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@article{Kucernak:2022:10.1021/acscatal.2c00609,
author = {Kucernak, A and Zhang, G and cui, Y},
doi = {10.1021/acscatal.2c00609},
journal = {ACS Catalysis},
pages = {6180--6190},
title = {Real-time in situ monitoring of CO2 electroreduction in the liquid and gas phases by coupled mass spectrometry and localized electrochemistry},
url = {http://dx.doi.org/10.1021/acscatal.2c00609},
volume = {12},
year = {2022}
}

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TY  - JOUR
AB  - The mechanism and dynamics of the CO2 reduction reaction (CO2RR) remain poorly understood, which is largely caused by mass transport limitations and lack of time-correlated product analysis tools. In this work, a custom-built gas accessible membrane electrode (GAME) system is used to comparatively assess the CO2RR behavior of Au and Au−Cu catalysts. The platform achieves high reduction currents (∼ – 50 mA cm–2 at 1.1 V vs RHE) by creating a three-phase boundary interface equipped with an efficient gas-circulation pathway, facilitating rapid mass transport of CO2. The GAME system can also be easily coupled with many other analytical techniques as exemplified by mass spectrometry (MS) and localized ultramicroelectrode (UME) voltammetry to enable real-time and in situ product characterization in the gas and liquid phases, respectively. The gaseous product distribution is explicitly and quantitatively elucidated with high time resolution (on the scale of seconds), allowing for the independent assessment of Tafel slope estimates for the hydrogen (159/168 mV decade–1), ethene (160/170 mV decade–1), and methane (96/100 mV decade–1) evolution reactions. Moreover, the UME is used to simultaneously measure the local pH shift during CO2RR and assess the production of liquid phase species including formate. A positive shift of 0.8 pH unit is observed at a current density of −11 mA cm–2 during the CO2RR.
AU  - Kucernak,A
AU  - Zhang,G
AU  - cui,Y
DO  - 10.1021/acscatal.2c00609
EP  - 6190
PY  - 2022///
SN  - 2155-5435
SP  - 6180
TI  - Real-time in situ monitoring of CO2 electroreduction in the liquid and gas phases by coupled mass spectrometry and localized electrochemistry
T2  - ACS Catalysis
UR  - http://dx.doi.org/10.1021/acscatal.2c00609
UR  - https://pubs.acs.org/doi/10.1021/acscatal.2c00609
UR  - http://hdl.handle.net/10044/1/96947
VL  - 12
ER  -

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