ZnFe2O4-α-Fe2O3/SiC泡沫结构催化剂的制备和丁烯氧化脱氢性能

doi:10.11901/1005.3093.2017.320

材料研究学报

2018, Vol. 32

Issue (3): 225-232 DOI: 10.11901/1005.3093.2017.320

研究论文

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ZnFe₂O₄-α-Fe₂O₃/SiC泡沫结构催化剂的制备和丁烯氧化脱氢性能

姜仁政^1,², 矫义来¹, 孙博¹, 杨晓丹¹, 杨振明¹, 张劲松¹(

)

1 中国科学院金属研究所沈阳 110016;
2 中国科学院大学北京 100049;

Preparation of Foam Structured Catalyst ZnFe₂O₄-α-Fe₂O₃/SiC and its Performance in Oxidative Dehydrogenation of Butene

Renzheng JIANG^1,², Yilai JIAO¹, Bo SUN¹, Xiaodan YANG¹, Zhenming YANG¹, Jinsong ZHANG¹(

)

1 Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China;
2 University of Chinese Academy of Sciences, Beijing 100049, China;

引用本文:

姜仁政, 矫义来, 孙博, 杨晓丹, 杨振明, 张劲松. ZnFe₂O₄-α-Fe₂O₃/SiC泡沫结构催化剂的制备和丁烯氧化脱氢性能[J]. 材料研究学报, 2018, 32(3): 225-232.
Renzheng JIANG, Yilai JIAO, Bo SUN, Xiaodan YANG, Zhenming YANG, Jinsong ZHANG. Preparation of Foam Structured Catalyst ZnFe₂O₄-α-Fe₂O₃/SiC and its Performance in Oxidative Dehydrogenation of Butene[J]. Chinese Journal of Materials Research, 2018, 32(3): 225-232.

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摘要:

以柠檬酸-硝酸盐作为粘结剂用浆料涂覆法制备出ZnFe₂O₄-α-Fe₂O₃/SiC泡沫结构催化剂,使用X射线衍射(XRD)、扫描电镜(SEM)和N₂气吸附仪等手段表征其物相组成、形貌和结构,研究了柠檬酸-硝酸盐浓度和涂层负载量对结构催化剂涂层形貌、孔结构以及1-丁烯氧化脱氢性能的影响。结果表明,柠檬酸-硝酸盐对活性组分物相组成和比例没有影响;制得的结构催化剂涂层紧凑、平整,且具有较宽的介孔孔径分布;柠檬酸-硝酸盐的浓度和最可几孔径尺寸对结构催化剂性能的影响不大。随着涂层负载量的增加结构催化剂的比表面积逐渐增大,氧化脱氢性能逐渐提高。当涂层的负载量达到0.2 g/mL、丁烯体积空速为300 h^-1时丁烯转化率和丁二烯选择性分别达到86%和91%,明显高于颗粒催化剂,表现出优异的氧化脱氢性能。

关键词 ：无机非金属材料, ZnFe₂O₄-α-Fe₂O₃;, 泡沫SiC, 结构催化剂, 1-丁烯氧化脱氢, 浆料涂覆

Abstract：

A foam structured catalyst of ZnFe₂O₄-α-Fe₂O₃/SiC was prepared by a slurry-coating method with citric acid-nitrates as binder. Its phase composition, morphology and pore structure were characterized by XRD, SEM and BET. The influence of the concentration of citric acid-nitrates and the deposited amount of slurry on the morphology, pore structure and catalytic performance in the oxidative dehydrogenation of 1-butene of the prepared catalyst were investigated. The result show that the concentration of citric acid-nitrates hardly changed the phase composition; the as-prepared structured catalyst has a compact and neat coating with a wide range distribution of pore size; the concentration of citric acid-nitrates of the slurry or the most probable pore size of the as-prepared catalyst has a little influence on the peformance of the structured catalyst. The BET surface area and the catalytic performance of the structured catalyst gradually increased with the incresing the deposited amount of slurry. In case of gas firing hourly space velocity of bntene of 300 h^-1, the conversion rate of 1-butene and selectivity of butadiene reache ca. 86% and 91%, respectively for the prepared structured catalyst with a deposited amount of 0.2 g/mL slurry, which are much higher than that for particulate catalysts, indicating superior oxidative dehydrogenation performance.

Key words： inorganic non-metallic materials ZnFe₂O₄-α-Fe₂O₃; foam SiC structured catalyst 1-butene oxidative dehydrogenation slurry-coating

收稿日期: 2017-05-17

ZTFLH:

TQ031

作者简介:

作者简介姜仁政,男,1985年生,博士

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https://www.cjmr.org/CN/10.11901/1005.3093.2017.320 或 https://www.cjmr.org/CN/Y2018/V32/I3/225

图1 共沉淀ZF-0颗粒、ZF-0.11涂层颗粒、ZFS-0.2结构催化剂和泡沫SiC的XRD图谱

图2 泡沫SiC和ZFS-0.2结构催化剂的SEM照片

图3 ZFS-0.2结构催化剂的高倍和)低倍率照片a、b、c和d所对应的CNS浓度分别为0.11、0.44、0.88和1.32 mol/L

表1 ZF-c涂层颗粒的比表面积和孔容

图4 ZF-c涂层颗粒的孔径分布

图5 涂层载量不同的ZFS-w结构催化剂的筋表面照片

表2 ZFS-w结构催化剂的比表面积和孔容

图6 ZFS-w结构催化剂的孔径分布

图7 在不同反应条件下CNS浓度对ZFS-0.2结构催化剂性能的影响

图8 在不同反应条件下涂层负载量对ZFS结构催化剂性能的影响

图9 在不同反应条件下ZFS-0.2结构催化剂、ZF-0.11颗粒催化剂和ZF-0共沉淀颗粒催化剂的性能

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