摘要
The development of high-efficiency and cost-effective bifunctional electrocatalysts for overall water splitting remains a formidable challenge.Herein,FeNi-Nd_(2)O_(3) nanoparticles anchored on N-doped carbon nanotubes(FeNi-Nd_(2)O_(3)/NCN) are designed for highly effective overall water splitting via a facile two-step hydrothermal approach.The synthetic FeNi-Nd_(2)O_(3) hetero-trimers(Fe 2p-Ni 2p-Nd 3d orbital coupling)on NCN achieve excellent oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) activities with overpotentials of 270 and 120 mV at 10 mA cm^(-2) in 1 M KOH solution.Moreover,a small voltage of 1.52 V at 10 mA cm^(-2) is achieved when FeNi-Nd_(2)O_(3)/NCN is assessed as bifunctional catalyst for overall water splitting,which is superior to the typically integrated Pt/C and RuO_(2) counterparts(1.54 V at 10 mA cm^(-2)).The related characterizations including X-ray absorption fine structure(XAFS)spectroscopy show that the remarkably improved activity is originated from Nd_(2)O_(3)-induced FeNi bimetallic lattice contraction.Furthermore,density functional theory(DFT) calculations indicate that the lattice contraction reduces binding energies of intermediates by downshifting the position of FeNi bimetallic d-band center relative to the Fermi level to optimize catalytic performance.Therefore,the Nd_(2)O_(3)-induced FeNi bimetallic lattice contraction may provide a new perspective for designing and synthesizing innovative catalytic systems.
基金
supported by the National Natural Science Foundation of China (NSFC) (52171206, 51762013)
the Key Project of Hebei Natural Science Foundation (E20202201030)
the BeijingTianjin-Hebei Collaborative Innovation Community Construction Project (21344301D)
The Second Batch of Young Talent of Hebei Province (70280016160250, 70280011808)
the Key Fund in Hebei Province Department of Education China (ZD2021014)
The Central Government Guide Local Funding Projects for Scientific and Technological Development (216Z4404G, 206Z4402G)
the Interdisciplinary Research Program of Natural Science of Hebei University (DXK202107)
the China Postdoctoral Science Foundation (No. 2021M701718)。
