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by David Chandler  (MIT News) Study reveals why some attempts to convert the greenhouse gas into fuel have failed, and offers possible solutions. — If researchers could find a way to chemically convert carbon dioxide into fuels or other products, they might make a major dent in greenhouse gas emissions. But many such processes that have seemed promising in the lab haven’t performed as expected in scaled-up formats that would be suitable for use with a power plant or other emissions sources.

Now, researchers at MIT have identified, quantified, and modeled a major reason for poor performance in such conversion systems. The culprit turns out to be a local depletion of the carbon dioxide gas right next to the electrodes being used to catalyze the conversion. The problem can be alleviated, the team found, by simply pulsing the current off and on at specific intervals, allowing time for the gas to build back up to the needed levels next to the electrode.

The findings, which could spur progress on developing a variety of materials and designs for electrochemical carbon dioxide conversion systems, were published today in the journal Langmuir, in a paper by MIT postdoc Álvaro Moreno Soto, graduate student Jack Lake, and professor of mechanical engineering Kripa Varanasi.

“Carbon dioxide mitigation is, I think, one of the important challenges of our time,” Varanasi says. While much of the research in the area has focused on carbon capture and sequestration, in which the gas is pumped into some kind of deep underground reservoir or converted to an inert solid such as limestone, another promising avenue has been converting the gas into other carbon compounds such as methane or ethanol, to be used as fuel, or ethylene, which serves as a precursor to useful polymers.

There are several ways to do such conversions, including electrochemical, thermocatalytic, photothermal, or photochemical processes. “Each of these has problems or challenges,” Varanasi says. 

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The team has focused on the electrochemical approaches, with a goal of getting “higher-C products” — compounds that contain more carbon atoms and tend to be higher-value fuels because of their energy per weight or volume. In these reactions, the biggest challenge has been curbing competing reactions that can take place at the same time, especially the splitting of water molecules into oxygen and hydrogen.

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One way of counteracting this depletion, they found, can be achieved by a pulsed system — a cycle of simply turning off the voltage, stopping the reaction and giving the carbon dioxide time to spread back into the depleted zone and reach usable levels again, and then resuming the reaction.

Often, the researchers say, groups have found promising catalyst materials but haven’t run their lab tests long enough to observe these depletion effects, and thus have been frustrated in trying to scale up their systems. Furthermore, the concentration of carbon dioxide next to the catalyst dictates the products that are made. Hence, depletion can also change the mix of products that are produced and can make the process unreliable.  READ MORE