Time-Resolved Product Observation for CO2 Electroreduction Using Synchronised Electrochemistry-Mass Spectrometry with Soft Ionisation (sEC-MS-SI) |
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Authors: | Dr Guohui Zhang Prof Anthony Kucernak |
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Institution: | Department of Chemistry, Imperial College London, White City Campus, London, W12 0BZ United Kingdom |
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Abstract: | The mechanistic understanding of electrochemical CO2 reduction reaction (CO2RR) requires a rapid and accurate characterisation of product distribution to unravel the activity and selectivity, which is yet hampered by the lack of advanced correlative approaches. Here, we present the time-resolved identification of CO2RR products by using the synchronised electrochemistry-mass spectrometry (sEC-MS). Transients in product formation can be readily captured in relation to electrochemical conditions. Moreover, a soft ionisation (SI) strategy is developed in MS for the direct observation of CO, immune to the interference of CO2 fragments. With the sEC-MS-SI, the kinetic information, such as Tafel slopes and onset potentials, for a myriad of CO2RR products are revealed and we show the hysteresis seen for the evolution of some species may originate from the potential-driven changes in surface coverage of intermediates. This work provides a real-time picture of the dynamic formation of CO2RR products. |
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Keywords: | Electrochemical CO2 Reduction Kinetics Operando Mass Spectrometry Reaction Mechanisms Soft Ionisation |
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