摘要
The two-dimensional layered double hydroxides(LDHs)and zero-dimensional metal clusters have emerged as promising nanomaterials in the field of sustainable water oxidation,which can also facilitate joint experimental and computational studies.In this study,the synthesis of Ni_(6)@LDH composites,comprising atomically precise Ni_(6)(MPA)12(MPA:mercaptopropionic acid)clusters embedded into LDH nanosheets via electrostatic interaction,represents a significant advancement in the development of nanomaterials for sustainable water oxidation.Ni_(6)@NiFe-LDH exhibits superior electrochemical performance in oxygen evolution reaction(OER),exhibiting OER overpotentials of 198 mV@10 mA·cm^(-2) and 290 mV@100 mA·cm^(-2) with a low Tafel slope of 29 mV·dec^(-1).It surpasses the corresponding NiFe-LDH and commercial RuO_(2) catalysts,primarily due to the synergistic interaction between Ni_(6) clusters and LDHs.Interestingly,our combined experimental and computational approach reveals that the M-OOH_(ads )formation is the rate-determining step(RDS)for the Ni_(6)-based catalysts,differing from the RDS for NiFe-LDH itself(the M-Oads formation).These efforts serve as an attempt to push forward the current research frontier to study structure–property relationships progressing from the micro-/nano-level to the precise atomic-level.
基金
Natural Science Foundation of China(No.22172167).
