4.6 Article

Deactivation and regeneration of a benchmark Pt/C catalyst toward oxygen reduction reaction in the presence of poisonous SO2 and NO

Journal

CATALYSIS SCIENCE & TECHNOLOGY
Volume 12, Issue 9, Pages 2929-2934

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d2cy00141a

Keywords

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Funding

  1. National Key Research and Development Program of China [2016YFB0101207]
  2. National Natural Science Foundation of China (NSFC) [21733004]
  3. National Basic Research Program of China (973 Program) [2015CB932303]

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This study investigates the deactivation and regeneration processes of Pt surfaces during ORR in the presence of both SO2 and NO. The results demonstrate that by controlling the appropriate NO:SO2 ratio, the adsorption of SO2 can be completely inhibited, preventing Pt deactivation.
SO2 is considered as the most poisonous ambient contaminant to proton exchange membrane fuel cell (PEMFC) cathodes, leading to severe Pt deactivation and oxygen reduction reaction (ORR) performance loss. Great efforts have been devoted to studying the deactivation and regeneration of SO2-poisoned Pt/C catalysts, but far less to cases with coexisting NO. Herein, the deactivation and regeneration processes of Pt surfaces during ORR in the presence of both SO2 and NO (in different molar ratios) are investigated by means of in situ electrochemical infrared spectroscopy and density functional theory (DFT) calculations. Interestingly, NO presents a stronger affinity to Pt sites than SO2-if an appropriate NO : SO2 ratio is applied, SO2 adsorption can be completely inhibited. Besides, the competitive adsorption of NO can weaken the Pt-S bond and expel adsorbed SO2. Given that adsorbed NO is readily reduced, a faster regeneration is observed if NO and SO2 are simultaneously fed into the cathode.

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