Understanding mechanisms of carbon dioxide conversion into methane for designing enhanced catalysts from first-principles

Dong Yun Shin, Jun Ho Jo, Jai Young Lee, Dong Hee Lim

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17 Scopus citations


Conversion of carbon dioxide (CO2) into methane (CH4) on copper (Cu) surfaces were investigated to understand the fundamental mechanism of CO2 reduction, and to suggest a key factor for designing promising catalysts for CO2 conversion into hydrocarbon fuels. The density functional theory calculations revealed the lowest-energy reaction pathways on Cu(100), Cu(110), and Cu(111) planes, and determined that the potential limiting step for CO2 reduction lies between the reaction intermediates CO* and CHO* (* denotes the state adsorbed on the catalyst surface). The energy barrier to the potential limiting step is lowered in the following order: Cu(110) < Cu(100) < Cu(111). A key factor for obtaining the lowest energy barrier on Cu(110) may be the largest interatomic distance on the Cu(110) surface among the three surfaces, which enhances the interaction between the key intermediate CHO and the Cu surface, compared to that between CO and the surface. This finding may be applied to developing promising catalysts for CO2 reduction by designing a Cu thin film on a supporting material with larger lattice constant than Cu. To demonstrate this, we evaluated the energy barriers to the potential limiting step on a single Cu thin layer supported on both palladium (Pd) and silver (Ag), and confirmed that the Pd supporting material can enlarge the interatomic distance of the single Cu(111) layer by 8.7% and thereby lower the energy barrier from 0.97 to 0.63 eV.

Original languageEnglish
Pages (from-to)31-37
Number of pages7
JournalComputational and Theoretical Chemistry
StatePublished - 1 May 2016


  • Copper catalyst
  • Density functional theory (DFT)
  • Electrochemical reduction of CO
  • Strain effect


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