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焙烧温度对Ru/CeO2催化剂在高通量甲醇水蒸气重整制氢反应中催化性能的影响
Effects of calcination temperature on catalytic performance of Ru/CeO2 catalysts for hydrogen production by high flux steam reforming of methanol
- 低碳化学与化工 2025, 50(3): 23-29.
- 作者机构：
1.辽宁石油化工大学 石油化工学院，辽宁 抚顺 113001
2.抚顺职业技术学院 化学工程系，辽宁 抚顺 113122
- 作者简介：
李佳祺（2003—），本科生，研究方向为氢能与催化，E-mail：3285349434@qq.com。
张磊（1983—），博士，教授，研究方向为氢能与催化，E-mail：lnpuzhanglei@163.com。
- 基金信息：国家自然科学基金(22379059);辽宁省应用基础研究计划(2023JH2/101300224);辽宁省教育厅服务地方项目（揭榜挂帅）(LJKFZ20220201);辽宁省教育厅面上项目(LJKMZ20220728);辽宁石油化工大学引进人才科研启动基金资助项目(2019-XJJL-028);天津市京津冀协同创新项目(22PTXTHZ00020);大学生创新创业训练计划(S202310148038)
DOI：10.12434/j.issn.2097-2547.20240285
中图分类号： TQ116.2收稿日期：2024-07-03，
修回日期：2024-08-20，
纸质出版日期：2025-03-25
- 稿件说明：
移动端阅览
李佳祺,刘明新,初奇瑞等.焙烧温度对Ru/CeO2催化剂在高通量甲醇水蒸气重整制氢反应中催化性能的影响[J].低碳化学与化工,2025,50(03):23-29.
LI Jiaqi,LIU Mingxin,CHU Qirui,et al.Effects of calcination temperature on catalytic performance of Ru/CeO2 catalysts for hydrogen production by high flux steam reforming of methanol[J].Low-carbon Chemistry and Chemical Engineering,2025,50(03):23-29.
李佳祺,刘明新,初奇瑞等.焙烧温度对Ru/CeO2催化剂在高通量甲醇水蒸气重整制氢反应中催化性能的影响[J].低碳化学与化工,2025,50(03):23-29. DOI： 10.12434/j.issn.2097-2547.20240285.
LI Jiaqi,LIU Mingxin,CHU Qirui,et al.Effects of calcination temperature on catalytic performance of Ru/CeO2 catalysts for hydrogen production by high flux steam reforming of methanol[J].Low-carbon Chemistry and Chemical Engineering,2025,50(03):23-29. DOI： 10.12434/j.issn.2097-2547.20240285.
摘要
高效催化剂的研制是高通量甲醇水蒸气重整制氢反应的关键技术之一。以RuCl
3
为原料、CeO
2
为载体，采用沉积-沉淀法制备了Ru/CeO
2
催化剂，通过XRD、N
2
吸/脱附、H
2
-TPR和XPS等对催化剂性质进行了分析，并考察了焙烧温度对催化剂在高通量甲醇水蒸气重整制氢反应中催化性能的影响。结果表明，随焙烧温度的升高，RuO
x
物种的还原性能先变强后变弱，表面氧空位相对含量先升高后降低。其中，Ru/CeO
2
-500催化剂中RuO
x
物种的还原性能较强，催化剂表面氧空位相对含量较高，催化活性较好。在反应温度为420 ℃、水醇物质的量比为1.2:1.0和甲醇水质量空速为6.0 h
-1
的条件下，Ru/CeO
2
-500催化剂的甲醇转化率为91.8%。
Abstract
The development of high efficiency catalyst is one of the key technologies of hydrogen production by high flux steam reforming of methanol. Using RuCl
3
as raw material and CeO
2
as support
Ru/CeO
2
catalysts were prepared by deposition-precipitation method. The properties of the catalysts were analyzed by XRD
N
2
adsorption/desorption
H
2
-TPR and XPS
and the effect of calcination temperature on the catalytic performance of the catalysts in high flux steam reforming of methanol for hydrogen production was investigated. The results show that with the increase of calcination temperature
the reducing performance of RuO
x
species increases first and then decreases
and the surface oxygen vacancy relative content increases first and then decreases. Among them
RuO
x
species in Ru/CeO
2
-500 catalyst have stronger reducing performance
higher surface oxygen vacancy relative content on the catalyst surface
and bett
er catalytic activity. The methanol conversion rate of Ru/CeO
2
-500 catalyst is 91.8% under the conditions of reaction temperature of 420 ℃
mole ratio of water and alcohol of 1.2:1.0 and weight hourly space velocity of methanol and water of 6.0 h
-1
.
关键词
Keywords
references
JACOBSON M Z , COLELLA W G , GOLDEN D M . Cleaning the air and improving health with hydrogen fuel-cell vehicles [J ] . Science , 2005 , 308 ( 5730 ): 1901 - 1905 .
KALINCI Y , DINCER I , HEPBASLI A . Energy and exergy analyses of a hybrid hydrogen energy system: A case study for Bozcaada [J ] . International Journal of Hydrogen Energy , 2016 , 42 ( 4 ): 2492 - 2503 .
