Engineering bipolar doping in a Janus dual‑atom catalyst for photo‑enhanced rechargeable Zn‑Air battery
Shanghai Jiao Tong University Journal Center
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Credit: Ning Liu, Yinwu Li, Wencai Liu, Zhanhao Liang, Bin Liao, Fang Yang, Ming Zhao, Bo Yan, Xuchun Gui, Hong Bin Yang, Dingshan Yu*, Zhiping Zeng*, Guowei Yang.
While rechargeable zinc-air batteries (RZABs) promise >1 kWh kg-1 at low cost, their air cathodes still struggle with sluggish oxygen redox kinetics and poor photon harvesting. Now researchers at Sun Yat-sen University—Prof. Zhiping Zeng and Prof. Dingshan Yu—report a one-step “bipolar-doped” Janus dual-atom catalyst (JDAC) that couples Ni-N4 and Fe-N4 sites on a narrow-band-gap C4N matrix. The material simultaneously splits water and sunlight, cutting charge voltage by 620 mV and extending cycle life to 6 000 cycles at 10 mA cm-2 under visible light.
Why Janus Dual-Atom Catalysis Matters
• Photo-Electro Synergy: Ni centers harvest holes for OER, Fe centers collect electrons for ORR, slashing recombination and raising photocurrent by 3×.
• Bipolar Doping: Coexisting n- and p-type domains widen the space-charge region, boosting carrier density 2.5-fold and shrinking charge-transfer resistance to 8.6 Ω.
• High-Current Stability: Light-assisted RZABs operate at 50 mA cm-2 for 300 cycles and 20 mA cm-2 for 1 600 cycles—an order-of-magnitude jump over prior photo-cathodes.
Innovative Design and Features
• Material System: Single-step hydrothermal co-assembly of hexaketocyclohexane, biphenylteramine, Fe/Ni acetates on carbon paper; 1.92 eV band-gap, atomically dispersed M-N4 verified by HAADF-STEM and XANES.
• Mechanistic Insight: In-situ Raman/XANES show Ni-OOH forms first at 1.3 V for OER while Fe-O₂H emerges at 0.85 V for ORR; DFT confirms 0.74 eV down-shift of Fe d-band center weakens *OH binding, lowering overpotentials to 170 mV (OER) and 350 mV (ORR).
• Device Architecture: Integrated directly as a freestanding air cathode—no binder, no conductive additive—yielding 267 mV photo-induced discharge gain and 0.53 V round-trip voltage gap at 1 mA cm-2.
Applications and Future Outlook
• Solar-Driven Storage: 2 × 2 cm2 pouch cells deliver 220 mW cm-2 peak power under 1 sun and maintain 80 % capacity after 500 deep cycles at 5 mA cm-2.
• Scalability: Precursor cost <$0.50 g-1, hydrothermal throughput >10 g L-1; roll-to-roll coating trials underway for 100 Wh module prototypes.
• Challenges & Next Steps: Long-term UV stability and rare-earth-free analogues (Cu/Co, Mn/Cr) are being explored; the team is also transferring the JDAC concept to photo-enhanced metal-sulfur and metal-N₂ batteries.
This work provides a universal blueprint for merging photocatalysis and electrocatalysis at the atomic limit, turning everyday sunlight into an extra voltage bonus for next-generation metal-air chemistries. Stay tuned for more light-harvesting battery breakthroughs from Prof. Zeng and Prof. Yu at Sun Yat-sen University!
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