Densely colonized isolated Cu-N single sites for efficient bifunctional electrocatalysts and rechargeable advanced Zn-air batteries
- Authors
- Wagh, Nayantara K.; Shinde, Sambhaji S.; Lee, Chi Ho; Jung, Jin-Young; Kim, Dong-Hyung; Kim, Sung-Hae; Lin, Chao; Lee, Sang Uck; Lee, Jung-Ho
- Issue Date
- Jul-2020
- Publisher
- Elsevier BV
- Keywords
- Single atoms; Carbon nitride spheroids; Alkaline reversible zn-air batteries; Robust bifunctional oxygen catalysts; Template-free synthesis strategy; DFT
- Citation
- Applied Catalysis B: Environmental, v.268, pp.1 - 9
- Indexed
- SCIE
SCOPUS
- Journal Title
- Applied Catalysis B: Environmental
- Volume
- 268
- Start Page
- 1
- End Page
- 9
- URI
- https://scholarworks.bwise.kr/hanyang/handle/2021.sw.hanyang/181922
- DOI
- 10.1016/j.apcatb.2020.118746
- ISSN
- 0926-3373
- Abstract
- The rational design of earth-abundant, highly efficient, and robust bifunctional oxygen electrocatalysts remains a contemporary challenge toward the widespread implementation of reversible metal-air batteries and fuel cells. Here, we report a universal strategy for the fabrication of single-atom (Cu, Co, and Fe) incorporated hollow nano-spheroids of nitrogen-deficient carbon nitride frameworks (CuSA@HNCNx. The interconnected three-dimensional 3D porous and hollow robust single-atom spheroid frameworks display a high surface area of 1286 m(2) g(-1), favorable electronic structure, local chemical coordination, effective density of active sites (Cu-N-x pyridinic, graphitic C-N etc.), and mass transport pathways. The obtained CuSA@HNCNx exhibited outstanding bifunctional reversible electrocatalytic activity and robustness for oxygen reduction and evolution reactions (ORR half-wave potential of 0.91 V, OER overpotential of 1.55 V at 10 mA cm(-2), Delta E = 0.64 V, 5000 cycles), outperforming benchmarked Pt/C and RuO2. Electrocatalytic activity towards ORR/OER was analyzed by n-band center correlation using density functional theory (DFT) calculations. Moreover, reversible alkaline Zn-air batteries with the designed CuSA@HNCNx cathode illustrated a high power 212 mW cm(-2), high energy density 1031 Wh kg(zn)(-1), and excellent discharge-charge cycle life of 1800 cycles for 300 h @10 mA cm(-2) with voltaic efficiency of 64.51 %. Notably, all-solid-state flexible ZABs showed long cycle life of 250 h with 1500 cycles at 25 mA cm(-2) with efficiency of 66.31 %. This unique strategy offers controlled design of entangled single-atom frameworks as advanced cathodes for next-generation energy storage technology.
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