ZHANG F , ZHAO P C , NIU M , et al . The survey of key technologies in hydrogen energy storage [J ] . International Journal of Hydrogen Energy , 2016 , 41 ( 33 ): 14535 - 14552 .
周君 , 安娟 , 杨宽辉 , 等 . 现代能源体系耦合绿氢化工应用的研究进展 [J ] . 低碳化学与化工 , 2023 , 48 ( 4 ): 46 - 54 .
ZHOU J , AN J , YANG K H , et al . Research progresses in application of modern energy system coupled with green hydrogen chemical industry [J ] . Low-Carbon Chemistry and Chemical Industry , 2023 , 48 ( 4 ): 46 - 54 .
隋朝霞 , 付亚轩 , 张丹 . 国内煤制天然气产业发展现状与趋势分析 [J ] . 低碳化学与化工 , 2024 , 49 ( 3 ): 129 - 136 .
SUI Z X , FU Y X , ZHANG D . Analysis of current situation and trends in development of coal-based synthetic natural gas industry in China [J ] . Low-Carbon Chemistry and Chemical Industry , 2024 , 49 ( 3 ): 129 - 136 .
SHIH C F , ZHANG T , LI J H , et al . Powering the future with liquid sunshine [J ] . Joule , 2018 , 2 ( 10 ): 1925 - 1949 .
FREI M S , MONDELLI C , SHORT M I M , et al . Methanol as a hydrogen carrier: Kinetic and thermodynamic drivers for its CO 2 -based synthesis and reforming over heterogeneous catalysts [J ] . ChemSusChem , 2020 , 13 ( 23 ): 6330 - 6337 .
FILOSA C , GONG X , BAVYKINA A , et al . Enabling the methanol economy: Opportunities and challenges for heterogeneous catalysis in the production of liquid fuels via methanol [J ] . Accounts of Chemical Research , 2023 , 56 ( 23 ): 3492 - 3503 .
张磊 , 潘立卫 , 倪长军 , 等 . 沉淀温度对CuO/ZnO/CeO 2 /ZrO 2 甲醇水蒸气重整制氢催化剂性能的影响 [J ] . 催化学报 , 2012 , 33 ( 12 ): 1958 - 1964 .
ZHANG L , PAN L W , NI C J , et al . Effect of precipitation temperature on the performance of CuO/ZnO/CeO 2 /ZrO 2 catalyst for methanol steam reforming [J ] . Journal of Catalytic Chemistry , 2012 , 33 ( 12 ): 1958 - 1964 .
邢月 , 杨劭杰 , 曹利星 , 等 . 甲醇水蒸气重整制氢CuO-ZnO/CeO 2 催化剂的制备及性能 [J ] . 石油化工 , 2022 , 51 ( 9 ): 1011 - 1016 .
XING Y , YANG S J , CAO L X , et al . Preparation and performance of CuO-ZnO/CeO 2 catalyst for producing hydrogen via methanol steam reforming [J ] . Petrochemical , 2022 , 51 ( 9 ): 1011 - 1016 .
QIAO W J , ZHANG L , ZHANG K W , et al . Low temperature synthesis of Cu 1- x Al 2.5 spinel solid solution as sustained release catalyst for metha nol to hydrogen [J ] . International Journal of Hydrogen Energy , 2022 , 47 ( 75 ): 32133 - 32144 .
HE J P , YANG Z X , ZHANG L , et al . Cu supported on ZnAl-LDHs precursor prepared by in-situ synthesis method on γ -Al 2 O 3 as catalytic material with high catalytic activity for methanol steam reforming [J ] . International Journal of Hydrogen Energy , 2017 , 42 ( 15 ): 9930 - 9937 .
YANG S Q , ZHOU F , LIU Y J , et al . Morphology effect of ceria on the performance of CuO/CeO 2 catalysts for hydrogen production by methanol steam reforming [J ] . International Journal of Hydrogen Energy , 2019 , 44 ( 14 ): 7252 - 7261 .
QIAO W J , YANG S Q , ZHANG L , et al . Performance of Cu-Ce/M - Al (M = Mg, Ni, Co, Zn) hydrotalcite derived catalysts for hydrogen production from methanol steam reforming [J ] . Energy Research , 2021 , 45 ( 9 ): 12773 - 12783 .
ARAIZA D G , GOMEZ-CORTES A , DIAZ G . Partial oxidation of methanol over copper supported on nanoshaped ceria for hydrogen production [J ] . Catalysts Today , 2017 , 282 : 185 - 194 .
TSONCHEVA T , GENOVA I , DIMITROV M , et al . Nanostructured copper-zirconia composites as catalysts for methanol decomposition [J ] . Applied Catalysis B: Environmental , 2015 , 165 : 599 - 610 .
张庆生 , 黄雪松 . 国内外氢能产业政策与技术经济性分析 [J ] . 低碳化学与化工 , 2023 , 48 ( 2 ): 133 - 139 .
ZHANG Q S , HUANG X S . Analysis of domestic and foreign hydrogen energy industrial policies and technical economy [J ] . Low-Carbon Chemistry and Chemical Engineering , 2023 , 48 ( 2 ): 133 - 139 .
