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

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: 5 January 2018
Revised Date: 29 January 2018
Accepted Date: 29 January 2018
Available Online: 6 August 2018
Fund Project: the State Key Laboratory of Organic-Inorganic Composites, China oic-201503005Fundamental Research Funds for the Central Universities, China buctrc201525The 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)Beijing National Laboratory for Molecular Sciences, China BNLMS20160133

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.
- CO₂ hydrogenation,
- Heterogeneous catalysis,
- C₂₊ species
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