Improving the intrinsic activity of electrocatalysts for sustainable energy conversion: where are we and where can we go?

Abstract

We evaluate the improvements over the past two decades in intrinsic activity of electrocatalysts for sustainable energy conversion, and highlight opportunities from tuning the electrolyte.

The mechanism for acetate formation in electrochemical CO(2)reduction on Cu: selectivity with potential, pH, and nanostructuring

“…, with x being a specific product of the SDS). 39 We evaluate our suggested reaction mechanism on representative facets: Cu(111) and Cu(100) as terraces and Cu(110) and Cu(211) as steps. We choose intermediates prior to HCCO* (and thus ketene) based on their thermodynamic or kinetic stability which is in line with established trends.…”

“…38 The same RDS is consistent with the range of similar Tafel , with x being a specific product of the SDS). 39 We evaluate our suggested reaction mechanism on representative facets:…”

Pathways for the Formation of C2+ Products under Alkaline Conditions during the Electrochemical Reduction of CO2

“…Computational approaches to modeling the electrochemical interface have emerged to fill this void and provide a reasonable pathway to identifying critical intermediate species and mechanisms for a variety of reaction chemistries . Investigating the alkaline pathway of the CO2RR, in which water is the proton source and produces hydroxide ions, has known challenges for computational studies, particularly those relying on an explicit electrolyte representation. − Nearly all computational studies of the CO2RR to date have therefore investigated the acidic pathway, where the proton source is hydronium cations. − However, recent experiments suggest that, even in the case of the bulk electrolyte pH being highly acidic, the pH near the interface is alkaline at operating conditions due to hydroxide anion transport limitations. − Furthermore, most experiments are conducted with neutral to alkaline bulk pH, resulting in an even higher local pH near the interface and limiting the availability of hydronium cations at an active site. − Considering the importance of the electrolyte pH on electrocatalysis − and the likely absence of hydronium cations near the interface in operando , in this work we investigate the alkaline pathway for the formation of C 2+ products during the CO2RR.…”

Mechanism for acetate formation in electrochemical CO(2) reduction on Cu: Selectivity with potential, pH, and nanostructuring

“…r x = r RDS r SDS x i r sDS i , with x being a specific product of the SDS). 39 We evaluate our suggested reaction mechanism on representative facets: Cu(111) and Cu(100) terraces and Cu(110) and Cu(211) as steps. We choose intermediates prior to HCCO* (and thus ketene) based on their thermodynamic or kinetic stability which is in line with established trends.…”