A-Site High-Entropy Perovskite Enabling Sulfur-Tolerant and Coking-Resistant Anodes for Hydrocarbon-Fueled Solid Oxide Fuel Cells.
basic_science · Level V
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- Record sourced from PubMed, PMID 42454621.
- Also identified by DOI 10.1002/adma.74091.
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Abstract
Solid oxide fuel cells (SOFCs) are capable of electrochemically converting fossil fuels such as natural gas and coal-based syngas directly into electricity with high efficiency and minimal emissions, yet the state-of-the-art nickel-based anodes are susceptible to sulfur poisoning or coking when operated with sulfur-containing or hydrocarbon fuels. Here, we report a high-entropy strategy in which five equimolar cations are introduced at the A-site to develop a highly active and robust perovskite anode, Pr<sub>0.2</sub>Ba<sub>0.2</sub>La<sub>0.2</sub>Sr<sub>0.2</sub>Ca<sub>0.2</sub>FeO<sub>3-δ</sub> (PBLSCF). In situ reduction of PBLSCF leads to the exsolution of nanoscale Fe particles, enhancing its tolerance to sulfur poisoning and coking. Electrolyte-supported single cells using PBLSCF anodes achieve a peak power density (PPD) of 1.22 W cm<sup>-2</sup> at 800°C in H<sub>2</sub>, maintain stable operation for 1000 h and exhibit promising sulfur tolerance in 50 ppm H<sub>2</sub>S-H<sub>2</sub>. Density functional theory (DFT) calculations reveal that the high-entropy strategy reduces oxygen-vacancy formation energy, contributing to improved sulfur tolerance and fuel oxidation performance. Furthermore, stable operation using a PBLSCF anode for 600 h is also achieved with propane as fuel. This work provides a synergistic strategy through A-site high-entropy engineering and in situ metal exsolution to achieve promising electrochemical performance and enhanced multi-tolerance anodes for fuel-flexible SOFCs.