Sodium-ion batteries(SIBs)have emerged as a promising contender for next-gener-ation energy storage systems.Hard carbon is re-garded as the most promising anode for commer-cial SIB,however,the large number of defects ...Sodium-ion batteries(SIBs)have emerged as a promising contender for next-gener-ation energy storage systems.Hard carbon is re-garded as the most promising anode for commer-cial SIB,however,the large number of defects on its surface cause irreversible electrolyte consump-tion and an uneven solid electrolyte interphase film.An advanced molecular engineering strategy to coat hard carbon with polycyclic aromatic mo-lecules is reported.Specifically,polystyrene-based carbon microspheres(CSs)were first synthesized and then coated with polycyclic aromatic mo-lecules derived from coal tar pitch by spray-drying and followed by oxidation.Compared to the traditional CVD coating meth-od,this molecular framework strategy has been shown to reduce the number of defects on the surface of CSs without sacrifi-cing internal storage sites and suppressing transport kinetics in hosting the sodium ions.Besides the lower surface defect con-centration,the synthesized hybrid carbon microspheres(HCSs)have a larger grain size and more abundant closed pores,and have a higher reversible sodium storage capacity.A HCS-P-60%electrode has a capacity of 332.3 mAh g^(-1)with an initial Cou-lombic efficiency of 88.5%.It also has a superior rate performance of 246.6 mAh g^(-1)at 2 C and a 95.2%capacity retention after 100 cycles at 0.2 C.This work offers new insights into designing high-performance hard carbon microsphere anodes,advan-cing the commercialization of sodium-ion batteries.展开更多
文摘Sodium-ion batteries(SIBs)have emerged as a promising contender for next-gener-ation energy storage systems.Hard carbon is re-garded as the most promising anode for commer-cial SIB,however,the large number of defects on its surface cause irreversible electrolyte consump-tion and an uneven solid electrolyte interphase film.An advanced molecular engineering strategy to coat hard carbon with polycyclic aromatic mo-lecules is reported.Specifically,polystyrene-based carbon microspheres(CSs)were first synthesized and then coated with polycyclic aromatic mo-lecules derived from coal tar pitch by spray-drying and followed by oxidation.Compared to the traditional CVD coating meth-od,this molecular framework strategy has been shown to reduce the number of defects on the surface of CSs without sacrifi-cing internal storage sites and suppressing transport kinetics in hosting the sodium ions.Besides the lower surface defect con-centration,the synthesized hybrid carbon microspheres(HCSs)have a larger grain size and more abundant closed pores,and have a higher reversible sodium storage capacity.A HCS-P-60%electrode has a capacity of 332.3 mAh g^(-1)with an initial Cou-lombic efficiency of 88.5%.It also has a superior rate performance of 246.6 mAh g^(-1)at 2 C and a 95.2%capacity retention after 100 cycles at 0.2 C.This work offers new insights into designing high-performance hard carbon microsphere anodes,advan-cing the commercialization of sodium-ion batteries.