过电位
杂原子
电催化剂
材料科学
催化作用
自旋态
氟
钙钛矿(结构)
兴奋剂
纳米技术
化学物理
化学
无机化学
物理化学
结晶学
光电子学
电极
有机化学
戒指(化学)
冶金
电化学
作者
Jiaqi Ran,Linchuan Wang,Mingsu Si,Xiaolei Liang,Daqiang Gao
出处
期刊:Small
[Wiley]
日期:2022-12-21
卷期号:19 (10)
被引量:13
标识
DOI:10.1002/smll.202206367
摘要
Promoting the initially deficient but economical catalysts to high-performing competitors is important for developing superior catalysts. Unlike traditional nano-morphology construction methods, this work focuses on intrinsic catalytic activity enhancement via heteroatom doping strategies to induce lattice distortion and optimize spin-dependent orbital interaction to alter charge transfer between catalysts and reactants. Experimentally, a series of different concentrations of fluorine-doped lanthanum cobaltate (Fx -LaCoO3 ) exhibiting excellent electrocatalytic activity is synthesized, including a low overpotential of 390 mV at j = 10 mA cm-2 for OER and a large half-wave potential of 0.68 V for ORR. Meanwhile, the assembled rechargeable Zn-air batteries deliver an excellent performance with a large specific capacity of 811 mAh/gZn under 10 mA cm-2 and stability of charge/recharge (120 h). Theoretically, taking advantage of density functional theory calculations, it is found that the prominent OER/ORR performance arises from the spin state transition of Co3+ (Low spin state (LS, t2g6 eg0 ) → Intermediate spin state (IS, t2g5 eg1 ) and the mediated d-band center upshift by F atom incorporation. This work establishes a novel avenue for designing superior electrocatalysts in perovskite-based oxides by regulating spin states.
科研通智能强力驱动
Strongly Powered by AbleSci AI