Heterogeneous Catalysis of CO<sub>2</sub> Hydrogenation to C<sub>2+</sub> Products

Citation: GAO Yunnan, LIU Shizhen, ZHAO Zhenqing, TAO Hengcong, SUN Zhenyu. Heterogeneous Catalysis of CO₂ Hydrogenation to C₂₊ Products[J]. Acta Physico-Chimica Sinica, 2018, 34(8): 858-872. doi: 10.3866/PKU.WHXB201802061 shu

二氧化碳多相催化加氢制C₂及以上烃类和醇的研究进展

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北京化工大学，有机无机复合材料国家重点实验室，北京 100029

作者简介:

SUN Zhenyu is currently a full professor in the College of Chemical Engineering at Beijing University of Chemical Technology (China). He completed his Ph.D. in the Institute of Chemistry, Chinese Academy of Sciences in 2006. He did postdoctoral research in Trinity College Dublin (Ireland) from 2006 to 2008, at Ruhr University Bochum (Germany) from 2011 to 2014, and University of Oxford from 2015 to 2016. He has obtained a Humboldt Research Fellowship for Experienced Researchers (Germany). His current research focuses on energy conversion reactions using two-dimensional materials;

通讯作者: 孙振宇, sunzy@mail.buct.edu.cn

基金项目:
有机无机复合材料国家重点实验室人才培育资助项目 oic-201503005

北京化工大学引进人才经费 buctrc201525

有机无机复合材料国家重点实验室人才培育资助项目(oic-201503005), 北京化工大学引进人才经费(buctrc201525)和北京分子科学国家实验室开放课题基金(BNLMS20160133)资助项目

北京分子科学国家实验室开放课题基金 BNLMS20160133

摘要: 通过可再生能源得到的氢气将二氧化碳转化为高附加值的燃料和化学品，对于缓解全球变暖、改善生态环境和解决化石资源日益枯竭的难题具有重要的意义。通过加氢反应合成碳氢化合物，尤其是C₂₊烃类和含氧化合物愈来愈引起大家的研究兴趣。设计制备兼具二氧化碳活化和碳-碳键耦合的多功能催化剂仍然是一较大的挑战。本文总结了二氧化碳加氢合成长链烷烃、低碳烯烃、高级醇的最新研究进展，探讨了二氧化碳加氢所涉及的相关反应的热力学和动力学、反应机理和反应路径，并对现阶段报道的多相催化剂进行了归纳和分析，最后指出未来在二氧化碳加氢的多相催化过程中所面临的问题和发展方向。

关键词:

English

Heterogeneous Catalysis of CO₂ Hydrogenation to C₂₊ Products

State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, P. R. China

Author Bio: SUN Zhenyu is currently a full professor in the College of Chemical Engineering at Beijing University of Chemical Technology (China). He completed his Ph.D. in the Institute of Chemistry, Chinese Academy of Sciences in 2006. He did postdoctoral research in Trinity College Dublin (Ireland) from 2006 to 2008, at Ruhr University Bochum (Germany) from 2011 to 2014, and University of Oxford from 2015 to 2016. He has obtained a Humboldt Research Fellowship for Experienced Researchers (Germany). His current research focuses on energy conversion reactions using two-dimensional materials;

Corresponding author: SUN Zhenyu, sunzy@mail.buct.edu.cn

Received Date: 05 January 2018
Accepted Date: 29 January 2018
Revised Date: 29 January 2018
Available Online: 15 August 2018
Fund Project:

The project was supported by the State Key Laboratory of Organic-Inorganic Composites, China (oic-201503005), Fundamental Research Funds for the Central Universities, China (buctrc201525) and Beijing National Laboratory for Molecular Sciences, China (BNLMS20160133)

Abstract: The increasing anthropogenic emission of CO₂ leads to global warming, to address which three strategies can be considered: (1) decrease fossil fuel consumption through increased utilization efficiency and lower per capita consumption; (2) replace fossil fuels with renewable energy sources like wind, tidal, solar, and biomass energies; (3) utilize CO₂ efficiently. Despite efforts to reduce energy use and increase the use of carbon-neutral biofuels, it seems that fossil fuels will continue to be a major energy source for the next few decades. Tremendous effort is therefore being focused on developing effective technologies for CO₂ capture and transformation. In particular, the transformation of CO₂ into fuels and chemicals via reduction with renewable hydrogen is a promising strategy for mitigating global warming and energy supply problems. The hydrogenation of CO₂, especially to C₂₊ hydrocarbons and oxygenates, has sparked growing interest. The C₂₊ species can be used as entry platform chemicals for existing value chains, thus providing more advantages than C₁ compounds. However, optimizing catalyst design by integrating multifunctionalities for both CO₂ activation and C-C coupling remains an ongoing challenge. Here, we provide a timely review on the recent progress that has been made in the hydrogenation of CO₂ to higher-order alkanes, olefins, and alcohols by various heterogeneous catalysts. The thermodynamics and kinetics, as well as possible reaction pathways for CO₂ hydrogenation, are discussed. The hydrogenation of CO₂ to hydrocarbons usually involves the initial generation of CO via a reverse water-gas shift (RWGS) reaction followed by hydrogenation of the CO intermediate. The RWGS reaction proceeds through a redox route and an associative pathway. "CH_x" insertion (carbide-type) and "CO" insertion are two proposed mechanisms for this Fischer-Tropsch-like synthesis. Fe-or Co-based catalysts have been widely used to catalyze the hydrogenation of CO₂ to C₂₊ hydrocarbons via the CO intermediate. C₂₊ hydrocarbons can also be obtained by combining CH₃OH synthesis with the methanol-to-hydrocarbon process (MTH). This reaction pathway has been realized over bifunctional systems comprising a CH₃OH synthesis catalyst and an MTH catalyst. Alternatively, CO₂ hydrogenation can occur via a RWGS reaction to the CO intermediate, and subsequent formation of higher alcohols from syngas. Higher alcohols (mostly CH₃CH₂OH) have been produced by using a hybrid tandem catalyst. Understanding of the activation mechanism, precise C-C coupling, and synergy control between the two active components requires further research. In the final part, we describe the future challenges and opportunities in heterogeneous catalysis of CO₂ hydrogenation. The combination of calculations (precise theoretical models) and experiments (in-situ spectroscopic techniques) will facilitate the design of advanced catalysts to achieve both high CO₂ conversion and C₂₊ product selectivity.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

二氧化碳多相催化加氢制C₂及以上烃类和醇的研究进展

通讯作者: 孙振宇, sunzy@mail.buct.edu.cn

English

Heterogeneous Catalysis of CO₂ Hydrogenation to C₂₊ Products

Corresponding author: SUN Zhenyu, sunzy@mail.buct.edu.cn

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

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二氧化碳多相催化加氢制C2及以上烃类和醇的研究进展

通讯作者: 孙振宇, sunzy@mail.buct.edu.cn

English

Heterogeneous Catalysis of CO2 Hydrogenation to C2+ Products

Corresponding author: SUN Zhenyu, sunzy@mail.buct.edu.cn

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

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

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