Electrochemistry holds the promise to be a cornerstone for the sustainable production of fuels and chemicals. However, these catalytic reactions are increasingly complex to understand and hereby also improve. In particular, reactions that suffer from selectivity challenges such as CO₂ reduction

In this talk, I will discuss how experiments and computational simulations can support each other. I will focus on electrochemical reduction of NO_x, CO₂, N_2, and the combinations. Importantly, all these reactions share a direct competition with hydrogen, and furthermore, several products are formed from each reactant of these reactants. I will give minimalistic models that do not overfit or over-interpretate experimental data. Examples are:

- Electrochemical CO₂ reduction show multiple different products depending on metal catalyst [1]. I will show why copper is unique as catalyst with a multiple-carbon product distribution [2]. Following I will discuss data analytics on copper facets to steer the product distribution [3].

- Electrochemical NO_x reduction, also multiple products are formed; N₂O, N₂ and NH₃[4]. Several catalyst enable reductions to ammonia amongst them copper [5] and recently also Co and Fe based catalysts close to their reduction potential [6].

- Electrochemical N₂ reduction to ammonia (NH₃) at ambient conditions is burgeoning [7-8]. Most interesting in aqueous there is not a “copper” catalyst [9]. While in non-aqueous, the univocally working system is a Li-mediate system [10]. For this system, I will show that varying multiple experimental parameters display similar performance characteristics [11] and I will discuss systems beyond lithium.

Finally, I will discuss how one can use these insights to establish predictive schemes for products beyond the typical reduction reaction products, hereunder synthesis of urea [12].

[1] Hori et. al., Journal of the Chemical Society, Faraday Transactions, 1989, 85, 2309-2326.

[2] Bagger, Ju, …, Strasser, Rossmeisl, ChemPhysChem, 2017, 18, 3266–3273.

[3] Bagger, Ju, …, Strasser, Rossmeisl, ACS Catalysis, 2019, 9, 7894−7899

[4] Rosca, Duca, Groot, Koper, Chem. Rev. 2009, 109, 2209–2244

[5] Wan, Bagger, Rossmeisl, Angewandte Chemie, 2021, 133 (40), 22137-22143

[6] Carvalho, …, Stoerzinger, JACS 2022, 144, 14809 14818.

[7] Andersen et al. Nature, 2019, 570, 504-508.

[8] Lazouski et al, Nature Catalysis, 2020, 3, 2520-1158.

[9] Bagger, Wan, Stephens, Rossmeisl, ACS Catalysis, 2021, 11 (11), 6596-6601

[10] Tsuneto et al. Journal of Electroanalytical Chemistry (1994)

[11] Spry, Westhead, Tort, Titirici, Stephens, Bagger, ACS Energy Letters, 2023, 8 (2), 1230-1235

[12] Wan, Wang, Tan, Filippi, Strasser, Rossmeisl, Bagger, ACS Catalysis, 2023, 13, 1926-1933