ZHANG L , PAN L W , NI C J , et al . CeO 2 -ZrO 2 -promoted CuO/ZnO catalyst for methanol steam reforming [J ] . International Journal of Hydrogen Energy . 2013 , 38 ( 11 ): 4397 - 4406 .
焦桐 , 许雪莲 , 张磊 , 等 . CuO/CeO 2 -ZrO 2 /SiC整体催化剂催化甲醇水蒸气重整制氢的研究 [J ] . 化学学报 , 2021 , 79 ( 4 ): 513 - 519 .
JIAO T , XU X L , ZHANG L , et al . Research on CuO/CeO 2 -ZrO 2 /SiC monolithic catalysts for hydrogen production by methanol steam reforming [J ] . Acta Chimica Sinica , 2021 , 79 ( 4 ): 513 - 519 .
XING Y , WU J X , ZHANG C S , et al . Mn-induced Cu/Ce catalysts with improved performance for CO preferential oxidation in H 2 /CO 2 -rich streams [J ] . International Journal of Hydrogen Energy , 2023 , 48 ( 54 ): 20667 - 20679 .
陈海波 , 刘明 , 李晓敏 , 等 . 分步沉淀法制备铜锌基甲醇合成催化剂及其性能研究 [J ] . 低碳化学与化工 , 2024 , 49 ( 5 ): 8 - 14 .
CHEN H B , LIU M , LI X M , et al . Preparation of copper-zinc based methanol catalysts synthesized by stepwise precipitation method and their performance study [J ] . Low-Carbon Chemistry and Chemical Engineering , 2024 , 49 ( 5 ): 8 - 14 .
武嘉欣 , 韩蛟 , 李学 , 等 . CO优先氧化反应MnCu/Ce催化剂的制备及性能 [J ] . 燃料化学学报（中英文） , 2024 , 52 ( 4 ): 565 - 576 .
WU J X , HAN J , LI X , et al . Preparation and properties of MnCu/Ce catalyst for CO preferential oxidation reaction [J ] . Journal of Fuel Chemistry and Technology , 2024 , 52 ( 4 ): 565 - 576 .
张楷文 , 刘鑫尧 , 张磊 , 等 . 甲醇水蒸气重整制氢Cu-Zn-Al尖晶石催化剂的研究 [J ] . 燃料化学学报 , 2022 , 50 ( 4 ): 494 - 502 .
ZHANG K W , LIU X Y , ZHANG L , et al . Cu-Zn-Al spinel catalyst for hydrogen production from methanol steam reforming [J ] . Journal of Fuel Chemistry and Technology , 2022 , 50 ( 4 ): 494 - 502 .
安国超 , 孙舒 , 焦桐 , 等 . 焙烧温度对甲醇水蒸气重整制氢CuO/CeO 2 -ZrO 2 /SiC整体催化剂的影响 [J ] . 化学工业与工程 , 2023 , 40 ( 6 ): 53 - 58 .
AN G C , SUN S , JIAO T , et al . Effect of calcination temperature on CuO/CeO 2 -ZrO 2 /SiC monolithic catalyst for hydrogen production by methanol steam reforming [J ] . Chemical Industry & Engineering , 2023 , 40 ( 6 ): 53 - 58 .
匡浩浩 , 蒋艳刚 , 马海乐 , 等 . Pd基催化剂载体对天然气催化燃烧影响的研究进展 [J ] . 低碳化学与化工 , 2024 , 49 ( 4 ): 12 - 22+43 .
KUANG H H , JIANG Y G , MA H L , et al . Research progress on influence of Pd-based catalyst supports on natural gas catalytic combustion [J ] . Low-Carbon Chemistry and Chemical Engineering , 2024 , 49 ( 4 ): 12 - 22+43 .
CHEN L N , QI Z Y , PENG X X , et al . Insights into the me chanism of methanol steam reforming tandem reaction over CeO 2 supported single-site catalysts [J ] . Journal of the American Chemical Society , 2021 , 143 ( 31 ): 12074 - 12081 .
卢畅 , 张财顺 , 刘道胜 , 等 . CuO-SiO 2 -CeO 2 催化剂的设计、制备及性能研究 [J ] . 石油化工高等学校学报 , 2022 , 35 ( 1 ): 29 - 34 .
LU C , ZHANG C S , LIU D S , et al . Design, preparation and performance of CuO-SiO 2 -CeO 2 catalyst [J ] . Journal of University of Petroleum and Chemical Engineering , 2022 , 35 ( 1 ): 29 - 34 .
范长帅 , 丁传敏 , 宋清文 , 等 . 焙烧气氛对棒状CeO 2 催化CO 2 和甲醇直接合成DMC的影响 [J ] . 低碳化学与化工 , 2024 , 49 ( 7 ): 104 - 110+119 .
FAN C S , DING C M , SONG Q W , et al . Effect of calcination atmospheres on direct synthesis of DMC from CO 2 and methanol catalyzed by rod-like CeO 2 [J ] . Low-Carbon Chemistry and Chemical Engineering , 2024 , 49 ( 7 ): 104 - 110+119 .
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