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Theoretical investigation of water-gas shift reaction catalyzed by water-soluble Rh(III)–EDTA complex

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Abstract

We systematically investigate the mechanisms of water-gas shift reaction (WGSR) on [Rh(EDTA)CO]− complex on the basis of density functional theory calculations. Two different reaction pathways have been considered: One is the synthesis of HCOOH, and the other is the direct formation of H2 from H2O and CO. The former offers new insights into the fundamental direct mechanism for WGSR. In this study, we combine with the energetic span model to study the catalytic activity of different active sites and two different reaction pathways. Our calculation results indicate that the formation of HCOOH mechanism is the energetically favorable pathway for the water-gas shift reaction on [Rh(EDTA)CO]− catalyst. Moreover, the Oc site acts as the most active site for the formation of HCOOH due to the highest value of TOF. NPA charges are calculated to shed further light on the properties leading up to the formation of HCOOH. Our work will be useful for developing the WGSR mechanism and designing better catalysts for WGSR.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Grant No. 20603021), the Natural Science Foundation of Shanxi (Grant No. 2013011009-6), the High School 131 Leading Talent Project of Shanxi, Undergraduate Training Programs for Innovation and Entrepreneurship of Shanxi Province (Grant No. 2013145 and Grant No. 2015537), Shanxi Normal University (SD2013CXCY-65, 105088), Teaching Reform Project of Shanxi Normal University (SD2013JGXM-51) and Graduate student innovation project (2016SY037).

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Authors and Affiliations

  1. School of Chemistry and Material Science, School of Modern Arts and Sciences, Shanxi Normal University, Linfen, 041004, China

    Zhaoru Cao, Ling Guo, Naying Liu, Wenli Li, Xiaoli Zheng, Yayin Shi, Juan Guo & Yaru Xi

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  1. Zhaoru Cao
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  2. Ling Guo
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Correspondence to Ling Guo.

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Cao, Z., Guo, L., Liu, N. et al. Theoretical investigation of water-gas shift reaction catalyzed by water-soluble Rh(III)–EDTA complex. Theor Chem Acc 136, 53 (2017). https://doi.org/10.1007/s00214-017-2080-4

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