4.8 Article

Identify the Removable Substructure in Carbon Activation

Journal

CHEMISTRY OF MATERIALS
Volume 29, Issue 17, Pages 7288-7295

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.7b01937

Keywords

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Funding

  1. National Science Foundation [1551693, 1507391]
  2. Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy
  3. Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy
  4. Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
  5. Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy [DE-AC02-05CH11231]
  6. U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Vehicle Technologies Office
  7. DOE Office of Science [DE-AC02-06CH11357]
  8. U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-765F00515]
  9. Direct For Mathematical & Physical Scien
  10. Division Of Materials Research [1507391] Funding Source: National Science Foundation

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Activated carbon plays a pivotal role in achieving critical functions, such as separation, catalysis, and energy storage. A remaining question of carbon activation is which substructures in amorphous carbon are preferentially removed during activation. Herein, we report the first structure activation correlation elucidated on the basis of unprecedented comprehensive characterization on carbon activation. We discover that activation under CO2 preferentially removes graphenic layers that are more defective. Therefore, the resulting activated carbon contains thinned turbostratic nanodomains that are of a higher local graphenic order. The mechanistic insights explain why more defective soft carbon is burned under CO2 at a much faster rate than hard carbon. The mechanism leads to an activation-based design principle of mesoporous carbon. Guided by this principle, a bimodal micro-mesoporous carbon is prepared simply by CO2 activation. Our findings may cause a paradigm shift for the rational design of nanoporous carbon.

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