纳米铁基催化剂在CO<sub>2</sub>加氢制烃中的性能

引用本文: 郑斌, 张安峰, 刘民, 丁凡舒, 代成义, 宋春山, 郭新闻. 纳米铁基催化剂在CO₂加氢制烃中的性能[J]. 物理化学学报, 2012, 28(08): 1943-1950. doi: 10.3866/PKU.WHXB201206051 shu

Citation: ZHENG Bin, ZHANG An-Feng, LIU Min, DING Fan-Shu, DAI Cheng-Yi, SONG Chun-Shan, GUO Xin-Wen. Properties of the Nano-Particle Fe-based Catalyst for the Hydrogenation of Carbon Dioxide to Hydrocarbons[J]. Acta Physico-Chimica Sinica, 2012, 28(08): 1943-1950. doi: 10.3866/PKU.WHXB201206051 shu

纳米铁基催化剂在CO₂加氢制烃中的性能

郑斌 ^1, ,
张安峰 ^1, ,
刘民 ^1, ,
丁凡舒 ^1, ,
代成义 ^1, ,
宋春山 ^1,2, ,
郭新闻 ^1,

摘要:

使用尿素沉淀凝胶、机械混合和等体积浸渍相结合的方法, 制备了一系列的纳米尺寸FeK-M/γ-Al₂O₃(M=Cd, Cu)催化剂, 采用扫描电镜(SEM)、透射电镜(TEM)、N2物理吸附、X射线衍射(XRD)光谱和H₂程序升温还原(H₂-TPR)仪对催化剂进行表征, 并在小型固定床反应器上考察其对CO₂加氢反应的催化性能. 结果表明:3 MPa, 400 °C, 3600 h^-1, H₂/CO₂摩尔比为3 的条件下, 15%(w, 下同)Fe10%K/γ-Al₂O₃催化剂可稳定运行100h 以上, CO₂转化率为51.3%, C₂₊烃类的选择性达62.6%. Fe 含量降至2.5%时, C₂₊烃类的选择性仍能达到60.0%. 随着K含量由0%增加至10%, 低碳烯烃选择性增加, 烯烷比增加至3.6. Cd和Cu助剂可促进Fe 物种的还原, 改善目的产物的分布, 其中Cu的加入使低碳产物烯烷比增至5.4, Cd的加入使C₅₊产物选择性增加了12%.

关键词:

English

Properties of the Nano-Particle Fe-based Catalyst for the Hydrogenation of Carbon Dioxide to Hydrocarbons

1.
1. State Key Laboratory of Fine Chemicals, Department of Catalysis Chemistry and Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, P. R. China;
2. EMS Energy Institute and Department of Energy and Mineral Engineering, Pennsylvania State University, University Park, Pennsylvania, 16802, USA
Received Date: 10 March 2012
Available Online: 10 July 2012

Abstract:

Combining co-precipitation-gelation, mechanical mixing and impregnation methods, a series of catalysts of FeK-M/γ-Al₂O₃(M=Cd or Cu) have been attained. The catalysts were characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), N₂ physisorption, X-ray diffraction (XRD) and temperature-programmed reduction of hydrogen (H₂-TPR). The hydrogenation of carbon dioxide over these catalysts was also investigated in a fixed bed. Given a reaction time of 100 h, CO₂ conversion over a 15%Fe/10%K/γ-Al₂O₃ catalyst reached 51.3 %, with a selectivity towards C₂₊ of 62.6 % at 3 MPa, 673 K, a space velocity of 3600 h-1 and at a molar ratio of H₂/CO₂ of 3. At the lower Fe content of 2.5%, the selectivity towards C₂₊ was still greater than 60.0%. Increasing the potassium content from 0% to 10%, increased the selectivity towards C₂-C₄⁼ and the molar ratio of C₂-C₄⁼ /C₂-C₄⁰ increased to 3.6. The addition of Cd and Cu improved the reduction and catalytic activities. Specifically, Cu improved the molar ratio of C₂-C₄⁼ /C₂-C₄⁰ from 3.6 to 5.4, and the Cd increased the selectivity of C₅₊ by 12%.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

纳米铁基催化剂在CO₂加氢制烃中的性能

English

Properties of the Nano-Particle Fe-based Catalyst for the Hydrogenation of Carbon Dioxide to Hydrocarbons

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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English

Properties of the Nano-Particle Fe-based Catalyst for the Hydrogenation of Carbon Dioxide to Hydrocarbons

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs