TY - JOUR
T1 - Engineering Charge Redistribution within Perovskite Oxides for Synergistically Enhanced Overall Water Splitting
AU - Wang, Xixi
AU - Dai, Jie
AU - Zhou, Chuan
AU - Guan, Daqin
AU - Wu, Xinhao
AU - Zhou, Wei
AU - Shao, Zongping
N1 - Publisher Copyright:
© 2021 American Chemical Society.
PY - 2021/8/2
Y1 - 2021/8/2
N2 - Inexpensive, highly active, durable bifunctional catalysts for both the hydrogen and oxygen evolution reaction (HER and OER) are fundamental for efficient energy conversion. It has been reported that a favorable electronic structure and high electrical conductivity contribute to obtaining superior electrocatalytic activity for perovskites; thus, effective strategies for engineering abundant beneficial factors must be explored to enhance HER and OER. Hence, we report a novel two-step solid-state phase reaction method combined with bulk doping for constructing perovskite LaxSr1-xFe1-20yCo19yPyO3-δ-ab (LSFCP-ab) with modest B-O length and high electrical conductivity. Induced by the strong charge redistribution via Fe4+-O2-x-Co3+, abundant active sites (O22-/O-, Fe4+, Co3+/Co4+), moderate adsorption and desorption energies of the intermediates are obtained during OER and HER. Besides, the activated surface lattice oxygen O2-x could participate in the OER with lattice oxygen-mediated mechanism (LOM). Consequently, the optimal LSFCP-55 exhibits improved intrinsic OER and HER activity than that of La0.2Sr0.8FeO3-δ (LSF). Furthermore, the cell possesses a small cell voltage of 1.57 V with superior durability when it employed as the bifunctional catalyst in overall water splitting. This work provides a novel strategy to engineer beneficial electronic structures over perovskite oxides for sustainable energy conversion.
AB - Inexpensive, highly active, durable bifunctional catalysts for both the hydrogen and oxygen evolution reaction (HER and OER) are fundamental for efficient energy conversion. It has been reported that a favorable electronic structure and high electrical conductivity contribute to obtaining superior electrocatalytic activity for perovskites; thus, effective strategies for engineering abundant beneficial factors must be explored to enhance HER and OER. Hence, we report a novel two-step solid-state phase reaction method combined with bulk doping for constructing perovskite LaxSr1-xFe1-20yCo19yPyO3-δ-ab (LSFCP-ab) with modest B-O length and high electrical conductivity. Induced by the strong charge redistribution via Fe4+-O2-x-Co3+, abundant active sites (O22-/O-, Fe4+, Co3+/Co4+), moderate adsorption and desorption energies of the intermediates are obtained during OER and HER. Besides, the activated surface lattice oxygen O2-x could participate in the OER with lattice oxygen-mediated mechanism (LOM). Consequently, the optimal LSFCP-55 exhibits improved intrinsic OER and HER activity than that of La0.2Sr0.8FeO3-δ (LSF). Furthermore, the cell possesses a small cell voltage of 1.57 V with superior durability when it employed as the bifunctional catalyst in overall water splitting. This work provides a novel strategy to engineer beneficial electronic structures over perovskite oxides for sustainable energy conversion.
UR - http://www.scopus.com/inward/record.url?scp=85111546556&partnerID=8YFLogxK
U2 - 10.1021/acsmaterialslett.1c00359
DO - 10.1021/acsmaterialslett.1c00359
M3 - 文章
AN - SCOPUS:85111546556
SN - 2639-4979
VL - 3
SP - 1258
EP - 1265
JO - ACS Materials Letters
JF - ACS Materials Letters
IS - 8
ER -