Journal
ADVANCED MATERIALS
Volume 34, Issue 42, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202206540
Keywords
4f electrons; e; (g) occupancy; Eu; O-2; (3)-Co; gradient orbital coupling; oxygen reduction reaction
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Funding
- National Natural Science Foundation of China [22109073, 22072067]
- Natural Science Foundation of Jiangsu Province [BK20221321]
- National and Local Joint Engineering Research Center of Biomedical Functional Materials
- Priority Academic Program Development of Jiangsu Higher Education Institutions
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This study proposes a novel gradient orbital coupling strategy to tune the performance of the oxygen reduction reaction (ORR). The optimized catalyst shows higher onset and half-wave potentials compared to commercial catalysts and exhibits superior selectivity and durability. It also demonstrates better performance in Zn-air batteries compared to noble-metal catalysts in terms of power/energy densities and cycle life.
The development of highly efficient and economical materials for the oxygen reduction reaction (ORR) plays a key role in practical energy conversion technologies. However, the intrinsic scaling relations exert thermodynamic inhibition on realizing highly active ORR electrocatalysts. Herein, a novel and feasible gradient orbital coupling strategy for tuning the ORR performance through the construction of Co 3d-O 2p-Eu 4f unit sites on the Eu2O3-Co model is proposed. Through the gradient orbital coupling, the pristine ionic property between Eu and O atoms is assigned with increased covalency, which optimizes the e(g) occupancy of Co sites, and weakens the O(sic)O bond, thus ultimately breaking the scaling relation between *OOH and *OH at Co-O-Eu unit sites. The optimized model catalyst displays onset and half-wave potential of 1.007 and 0.887 V versus reversible hydrogen electrode, respectively, which are higher than those of commercial Pt/C and most Co-based catalysts ever reported. In addition, the catalyst is found to possess superior selectivity and durability. It also reveals better cell performance than commercial noble-metal catalysts in Zn-air batteries in terms of high power/energy densities and long cycle life. This study provides a new perspective for electronic modulation strategy by the construction of gradient 3d-2p-4f orbital coupling.
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