UltrafastsodiumstorageofalkylaminemoleculetailoredMnPS3enabledbyquasi-topologicalintercalationmechanism<iclass="icon-zqcb"></i>

Two-dimensional transition metal trithiophosphates（TMPS3,TM=Mn,Fe,Co,etc.） are competitive anode materials for sodium-ion batteries（SIBs） due to their high theoretical capacity(>1,300 mAh g-1) but suffer from limited practical capacity(～300 mAh g-1) and inferior rate capability caused by sluggish Na+intercalation/deintercalation kinetics and severe structural collapse.Herein,alkylamine molecules are first proposed as intercalation guests to significantly boost the electrochemical activity and stability of MnPS3.Compared to MnPS3,C3H9N-MnPS3enlarges the interlayer spacing from 6.48 to 10.23? and shows a 10～5 times higher electrical conductivity,which provides fast ion/electron transport and high strain adaptability,realizing a quasi-topological Na+intercalation mechanism.Consequently,C3H9N-MnPS3 exhibits an ultrahigh reversible capacity of 775 mAh g-1at 0.5 A g-1and superior high-rate cycling stability with～100%capacity retention after 2,500 cycles at 15 A g-1,ranking it among the top metal trithiophosphate-based anode materials reported.Theoretical calculations indicate that the improved sodium storage performance of C3H9N-MnPS3 results from the reduced bonding energy of P–S bonds and increased adsorption energy of Na+.This work is expected to provide an efficient strategy for the design of high-performance layered anode materials for SIBs.