Chemical Recycling of Carbon Dioxide to Methanol and Dimethyl Ether: From Greenhouse Gas to Renewable, Environmentally Carbon Neutral Fuels and Synthetic Hydrocarbons

Loker Hydrocarbon Research Institute and Department of Chemistry, University of Southern California, University Park, Los Angeles, California 90089-1661, USA.
The Journal of Organic Chemistry (Impact Factor: 4.72). 01/2009; 74(2):487-98. DOI: 10.1021/jo801260f
Source: PubMed


Nature's photosynthesis uses the sun's energy with chlorophyll in plants as a catalyst to recycle carbon dioxide and water into new plant life. Only given sufficient geological time can new fossil fuels be formed naturally. In contrast, chemical recycling of carbon dioxide from natural and industrial sources as well as varied human activities or even from the air itself to methanol or dimethyl ether (DME) and their varied products can be achieved via its capture and subsequent reductive hydrogenative conversion. The present Perspective reviews this new approach and our research in the field over the last 15 years. Carbon recycling represents a significant aspect of our proposed Methanol Economy. Any available energy source (alternative energies such as solar, wind, geothermal, and atomic energy) can be used for the production of needed hydrogen and chemical conversion of CO(2). Improved new methods for the efficient reductive conversion of CO(2) to methanol and/or DME that we have developed include bireforming with methane and ways of catalytic or electrochemical conversions. Liquid methanol is preferable to highly volatile and potentially explosive hydrogen for energy storage and transportation. Together with the derived DME, they are excellent transportation fuels for internal combustion engines (ICE) and fuel cells as well as convenient starting materials for synthetic hydrocarbons and their varied products. Carbon dioxide thus can be chemically transformed from a detrimental greenhouse gas causing global warming into a valuable, renewable and inexhaustible carbon source of the future allowing environmentally neutral use of carbon fuels and derived hydrocarbon products.

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    • "Among valuable products produced by utilizing the captured CO 2 (CCU), methanol (MeOH) has received growing interests in literature. The significance of MeOH synthesis in CCU process was comprehensively discussed by Olah and Goeppert [4] "
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    ABSTRACT: This paper explores a possible ‘methanol economy’ transition strategy—a novel carbon capture and utilization (CCU) configuration for methanol (MeOH) production (CCU–MeOH). In this CCU–MeOH, the captured CO2 is co-fed with natural gas (NG) to produce syngas suitable for MeOH synthesis. The main objective of this work is to compare two aspects, namely CO2 emission intensity and the extent of methane reliance, of six CCU–MeOH scenarios derived from four reforming methodologies (steam methane reforming (SMR), dry methane reforming (DMR), bireforming and trireforming). Among the studied CCU–MeOH scenarios, Scenario 2 (DMR with H2 addition) significantly outperformed the other scenarios by 12.7% and 22% on average in terms of CO2 emission intensity and methane reliance, respectively. The outperformance of Scenario 2 in CO2 emission intensity is found to originate from a 22% reduction in CH4 consumption on average compared to the other scenarios. In intermediate term, Scenario 2 may provide an attractive option for transitioning into ‘methanol economy’ of the future
    International Journal of CO2 Utilization 08/2015; DOI:10.1016/j.jcou.2015.07.001 · 3.09 Impact Factor
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    • "The energy requirements for the production of such renewable fuels depend on the methods that are used to capture CO 2 and to produce hydrogen. In a recent survey of their work, Olah et al. have stated: "Carbon dioxide can be chemically transformed from a detrimental greenhouse gas causing global warming into a valuable, renewable and inexhaustible carbon source of the future allowing environmentally neutral use of carbon fuels and derived hydrocarbon products" [6]. "
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    ABSTRACT: The photocatalytic reduction of CO2 with water vapour and catalysts under UV irradiation to yield hydrocarbons is a potential way of decreasing greenhouse gas and it represents an attractive alternative energy source to fossil fuels. However, this process still has to overcome several hurdles, because it involves the activation of two stable molecules, H2O and CO2, and simultaneous conversion through a multi-step electron transfer reaction. The problem of CO2 emission and the possibility of exploiting CO2 as a raw material reaction is first reported in this short review. Subsequently, the fundamentals of photocatalysis are described. Finally, TiO2-based photocatalysts are reviewed, taking into consideration the optimization methods that can be adopted to improve performances. The information gained from this analysis will help to contribute towards a better understanding of the main parameters that affect the activity of photocatalysts and will ultimately lead to the optimized synthesis of more efficient photocatalytic material for the photocatalytic reduction of CO2 to fuels.
    11/2014; 1(2):16-25. DOI:10.15379/2408-9834.2014.01.02.03
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    • "As one of the important raw materials for organic chemical industry, methanol has been widely applied in the preparation of varieties of chemicals including formaldehyde, dimethyl ether and ethanediol [1]. With the amounts of fossil fuels available to us are gradually depleting, the use of methanol is an alternative way for us as prospective energy. "
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    ABSTRACT: Syngas production by CO2 reforming of coke oven gas (COG) was studied in a fixed-bed reactor over Ni/La2O3-ZrO2 catalysts. The catalysts were prepared by sol-gel technique and tested by XRF, BET, XRD, H2-TPR, TEM and TG-DSC. The influence of nickel loadings and calcination temperature of the catalysts on reforming reaction was measured. The characterization results revealed that all of the catalysts present excellent resistance to coking. The catalyst with appropriate nickel content and calcination temperature has better dispersion of active metal and higher conversion. It is found that the Ni/La2O3-ZrO2 catalyst with 10 wt% nickel loading provides the best catalytic activity with the conversions of CH4 and CO2 both more than 95% at 800°C under the atmospheric pressure. The Ni/La2O3-ZrO2 catalysts show excellent catalytic performance and anti-carbon property, which will be of great prospects for catalytic CO2 reforming of COG in the future. © 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
    International Journal of Hydrogen Energy 10/2014; 39(32):18650-18658. DOI:10.1016/j.ijhydene.2014.02.029 · 3.31 Impact Factor
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