Abstract

A major goal within the CO2 electrolysis community is to replace the generally used Ir anode catalyst with a more abundant material, which is stable and active for water oxidation under process conditions. Ni is widely applied in alkaline water electrolysis, and it has been considered as a potential anode catalyst in CO2 electrolysis. Here we compare the operation of electrolyzer cells with Ir and Ni anodes and demonstrate that, while Ir is stable under process conditions, the degradation of Ni leads to a rapid cell failure. This is caused by two parallel mechanisms: (i) a pH decrease of the anolyte to a near neutral value and (ii) the local chemical environment developing at the anode (i.e., high carbonate concentration). The latter is detrimental for zero-gap electrolyzer cells only, but the first mechanism is universal, occurring in any kind of CO2 electrolyzer after prolonged operation with recirculated anolyte.

Highlights

  • A major goal within the CO2 electrolysis community is to replace the generally used Ir anode catalyst with a more abundant material, which is stable and active for water oxidation under process conditions

  • Taking a look at the Pourbaix diagrams,[9] Ni seems an ideal choice as anode catalyst for CO2 reduction reaction (CO2RR), as it is stable at high pH values even at high positive potentials

  • Ni has already been employed as anode catalyst in recent studies on CO2RR.[24−32] Concentrated electrolyte solutions (e.g., 1 M KOH) were used in most of these studies, and stability was mostly demonstrated in electrolyzer cells operating with liquid catholyte for relatively short time periods

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Summary

Introduction

A major goal within the CO2 electrolysis community is to replace the generally used Ir anode catalyst with a more abundant material, which is stable and active for water oxidation under process conditions. The operation of a custom-designed zero-gap electrolyzer cell (Scheme 1) was compared with Ir and Ni anode catalysts.[34,39,3] First, the cathode was purged with humidified Ar gas, and a 0.1 M CsOH solution was recirculated in the anode compartment, performing water electrolysis in the electrolyzer cell as a baseline experiment.

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