Harnessing High-Throughput Computational Methods to Accelerate the Discovery of Optimal Proton Conductors for...

The pursuit of high-performance and long-lasting protonic ceramic electrochemical cells (PCECs) is impeded by the lack of efficient and enduring proton conductors. Conventional research approaches, predominantly based on a trial-and-error methodology, have proven to be demanding of resources and time-consuming. Here, this work reports the findings in harnessing high-throughput computational methods to expedite the discovery of optimal electrolytes for PCECs. This work methodically computes the oxygen vacancy formation energy (E_V), hydration energy (E_H), and the adsorption energies of H₂O and CO₂ for a set of 932 oxide candidates. Notably, these findings highlight BaSn_xCe_0.8-xYb_0.2O_3-δ (BSCYb) as a prospective game-changing contender, displaying superior proton conductivity and chemical resilience when compared to the well-regarded BaZr_xCe_0.8-xY_0.1Yb_0.1O_3-δ (BZCYYb) series. Experimental validations substantiate the computational predictions; PCECs incorporating BSCYb as the electrolyte achieved extraordinary peak power densities in the fuel cell mode (0.52 and 1.57 W cm^-2 at 450 and 600 °C, respectively), a current density of 2.62 A cm^-2 at 1.3 V and 600 °C in the electrolysis mode while demonstrating exceptional durability for over 1000-h when exposed to 50% H₂O. This research underscores the transformative potential of high-throughput computational techniques in advancing the field of proton-conducting oxides for sustainable power generation and hydrogen production.