In a unified regenerative fuel cell (URFC) or reversible fuel cell, the oxygen bifunctional catalyst must switch reversibly between the oxygen reduction reaction (ORR), fuel cell mode, and the oxygen evolution reaction (OER), electrolyzer mode. However, it is often unclear what effect alternating between ORR and OER has on the electrochemical behavior and physiochemical properties of the catalyst. Herein, operando X-ray absorption spectroscopy (XAS) is utilized to monitor the continuous and dynamic evolution of the Co, Mn, and Fe oxidation states of perovskite catalysts Ba0.5Sr0.5Co0.8Fe0.2O3-δ (BSCF) and La0.4Sr0.6MnO3-δ (LSM), while the potential is oscillated between reducing and oxidizing potentials with cyclic voltammetry. The results reveal the importance of investigating bifunctional catalysts by alternating between fuel cell and electrolyzer operation and highlight the limitations and challenges of bifunctional catalysts. It is shown that the requirements for ORR and OER performance are divergent and that the oxidative potentials of OER are detrimental to ORR activity. These findings are used to give guidelines for future bifunctional catalyst design. Additionally, it is demonstrated how sunlight can be used to reactivate the ORR activity of LSM after rigorous cycling.
The development of high-performance organic solar cells (OSCs) with high operational stability is essential to accelerate their commercialization. Unfortunately, our understanding of the origin of instabilities in state-of-the-art OSCs based on bulk heterojunction (BHJ) featuring non-fullerene acceptors (NFAs) remains limited. Herein, we developed NFA-based OSCs using different charge extraction interlayer materials and studied their storage, thermal, and operational stabilities. Despite the high power conversion efficiency (PCE) of the OSCs (17.54%), we found that cells featuring self-assembled monolayers (SAMs) as hole-extraction interlayers exhibited poor stability. The time required for these OSCs to reach 80% of their initial performance (T80) was only 6 h under continuous thermal stress at 85 °C in a nitrogen atmosphere and 1 h under maximum power point tracking (MPPT) in a vacuum. Inserting MoOx between ITO and SAM enhanced the T80 to 50 and ~15 h after the thermal and operational stability tests, respectively, while maintaining a PCE of 16.9%. Replacing the organic PDINN electron transport layer with ZnO NPs further enhances the cells' thermal and operational stability, boosting the T80 to 1000 and 170 h, respectively. Our work reveals the synergistic roles of charge-selective interlayers and device architecture in developing efficient and stable OSCs.
The separator is an essential component of sodium-ion batteries (SIBs) to determine their electrochemical performances. However, the separator with high mechanical strength, good electrolyte wettability and excellent electrochemical performance remains an open challenge. Herein, a new separator consisting of amphoteric nanofibers with abundant functional groups was fabricated through supramolecular assembly of natural polymers for SIB. The uniform nanoporous structure, remarkable mechanical properties and abundant functional groups (e.g. −COOH, −NH2 and −OH) endow the separator with lower dissolution activation energy and higher ion migration numbers. These metrics enable the separator to lower the barrier for desolvation of Na+, accelerate the migration of Na+, and generate more stable solid electrolyte interphase (SEI) and cathode electrolyte interphase (CEI). The battery assembled with the amphoteric nanofiber separator shows higher specific capacity and better stability than that assembled with glass fiber (GF) separator.
Aluminum (Al)-ion batteries have emerged as a potential alternative to conventional ion batteries that rely on less abundant and costly materials like lithium. Nonetheless, given the nascent stage of advancement in Al-ion batteries (AIBs), attaining electrode materials that can leverage both intercalation capacity and structural stability remains challenging. Herein, we demonstrate a C3N4-derived layered N,S heteroatom−doped carbon, obtained at different pyrolysis temperatures, as a cathode material for AIBs, encompassing the diffusion−controlled intercalation and surface-induced capacity with ultrahigh reversibility. The developed layered N,S-doped corbon (N,S-C) cathode, synthesized at 900 °C, delivers a specific capacity of 330 mAh g−1 with a relatively high coulombic efficiency of ~85% after 500 cycles under a current density of 0.5 A g−1. Owing to its reinforced adsorption capability and enlarged interlayer spacing by doping N and S heteroatoms, the N,S-C900 cathode demonstrates outstanding energy storage capacity with excellent rate performance (61 mAh g−1 at 20 A g−1) and ultrahigh reversibility (90 mAh g−1 at 5 A g−1 after 10 000 cycles).