Chemical Recycling of Carbon Dioxide to Methanol and Dimethyl
Ether: From Greenhouse Gas to Renewable, Environmentally
Carbon Neutral Fuels and Synthetic Hydrocarbons
George A. Olah,* Alain Goeppert, and G. K. Surya Prakash
Loker Hydrocarbon Research Institute and Department of Chemistry, UniVersity of Southern California,
UniVersity Park, Los Angeles, California 90089-1661
ReceiVed June 11, 2008
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 CO2. Improved new methods for the efficient
reductive conversion of CO2to 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.
A perspective article on the chemical recycling of carbon
dioxide may not be a usual topic for the Journal of Organic
Chemistry. It may be even questioned whether CO2recycling
would qualify as a topic for an organic chemistry journal.
However, CO2 is an ubiquitous carbon source allowing the
production of methanol and dimethyl ether, efficient alternative
transportation fuels, as well as their varied derived products.
The topic thus clearly falls into the scope of organic chemistry.
Copyright 2009 by the American Chemical Society
VOLUME 74, NUMBER 2January 16, 2009
10.1021/jo801260f CCC: $40.75 2009 American Chemical Society
Published on Web 12/08/2008
J. Org. Chem. 2009, 74, 487–498
Further, one of the major challenges of our time is to find
efficient new solutions beyond our diminishing fossil fuels
resources (oil, natural gas, coal) and the grave environmental
consequences of excessive combustion of carbon-containing
fuels and their products. The concept of the “Methanol
Economy” that we have developed hinges on the chemical
recycling of CO2to useful fuels. (i.e., methanol and DME) and
other products.1,2At the same time, it renders carbon-containing
fuels renewable (on the human time scale) and environmentally
neutral. This not only allows us to mitigate a major human made
cause of global warming but also provides us with an inexhaust-
ible and generally available carbon source for ages to come.
Introduction and Concept
Starting with coal and subsequently petroleum oil and natural
gas, fossil fuels allowed an unprecedented era of prosperity and
advancement for human development in the past two centuries.
The world still relies heavily today on fossil fuels to cover about
80% of its energy needs and to produce the vast multitude of
derived fuels and essential products. The amounts of fossil fuels
available to us are, however, finite and are rapidly depleting.
Once consumed, they are not renewed on the human time scale.
One of us (G.A.O.) has proposed some time ago the use of
methanol as an alternative way to store, transport, and use energy
(the so-called “Methanol Economy”).1,3-6Methanol and derived
dimethyl ether (DME) are also excellent fuels in internal
combustion engines (ICE) and in a new generation of direct
oxidation methanol fuel cells (DMFC), as well as convenient
starting materials for producing light olefins (ethylene and
propylene) and subsequently practically any derived hydrocar-
bon product. The “Methanol Economy”, detailed in our recent
monograph,2is capable of providing an environmentally carbon
neutral, or in some cases even carbon negative, alternative to
our diminishing oil and natural gas sources.1-3,5Methanol, as
discussed subsequently, can be efficiently produced from a wide
variety of sources including still available fossil fuels (coal, oil
shale, tar sands, etc.) by improved methods, but also from
agricultural products, municipal and industrial waste, wood, and
varied biomass. More importantly, as discussed in the present
perspective, methanol can also be produced in a new way from
chemical recycling of carbon dioxide. Initially, this will be
achieved from higher concentrations of CO2-rich flue gases of
fossil fuel burning power plants or exhausts of cement,
fermentation, and other industrial plants, aluminum and iron
ore smelters, etc. but also from major natural sources of CO2
such as those accompanying natural gas or geothermal hot water
and steam. In the future, however, even the low concentration
of CO2from our air, presently around 380 ppm, can be captured
and recycled to methanol, thus mimicking nature’s own
photosynthetic CO2cycle. Efficient new absorbents to capture
atmospheric CO2are being developed. Chemical recycling of
CO2 to new fuels and materials is thus becoming possible,
making them renewable on the human time scale. In contrast,
nature’s transformation of new plant life formed via photosyn-
thesis into fossil fuels may take many millions of years7for
which humankind cannot wait. Agricultural and natural product
based biofuels are increasingly produced and used. This requires,
however, at least in part shifting valuable food resources to fuel
production and has already resulted in sharply increasing food
prices8and increased pollution.9,10
Fossil fuels, as any carbon-containing materials, upon their
combustion release carbon dioxide and water. The presently used
conversion of fossil fuels (coal, natural gas) to liquid hydro-
carbons and their products primarily by syngas-based chemistry
(vide infra) itself generates large amounts of CO2and byprod-
ucts. CO2is a major greenhouse gas significantly contributing
to global warming.11Mitigating its harmful effects is a well
recognized major challenge for humankind. The Kyoto agree-
ment and subsequent international efforts were directed to limit
CO2 emission into the atmosphere. Whereas econo-political
approaches such as carbon quotas and trading were suggested
and are increasingly put into effect in many countries, no new
major technological solution has emerged. Our suggested
Methanol Economy with the chemical recycling of carbon
dioxide to methanol and/or dimethyl ether and subsequently to
synthetic hydrocarbons and products offers such a new way to
render fuels renewable and environmentally carbon neutral or
even negative. It also offers humankind an inexhaustible carbon
source in the form of recyclable CO2, while at the same time
mitigating human-caused climate change (i.e., global warming).
