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Gadolinium‐Induced Valence Structure Engineering for Enhanced Oxygen Electrocatalysis
Author(s) -
Li Meng,
Wang Yu,
Zheng Yang,
Fu Gengtao,
Sun Dongmei,
Li Yafei,
Tang Yawen,
Ma Tianyi
Publication year - 2020
Publication title -
advanced energy materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.08
H-Index - 220
eISSN - 1614-6840
pISSN - 1614-6832
DOI - 10.1002/aenm.201903833
Subject(s) - gadolinium , materials science , electrocatalyst , valence (chemistry) , density functional theory , nanoparticle , catalysis , heterojunction , oxygen , doping , graphene , nanotechnology , chemical engineering , analytical chemistry (journal) , chemistry , electrode , computational chemistry , electrochemistry , optoelectronics , biochemistry , organic chemistry , engineering , metallurgy , chromatography
Rare earth doped materials with unique electronic ground state configurations are considered emerging alternatives to conventional Pt/C for the oxygen reduction reaction (ORR). Herein, gadolinium (Gd)‐induced valence structure engineering is, for the first, time investigated for enhanced oxygen electrocatalysis. The Gd 2 O 3 –Co heterostructure loaded on N‐doped graphene (Gd 2 O 3 –Co/NG) is constructed as the target catalyst via a facile sol–gel assisted strategy. This synthetic strategy allows Gd 2 O 3 –Co nanoparticles to distribute uniformly on an N‐graphene surface and form intimate Gd 2 O 3 /Co interface sites. Upon the introduction of Gd 2 O 3 , the ORR activity of Gd 2 O 3 –Co/NG is significantly increased compared with Co/NG, where the half‐wave potential (E 1/2 ) of Gd 2 O 3 –Co/NG is 100 mV more positive than that of Co/NG and even close to commercial Pt/C. The density functional theory calculation and spectroscopic analysis demonstrate that, owing to intrinsic charge redistribution at the engineered interface of Gd 2 O 3 /Co, the coupled Gd 2 O 3 –Co can break the OOH*–OH* scaling relation and result in a good balance of OOH* and OH* binding on Gd 2 O 3 –Co surface. For practical application, a rechargeable Zn–air battery employing Gd 2 O 3 –Co/NG as an air–cathode achieves a large power density and excellent charge–discharge cycle stability.