Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 276, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2020.119172
Keywords
Holey graphene; Single-atom Mo; defects/edges; Oxygen reduction reaction; Oxygen evolution reaction
Funding
- National Natural Science Foundation of China [51702031, 51871077, 61704096]
- Shenzhen Fundamental Research Program [JCYJ20180306171644942, JCYJ20180507184623297, KQJSCX20180328165656256]
- JSPS [JP18H04477, JP 20H04628]
- JSPS KAKENHI of MEXT, Japan [JP18K14174]
- Japanese government (MONBUKAGAKUSHO: MEXT) scholarship
- Sasakawa Scientific Research Grant from the Japan Science Society
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Materials co-design of the single-atom catalytic centers and the supports can push the limits of the emerging wearable metal-air batteries. The metal single-atom catalysts are required to be bifunctional with high efficient electrocatalytic activities for both oxygen reduction and evolution reactions (ORR and OER), and preferably non-noble. The supports, on the other hand, in addition to the requirements of being free-standing, flexible and porous, are required to strongly interact with the metal species to prevent their aggregation. However, satisfying these requirements simultaneously is yet challenging. Here, a free-standing 3D nanoporous holey graphene with both N and single-atom Mo dopants is prepared. The nanoholes are created by chemical vapor deposition method on nanoporous NiMo alloy templates with their surface decorated with catalytically inert SiO2 nanoparticles. The edge-rich graphene induced by the nanoholes facilitates the doping of pyridinic N and single-atom Mo in the fringe near the edges. The resulting N and Mo co-doped nanoporous holey graphene exhibits high bifunctional ORR and OER catalytic activities in alkaline electrolytes. The synergetic effects between N and Mo dopants are also revealed by density functional theory calculations. When incorporated in a solid-state zinc-air battery, the battery is bendable and can be continuously discharged/charged for 88 h with a high power density of 83 mW cm(-2). This work provides an efficient route to design metal single atom/cluster doped 3D freestanding nanoporous graphene as flexible electrodes.
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