TY - JOUR
T1 - Hydrogen spillover in complex oxide multifunctional sites improves acidic hydrogen evolution electrocatalysis
AU - Dai, Jie
AU - Zhu, Yinlong
AU - Chen, Yu
AU - Wen, Xue
AU - Long, Mingce
AU - Wu, Xinhao
AU - Hu, Zhiwei
AU - Guan, Daqin
AU - Wang, Xixi
AU - Zhou, Chuan
AU - Lin, Qian
AU - Sun, Yifei
AU - Weng, Shih-Chang
AU - Wang, Huanting
AU - Zhou, Wei
AU - Shao, Zongping
N1 - Funding Information:
This work was financially supported by National Natural Science Foundation of China under Nos. 21878158 and 21576135, and Priority Academic Program Development (PAPD) of Jiangsu Higher Education Institutions. Y.Z. acknowledges the Australian Research Council (Discovery Early Career Researcher Award No. DE190100005, Discovery Project No. DP200100500), and Z.H. acknowledges the support from the Max Planck-POSTECH-Hsinchu Center for Complex Phase Materials. We also acknowledge the use of instruments and scientific and technical assistance at the Monash Centre for Electron Microscopy, a Node of Microscopy Australia, and the help from Dr. Hassan A. Tahini in DFT calculations.
Publisher Copyright:
© 2022, The Author(s).
PY - 2022/3/4
Y1 - 2022/3/4
N2 - Improving the catalytic efficiency of platinum for the hydrogen evolution reaction is valuable for water splitting technologies. Hydrogen spillover has emerged as a new strategy in designing binary-component Pt/support electrocatalysts. However, such binary catalysts often suffer from a long reaction pathway, undesirable interfacial barrier, and complicated synthetic processes. Here we report a single-phase complex oxide La2Sr2PtO7+δ as a high-performance hydrogen evolution electrocatalyst in acidic media utilizing an atomic-scale hydrogen spillover effect between multifunctional catalytic sites. With insights from comprehensive experiments and theoretical calculations, the overall hydrogen evolution pathway proceeds along three steps: fast proton adsorption on O site, facile hydrogen migration from O site to Pt site via thermoneutral La-Pt bridge site serving as the mediator, and favorable H2 desorption on Pt site. Benefiting from this catalytic process, the resulting La2Sr2PtO7+δ exhibits a low overpotential of 13 mV at 10 mA cm−2, a small Tafel slope of 22 mV dec−1, an enhanced intrinsic activity, and a greater durability than commercial Pt black catalyst.
AB - Improving the catalytic efficiency of platinum for the hydrogen evolution reaction is valuable for water splitting technologies. Hydrogen spillover has emerged as a new strategy in designing binary-component Pt/support electrocatalysts. However, such binary catalysts often suffer from a long reaction pathway, undesirable interfacial barrier, and complicated synthetic processes. Here we report a single-phase complex oxide La2Sr2PtO7+δ as a high-performance hydrogen evolution electrocatalyst in acidic media utilizing an atomic-scale hydrogen spillover effect between multifunctional catalytic sites. With insights from comprehensive experiments and theoretical calculations, the overall hydrogen evolution pathway proceeds along three steps: fast proton adsorption on O site, facile hydrogen migration from O site to Pt site via thermoneutral La-Pt bridge site serving as the mediator, and favorable H2 desorption on Pt site. Benefiting from this catalytic process, the resulting La2Sr2PtO7+δ exhibits a low overpotential of 13 mV at 10 mA cm−2, a small Tafel slope of 22 mV dec−1, an enhanced intrinsic activity, and a greater durability than commercial Pt black catalyst.
UR - http://www.scopus.com/inward/record.url?scp=85125791950&partnerID=8YFLogxK
U2 - 10.1038/s41467-022-28843-2
DO - 10.1038/s41467-022-28843-2
M3 - Article
C2 - 35246542
AN - SCOPUS:85125791950
VL - 13
JO - Nature Communications
JF - Nature Communications
SN - 2041-1723
IS - 1
M1 - 1189
ER -
