Ionic-caged heterometallic bismuth-platinum complex exhibiting electrocatalytic CO2 reduction.
Dalton transactions (Cambridge, England : 2003)
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Yoshida, T., Ahsan, H. M., Zhang, H., Izuogu, D., Abe, H., Ohtsu, H., Yamaguchi, T., et al. (2020). Ionic-caged heterometallic bismuth-platinum complex exhibiting electrocatalytic CO2 reduction.. Dalton transactions (Cambridge, England : 2003), 49 (8), 2652-2660. https://doi.org/10.1039/c9dt04817k
An air-stable heterometallic Bi-Pt complex with the formula [BiPt(SAc)5]n (1; SAc = thioacetate) was synthesized. The crystal structure, natural bond orbital (NBO) and local orbital locator (LOL) analyses, localized orbital bonding analysis (LOBA), and X-ray absorption fine structure (XAFS) measurements were used to confirm the existence of Bi-Pt bonding and an ionic cage of O atoms surrounding the Bi ion. From the cyclic voltammetry (CV) and controlled potential electrolysis (CPE) experiments, 1 in tetrahydrofuran reduced CO2 to CO, with a faradaic efficiency (FE) of 92% and a turnover frequency (TOF) of 8 s-1 after 30 min of CPE at -0.79 V vs. NHE. The proposed mechanism includes an energetically favored pathway via the ionic cage, which is supported by the results of DFT calculations and reflectance infrared spectroelectrochemistry data.
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External DOI: https://doi.org/10.1039/c9dt04817k
This record's URL: https://www.repository.cam.ac.uk/handle/1810/301861
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