Oxygen
electrocatalysts are crucial for the development of renewable
and sustainable energy conversion/storage (ECS) systems, but a shortage
of efficient and low-cost oxygen electrocatalysts is impeding their
widespread applications. In this work, to investigate the bifunctionality
of the oxygen reduction reaction (ORR) and the oxygen evolution reaction
(OER), Ni-substituted LaMnO3 perovskite oxides (LaNi
x
Mn1–x
O3, x = 0.1, 0.3, 0.5, 0.7, and 0.9) and pristine
LaNiO3 and LaMnO3 were synthesized using a sol–gel
process. After the compositional optimization and electrochemical
characterizations, we identified that LaNi0.3Mn0.7O3 (SG LNM-3) within the compositions exhibited balanced
intrinsic activity for bifunctional ORR and OER. To further improve
the apparent activity of the optimized SG LNM-3, electrospinning was
used to prepare one-dimensional nanostructured LaNi0.3Mn0.7O3 (ES LNM-3). ES LNM-3 had a higher specific
surface area and continuous electron-transfer pathways, resulting
in much improved bifunctional activity in comparison to SG LNM-3.
In addition to the morphological effect, we ascribed the high electrochemical
performance of ES LNM-3 to the high-spin Mn3+ and low-spin
Ni3+ with electron configurations of t2g
3eg
1 and t2g
6eg
1 (a well-recognized design descriptor), as well
as the high degree of Jahn–Teller distortion. After assembling
ES LNM-3 within Zn–air batteries, promising electrochemical
performances such as high power density and rate capability were obtained.
Our findings will advance the development of high-performance and
inexpensive oxygen electrocatalysts and associated ECS devices.