Partial Exsolution Enables Superior Bifunctionality of Ir@SrIrO3 for Acidic Overall Water Splitting.

The pursuit of efficient and durable bifunctional electrocatalysts for overall water splitting in acidic media is highly desirable, albeit challenging. SrIrO3 based perovskites are electrochemically active for oxygen evolution reaction (OER), however, their inert activities toward hydrogen evolution reaction (HER) severely restrict the practical implementation in overall water splitting. Herein, an Ir@SrIrO3 heterojunction is newly developed by a partial exsolution approach, ensuring strong metal-support interaction for OER and HER. Notably, the Ir@SrIrO3-175 electrocatalyst, prepared by annealing SrIrO3 in 5% H2 atmosphere at 175 °C, delivers ultralow overpotentials of 229 mV at 10 mA cm-2 for OER and 28 mV at 10 mA cm-2 for HER, surpassing most recently reported bifunctional electrocatalysts. Moreover, the water electrolyzer using the Ir@SrIrO3-175 bifunctional electrocatalyst demonstrates the potential application prospect with high electrochemical performance and excellent durability in acidic environment. Theoretical calculations unveil that constructing Ir@SrIrO3 heterojunction regulates interfacial electronic redistribution, ultimately enabling low energy barriers for both OER and HER.

Reverse Atom Capture on Perovskite Surface Enabling Robust and Efficient Cathode for Protonic Ceramic Fuel Cells.

Protonic ceramic fuel cells (PCFCs) hold potential for sustainable energy conversion, yet their widespread application is hindered by the sluggish kinetics and inferior stability of cathode materials. Here, a facile and efficient reverse atom capture technique is developed to manipulate the surface chemistry of PrBa0.5Sr0.5Co1.5Fe0.5O5+ δ (PBSCF) cathode for PCFCs. This method successfully captures segregated Ba and Sr cations on the PBSCF surface using W species, creating a (Ba/Sr)(Co/Fe/W)O3- δ (BSCFW)@PBSCF heterostructure. Benefiting from enhanced kinetics of proton-involved oxygen reduction reaction and strengthened chemical stability, the single cell using the optimized 2W-PBSCF cathode demonstrates an exceptional peak power density of 1.32 W cm-2 at 650 °C and maintains durable performance for 240 h. Theoretical calculations unveil that the BSCFW perovskite delivers lower oxygen vacancy formation energy, hydration energy, and proton transfer energy compared to the PBSCF perovskite. This protocol offers new insights into advanced atom capture techniques for sustainable energy infrastructures.

Smart Dual-Exsolved Self-Assembled Anode Enables Efficient and Robust Methane-Fueled Solid Oxide Fuel Cells.

Perovskite oxides have emerged as alternative anode materials for hydrocarbon-fueled solid oxide fuel cells (SOFCs). Nevertheless, the sluggish kinetics for hydrocarbon conversion hinder their commercial applications. Herein, a novel dual-exsolved self-assembled anode for CH4 -fueled SOFCs is developed. The designed Ru@Ru-Sr2 Fe1.5 Mo0.5 O6-δ (SFM)/Ru-Gd0.1 Ce0.9 O2-δ (GDC) anode exhibits a unique hierarchical structure of nano-heterointerfaces exsolved on submicron skeletons. As a result, the Ru@Ru-SFM/Ru-GDC anode-based single cell achieves high peak power densities of 1.03 and 0.63 W cm-2 at 800 °C under humidified H2 and CH4 , surpassing most reported perovskite-based anodes. Moreover, this anode demonstrates negligible degradation over 200 h in humidified CH4 , indicating high resistance to carbon deposition. Density functional theory calculations reveal that the created metal-oxide heterointerfaces of Ru@Ru-SFM and Ru@Ru-GDC have higher intrinsic activities for CH4 conversion compared to pristine SFM. These findings highlight a viable design of the dual-exsolved self-assembled anode for efficient and robust hydrocarbon-fueled SOFCs.

Enhancing the bifunctional activity of CoSe2 nanocubes by surface decoration of CeO2 for advanced zinc-air batteries.

The coupling of oxygen evolution and reduction reactions (OER and ORR) plays a key role in rechargeable Zn-air batteries (ZABs). However, both OER and ORR still suffer from sluggish kinetics, even when using the mainstream precious metal-based catalysts. Herein, oxygen vacancies-rich CeO2 decorated CoSe2 nanocubes are proposed as a novel air electrode to drive OER and ORR for ZABs. The resultant CeO2 coupled CoSe2 nanocubes (CeO2@CoSe2-NCs) catalyst exhibits a significantly enhanced bifunctional activity relative to the pristine CoSe2-NCs and the pristine CeO2. Moreover, an assembled ZABs using this CeO2@CoSe2-NCs electrode delivers a high output power density of 153 mW cm-2 and a long-life stability over 400 cycles, superior to the benchmark Pt/C-IrO2 electrode. Theoretical calculations reveal that the electronic interaction and oxygen vacancies in CeO2@CoSe2-NCs contribute to efficient oxygen electrocatalysis. This protocol provides a promising approach of constructing oxygen vacancies in hybrid catalysts for energy conversion and storage devices.