Harnessing High-Throughput Computational Methods to Accelerate the Discovery of Optimal Proton Conductors for High-Performance and Durable Protonic Ceramic Electrochemical Cells.

The pursuit of high-performance and long-lasting protonic ceramic electrochemical cells (PCECs) has been 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 we report our findings in harnessing high-throughput computational methods to expedite the discovery of optimal electrolytes for PCECs. We methodically computed the oxygen vacancy formation energy (E V ), hydration energy (E H ), and the adsorption energies of H 2 O and CO 2 for a set of 932 oxide candidates. Notably, our findings highlight BaSn x Ce 0.8-x Yb 0.2 O 3-δ (BSCYb) as a prospective game-changing contender, displaying superior proton conductivity and chemical resilience when compared to the well-regarded BaZr x Ce 0.8-x Y 0.1 Yb 0.1 O 3-δ (BZCYYb) series. Experimental validations substantiate our 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 hours when exposed to 50% H 2 O. 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. This article is protected by copyright. All rights reserved.