-precipitation method for acetic acid reaction

    图  4  甲醇水蒸气重整的反应路径[50]

    Figure  4  Reaction pathways of steam reforming of methanol.

    图  5  Ni/Al2O3催化剂上乙醇水蒸气重整机理示意图[51]

    Figure  5  Schematic diagram of steam reforming mechanism of ethanol over Ni/Al2O3 catalyst

    Note: Blue balls indicate Al2O3 support, red balls Ni particles, * indicates free radicals, solid lines indicate strong chemical bonds, dashed lines indicate the interaction between catalyst and intermediate species.

    图  6  (a)TiO2水蒸气重整反应中苯酚的吸附模式机理;(b)Ni/TiO2水蒸气重整反应过程中苯酚的吸附模式机理[65]

    Figure  6  (a) The adsorption mode mechanism of phenol in the TiO2 steam reforming reaction; (b) the adsorption mode mechanism of phenol in the Ni/TiO2 steam reforming reaction process

    图  7  水相生物油催化重整的触发机理及积炭形成路径[73]

    Figure  7  Triggering mechanism and coke formation pathway of aqueous bio-oil catalytic reforming

    Note: White balls represent H atoms, red are O atoms, and gray balls are C atoms

    表  1  生物油水蒸气催化重整过程中反应方程式

    Table  1  Reaction equations during steam catalytic reforming of bio-oil

    Reaction nameReaction equation
    Steam reforming reaction${\text{C} }_{\text{n} }{\text{H} }_{\text{m} }{\text{O} }_{\text{k} } \text{ + } \left(\text{n}-\text{k}\right){\text{H} }_{\text{2} }\text{O}\to \mathrm{n}\text{CO} + \left(\text{n + }\dfrac{\text{m} }{\text{2} }-\text{k}\right){\text{H} }_{\text{2} }$(1)
    WGS$ \text{CO}\text{}\text{ + }\text{}{\text{H}}_{\text{2}}\text{O}\text{}\text{→}\text{}\text{C}{\text{O}}_{\text{2}}\text{}\text{ + }\text{}{\text{H}}_{\text{2}} $(2)
    Overall reaction${\text{C} }_{\text{n} }{\text{H} }_{\text{m} }{\text{O} }_{\text{k} }\text{ + }\left(\text{2n}-\text{k}\right){\text{H} }_{\text{2} }\text{O}\text{}\text{→}\text{}\text{nC}{\text{O} }_{\text{2} }\text{ + }\left(\text{2n }\text{ + }\dfrac{\text{m} }{\text{2} }-\text{k}\right){\text{H} }_{\text{2} }$(3)
    Methane decomposition reaction$ \text{C}{\text{H}}_{\text{4}}\text{}\text{→}\text{}\text{2}{\text{H}}_{\text{2}}\text{ + }\text{C} $(4)
    Methane reforming$ \text{C}{\text{H}}_{\text{4}}\text{ + }{\text{}\text{H}}_{\text{2}}\text{O}\text{}\text{→}\text{}\text{3}{\text{H}}_{\text{2}}\text{ + }\text{CO} $(5)
    Carbon gasification reaction$ \text{C}\text{ + }{\text{H}}_{\text{2}}\text{O}\text{}\text{→}\text{}\text{CO}\text{ + }{\text{H}}_{\text{2}} $(6)
    Thermal cracking reaction$ {\text{C}}_{\text{n}}{\text{H}}_{\text{m}}{\text{O}}_{\text{k}}\to {\text{C}}_{\text{a}}{\text{H}}_{\text{b}}{\text{O}}_{\text{c}} + $gases ($ {\text{H}}_{\text{2}}\text{,} $ $ {\text{H}}_{\text{2}}\text{O,CO,}\text{C}{\text{O}}_{\text{2}}\text{,}\cdots $) $ \text{ + } $ cokes(7)
    Boudouard reaction$ \text{2CO}\text{}\text{→}\text{}\text{C}{\text{O}}_{\text{2}}\text{ + }\text{C} $(8)
    Methanation reaction$ \text{CO}\text{ + }\text{3}{\text{H}}_{\text{2}}\text{}\text{→}\text{}\text{C}{\text{H}}_{\text{4}}\text{ + }{\text{H}}_{\text{2}}\text{O} $
    $ \text{C}{\text{O}}_{\text{2}}\text{ + }\text{4}{\text{H}}_{\text{2}}\text{}\text{→}\text{}\text{C}{\text{H}}_{\text{4}}\text{ + }\text{2}{\text{H}}_{\text{2}}\text{O} $
    (9)
    下载: 导出CSV

    表  2  阶梯Ni表面甲酸解离基本反应[36]

    Table  2  basic reaction of formic acid dissociation on stepped Ni surface

    StepsReaction equation
    R1HCOO→HCOO + H(10)
    R2HCOOH→HCO + OH(11)
    R3HCOOH→COOH + H(12)
    R4HCOOH→HCOH + O(13)
    R5HCOO→HCO + O(14)
    R6HCOO→HCOH + O(15)
    R7HCOO→CO2 + O(16)
    R8HCO→HCO + H(17)
    R9COOH→CO + OH(18)
    R10COOH→trans-COOH(19)
    R11trans-COOH→CO2 + H(20)
    R12H + H→HCOH + O(21)
    R13HCOOH→H2(22)
    R14O + H→OH(23)
    Notes: 1. All intermediates are located on the Ni surface. 2. Except for R12 and R13, all other reactions are reversible.
    下载: 导出CSV

    表  3  生物油模化物的水蒸气催化重整

    Table  3  Steam catalytic reforming of bio-oil model compound

    Bio-oil modelCatalystT(℃)Space timeS/C ratioX(%)YH2Ref
    Acetic acidNi-TiS/ATP60028.6 h−1393.477.6%[38]
    Acetic acidNi/CaFe2O46003.4 h−15-92.1%[44]
    MethanolCeCuZn/CNTs3007.5 h−1294.298.2%[53]
    MethanolCeO2-Cu/KIT-63002 h−1-9699.8%[56]
    EthanolNiMo/SBA-156001.5 ml/h29050%[58]
    EthanolCa-Ni/sepiolite70059.5 h−11.59565%[59]
    GlycerinCo-La-Ni/Al2O36002 h−1< 388.2384.3%[63]
    PhenolNi-Co/CaO-Ca12Al14O33650-382.232.31 L/g[67]
    PhenolNi/ZrO26500.36 ml/min-75.980.7%[72]
    TolueneNi/Perovskite-CaO6504500 h−1275%[71]
    FurfuralNi/Al2O380010 h−112.859570%[72]
    Ethyl acetateNi/Al2O380010 h−110-120 ml/min[73]
    HydroxyacetoneNi/Al2O380010 h−110-165 ml/min[73]
    Ethylene GlycolNi/Al2O380010 h−110-240 ml/min[73]
    2-MethoxyphenolNi/Al2O380010 h−157.89-50 ml/min[73]
    LevoglucosanNi/Al2O380010 h−110-135 ml/min[73]
    Notes: S/C ratio is steam to carbon ratio. X is the reforming conversion. YH2 is hydrogen yield.
    下载: 导出CSV
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  • 收稿日期:  2022-06-02
  • 录用日期:  2022-07-14
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