Kinetics of CoCu/SiO2 for synthesis of lower carbon mixed alcohols directly from syngas

doi:10.3969/j.issn.0438-1157.2014.01.018

CIESC Journal ›› 2014, Vol. 65 ›› Issue (1): 143-151.DOI: 10.3969/j.issn.0438-1157.2014.01.018

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Kinetics of CoCu/SiO₂ for synthesis of lower carbon mixed alcohols directly from syngas

SU Junjie, MAO Wei, YANG Zhen, XU Jing, HAN Yifan

State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China

Received:2013-07-01 Revised:2013-11-03 Online:2014-01-05 Published:2014-01-05
Supported by:
supported by the National Natural Science Foundation of China (21176071, 21106041, 21273070） and Shanghai Pujiang Talent Program (2011/11PJ1402400).

CoCu/SiO₂催化剂用于合成气直接制备低碳混合醇的动力学

苏俊杰, 茅威, 杨震, 徐晶, 韩一帆

华东理工大学化学工程联合国家重点实验室, 上海 200237

通讯作者: 韩一帆
作者简介:苏俊杰（1990-），男，博士研究生。
基金资助:
国家自然科学基金项目（21176071，21106041，21273070）；上海市浦江人才计划项目（2011/11PJ1402400）。

Abstract

Abstract: Synthesis of lower carbon mixed alcohols directly from syngas is one of the most promising approaches for utilizing coal resources cleanly and efficiently. The intrinsic kinetics for this reaction, in which the effects of internal and external diffusion had been excluded, was studied over CoCu/SiO₂ catalysts prepared by the impregnation method in a fixed-bed reactor at 503—543 K with molar ratios of H₂/CO varying from 4 to 0.5. The apparent activation energies and the reaction orders with respect to H₂ and CO for products were calculated through power law models. With the combination of chain growth probability and kinetics, the effect of temperature on reaction mechanism was discussed.

Key words: kinetics, carbon monoxide, hydrogenation, lower alcohols, CoCu/SiO₂, syngas

摘要： 由合成气直接制取低碳混合醇是洁净高效利用煤炭资源的最佳途径之一。通过浸渍法制备了CoCu/SiO₂催化剂，采用固定床反应器，排除了内外扩散影响，在反应温度为503～543 K，H₂与CO的比值为4～0.5条件下，对合成气直接制取低碳混合醇反应进行了本征动力学研究。使用幂函数速率模型对反应结果进行了拟合，计算得出各产物的反应活化能以及对应的H₂和CO的反应级数。最后结合碳链增长可能性的变化，讨论了不同温度对CoCu/SiO₂催化剂催化合成气直接制备低碳醇反应机理的影响。

关键词: 动力学, 一氧化碳, 加氢, 低碳醇, CoCu/SiO₂, 合成气

CLC Number:

O643.1

SU Junjie, MAO Wei, YANG Zhen, XU Jing, HAN Yifan. Kinetics of CoCu/SiO₂ for synthesis of lower carbon mixed alcohols directly from syngas[J]. CIESC Journal, 2014, 65(1): 143-151.

苏俊杰, 茅威, 杨震, 徐晶, 韩一帆. CoCu/SiO₂催化剂用于合成气直接制备低碳混合醇的动力学[J]. 化工学报, 2014, 65(1): 143-151.

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Kinetics of CoCu/SiO₂ for synthesis of lower carbon mixed alcohols directly from syngas

CoCu/SiO₂催化剂用于合成气直接制备低碳混合醇的动力学

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