A first-principles microkinetic study on the hydrogenation of carbon dioxide over Cu(211) in the presence of water

  • Xitong Sun
  • Peng Wang
  • Zhengjiang Shao
  • Xiaoming CaoEmail author
  • P. HuEmail author


The hydrogenation of carbon dioxide (CO2) is one of important processes to effectively convert and utilize CO2, which is also regarded as the key step at the industrial methanol synthesis. Water is likely to play an important role in this process, but it still remains elusive. To systematically understand its influence, here we computationally compare the reaction mechanisms of CO2 hydrogenation over the stepped Cu(211) surface between in the absence and presence of water based on microkinetic simulations upon density functional theory (DFT) calculations. The effects of water on each hydrogenation step and the whole activity and selectivity are checked and its physical origin is discussed. It is found that the water could kinetically accelerate the hydrogenation on CO2 to COOH, promoting the reverse water gas shift reaction to produce carbon monoxide (CO). It hardly influences the CO2 hydrogenation to methanol kinetically. In addition, the too high initial partial pressure of water will thermodynamically inhibit the CO2 conversion.

CO2 activation microkinetic modeling DFT CH3OH selectivity 


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This work was supported by the National Key Research and Development Program of China (2018YFA0208600), the National Natural Science Foundation of China (21673072, 21333003, 91845111), and Program of Shanghai Subject Chief Scientist (17XD1401400).

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11426_2019_9639_MOESM1_ESM.pdf (1.5 mb)
A first-principles microkinetic study on the hydrogenation of carbon dioxide over Cu(211) in the presence of water


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Copyright information

© Science China Press and Springer-Verlag GmbH Germany, part of Springer Nature 2019

Authors and Affiliations

  1. 1.Key Laboratories for Advanced Materials, Centre for Computational Chemistry and Research Institute of Industrial Catalysis, School of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghaiChina
  2. 2.School of Chemistry and Chemical EngineeringQueen’s University of BelfastBelfastUK

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