Double-site Substitution of Ce into (Ba, Sr)MnO3 Perovskites for Solar Thermochemical Hydrogen Production

TL;DR

This study develops a high-throughput experimental approach to identify and optimize Ce-substituted (Ba,Sr)MnO3 perovskites for solar thermochemical hydrogen production, demonstrating enhanced stability and hydrogen yield.

Contribution

It introduces a combined bulk synthesis and thin film screening method to discover and improve complex oxide materials for STCH, focusing on double-site Ce substitution.

Findings

Ce substitution increases hydrogen production 2-3x over CeO2.

Double-site Ce substitution enhances Ce solubility and structural stability.

High-throughput screening accelerates discovery of promising STCH materials.

Abstract

Solar thermochemical hydrogen production (STCH) is a renewable alternative to hydrogen produced using fossil fuels. While serial bulk experimental methods can accurately measure STCH performance, screening chemically complex materials systems for new promising candidates is more challenging. Here we identify double-site Ce-substituted (Ba,Sr)MnO3 oxide perovskites as promising STCH candidates using a combination of bulk synthesis and high-throughput thin film experiments. The Ce substitution on the B-site in 10H-BaMnO3 and on the A-site in 4P-SrMnO3 lead to 2-3x higher hydrogen production compared to CeO2, but these bulk single-site substituted perovskites suffer from incomplete reoxidation. Double-site Ce substitution on both A- and B-site in (Ba,Sr)MnO3 thin films increases Ce solubility and extends the stability of 10H and 4P structures, which is promising for their thermochemical reversibility. This study demonstrates a high-throughput experimental method for screening complex oxide materials for STCH applications.