Publication date: 10th April 2024
Interfacial reactions at the solid electrolyte interphase control the performance of batteries and electrochemical N2 and CO2 reduction. In batteries, degradation is typically accompanied by parasitic gas evolution reaction. In this contribution I will explore the commonalities between battery science and electrocatalysis and demonstrate the insight to be gained by studying different electrochemical reactions in parallel.
We recently demonstrated that on chip electrochemistry mass spectrometry - previously developed for aqueous electrocatalysis1 - can detect and quantify gases such as O2, CO2, C2H4 and H2 with ultra high sensitivity and time resolution during lithium ion battery operation.2 It allows us to probe degradation processes, which were previously unobservable. Augmented by 18O2 isotopic labelling, we reveal that lattice oxygen, not singlet oxygen is the more probable reactive species during the degradation of lithium nickel manganese cobalt oxide electrodes. We also show that CO2 reduction to ethylene takes place at graphite anodes.
Electrochemical nitrogen reduction to ammonia is a potentially sustainable and scalable alternative to the Haber Bosch process. Thus far, amongst solid electrodes, only lithium and calcium based electrodes in organic electrolytes can unequivocally reduce nitrogen to ammonia.3-5 Even so, at present, the lithium based system is far too inefficient and unstable for many practical uses. We hypothesise that the reactivity of lithium and calcium is due to (a) their ability to bind and dissociate N2 and (b) their ability to form solid electrolyte interphases that can moderate access to Li+ and H+ but facilitate access to N2.6 Herein, I will peruse upon these hypotheses, using a combination of electrochemical experiments, cryo-microscopy, infrared spectroscopy, electrochemistry mass spectrometry, time-of-flight secondary ion mass spectrometry, X-ray photoelectron spectroscopy and density functional theory On the basis of our insight, we propose new avenues towards going beyond lithium and calclium in electrochemical nitrogen fixation.
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