Breakthrough in CO2 conversion to useful forms of carbon

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CO2 is an important air pollution emission contributing to climate change. Researchers around the globe are looking at ways to remove CO2 from flue gasses and to store it (sequestering) or to in someway use it. By tuning gold nanoparticles to just the right size, researchers from Brown University have developed a catalyst that selectively converts carbon dioxide (CO2) to carbon monoxide (CO), an active carbon molecule that can be used to make alternative fuels and commodity chemicals. "Our study shows potential of carefully designed gold nanoparticles to recycle CO2 into useful forms of carbon," said Shouheng Sun, professor of chemistry and one of the study’s senior authors. "The work we've done here is preliminary, but we think there's great potential for this technology to be scaled up for commercial applications."

CO2 is an important air pollution emission contributing to climate change. Researchers around the globe are looking at ways to remove CO2 from flue gasses and to store it (sequestering) or to in someway use it.

By tuning gold nanoparticles to just the right size, researchers from Brown University have developed a catalyst that selectively converts carbon dioxide (CO2) to carbon monoxide (CO), an active carbon molecule that can be used to make alternative fuels and commodity chemicals.

"Our study shows potential of carefully designed gold nanoparticles to recycle CO2 into useful forms of carbon," said Shouheng Sun, professor of chemistry and one of the study's senior authors. "The work we've done here is preliminary, but we think there's great potential for this technology to be scaled up for commercial applications."
The idea of recycling CO2 — a greenhouse gas the planet current has in excess — is enticing, but there are obstacles. CO2 is an extremely stable molecule that must be reduced to an active form like CO to make it useful. CO is used to make synthetic natural gas, methanol, and other alternative fuels.

Converting CO2 to CO isn't easy. Prior research has shown that catalysts made of gold foil are active for this conversion, but they don't do the job efficiently. The gold tends to react both with the CO2 and with the water in which the CO2 is dissolved, creating hydrogen byproduct rather than the desired CO.

The Brown experimental group, led by Sun and Wenlei Zhu, a graduate student in Sun’s group, wanted to see if shrinking the gold down to nanoparticles might make it more selective for CO2. They found that the nanoparticles were indeed more selective, but that the exact size of those particles was important. Eight nanometer particles had the best selectivity, achieving a 90-percent rate of conversion from CO2 to CO. Other sizes the team tested — four, six, and 10 nanometers — didn't perform nearly as well.

"At first, that result was confusing," said Andrew Peterson, professor of engineering and also a senior author on the paper. "As we made the particles smaller we got more activity, but when we went smaller than eight nanometers, we got less activity."

To understand what was happening, Peterson and postdoctoral researcher Ronald Michalsky used a modeling method called density functional theory. They were able to show that the shapes of the particles at different sizes influenced their catalytic properties.

Gold nanoparticles make better catalysts for CO2 recycling than bulk gold metal. Size is crucial though, since edges produce more desired results than corners (red points, above). Nanoparticles of 8 nm appear to have a better edge-to-corner ratio than 4 nm, 6 nm, or 10 nm nanoparticles. Image credit: Sun lab/Brown University

Read more at Brown University.