Hydrogen needed for the chemical recycling of carbon dioxide
can come from water (by electrolysis or other cleavage) or from
still-existing significant hydrocarbon sources. Presently, avail-
able methane, primarily natural gas, but also other natural
sources such as coalbed methane, methane hydrate, and methane
from agricultural, domestic, and industrial sources can be
effectively utilized to produce methanol using improved ways,
including our new bireforming process (vide infra). We review
here efficient new ways to achieve the chemical recycling of
carbon dioxide including its capture, conversion to methanol
and/or dimethyl ether combining chemical and hydrogenative
reduction, or initial electrochemical reduction of CO2to CO.
Of course, all ways to recycle carbon dioxide to methanol
necessitate the use of significant energy. It should be emphasized
that we are not dealing with energy generation but only its
storage and use in a suitable form (i.e., methanol and/or dimethyl
ether). At the same time, our carbon recycling chemistry and
the Methanol Economy concept can utilize any form of energy;
still existing fossil fuels and alternative sources such as solar,
wind, hydro, geothermal, as well as atomic energy. They thus
offer extensive versatility and practical applications. As es-
sentially most of our energy in one form or another comes from
the sun, humankind will not experience a real energy shortage.
We only need to find suitable new ways to capture, store,
transport, and utilize energy.
Methanol was first produced as a minor byproduct of
producing charcoal by destructive distillation of wood and was
therefore called wood alcohol. Methanol produced this way was
used in the 19th century for lighting, cooking, and heating
purposes but was later replaced by cheaper fuels, especially
kerosene. Up to the 1920s, wood was the only source for
methanol, which was also needed in increasing quantities in
the developing chemical industry. Beginning in the 1920s, the
production of methanol from syngas, a mixture of CO and H2,
on an industrial scale was introduced by BASF in Germany.
Whereas coal was initially used as a feedstock for the syngas,
natural gas became the preferred feedstock after World War II.
It offered a higher hydrogen content and lower energy con-
sumption and contained fewer harmful impurities such as sulfur,
nitrogen, halogenated compounds, and heavy metals.12-16
Today, methanol is a primary raw material for the chemical
industry. It is manufactured in large quantities (about 40 million
J. Org. Chem. Vol. 74, No. 2, 2009
Outlook. We do not believe that there will be a single solution
to the discussed global problems. However, the approach of
the chemical recycling of carbon dioxide to produce carbon
neutral renewable fuels and materials offers a feasible and
powerful new alternative and is entering the stage of gradual
In conclusion, it needs to be again emphasized that the
chemical recycling of carbon dioxide to methanol and DME
provides a renewable, carbon-neutral, inexhaustible source for
efficient transportation fuels, for storing and transporting energy,
as well as convenient starting materials for producing ethylene
and propylene and from them synthetic hydrocarbons and their
products. It thus essentially replaces petroleum oil and natural
gas. While allowing the continued use of carbon-containing fuels
and materials, it also curtains harmful excessive CO2emissions
causing global warming. The concept of what we call the
“Methanol Economy” and much of the underlying chemistry
was developed in our work over the past 15 years and is
discussed in our monograph.2,108The present discussion on the
chemical recycling of carbon dioxide is an important part of
our overall approach.
Acknowledgment. We thank all members of the Olah-Prakash
research groups who have significantly contributed to the
discussed chemical recycling of carbon dioxide to methanol and
DME (and derived synthetic hydrocarbon and their products).
Their names are cited in the references. Our work was supported
by USC’s Loker Institute through generous gifts of friends,
private foundations, and institutions, including the John Stauffer
Charitable Trust and the Hydrocarbon Research Foundation.
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