Polymer materials offer controllable structure-dependent performances in separation,catalysis and drug release.Their molecular structures can be precisely tailored to accept Li^(+)for energy storage applications.Here ...Polymer materials offer controllable structure-dependent performances in separation,catalysis and drug release.Their molecular structures can be precisely tailored to accept Li^(+)for energy storage applications.Here the design of sp^(2)carbon-based polyphenylene(PPH)with high lithium-ion uptakes and long-term stability is reported.Linear-PPH(L-PPH)exceeds the performance of crosslink-PPH(C-PPH),due to the fact that it has an ordered lamellar structure,promoting the Li^(+)intercalation/deintercalation channel.The L-PPH cell shows a clear charge and discharge plateau at 0.35 and 0.15 V vs.Li^(+)/Li,respectively,which is absent in the C-PPH cell.The Li^(+)storage capacity of L-PPH is five times that of the C-PPH.The reversible storage capacity is further improved to 261 m Ah g;by functionalizing the L-PPH with the–SO_(3)H groups.In addition,the Li-intercalated structures of C-PPH and L-PPH are investigated via near-edge X-ray absorption fine structure(NEXAFS),suggesting the high reversible Li^(+)–C=C bond interaction at L-PPH.This strategy,based on new insight into sp^(2)functional groups,is the first step toward a molecular understanding of the structure storage-capacity relationship in sp^(2)carbon-based polymer.展开更多
基金funded by the Engineering and Physical Sciences Research Council(EPSRC)(EP/P02467X/1 and EP/S018204/1)the Centre for Nature Inspired Chemical Engineering(EP K038656/1)。
文摘Polymer materials offer controllable structure-dependent performances in separation,catalysis and drug release.Their molecular structures can be precisely tailored to accept Li^(+)for energy storage applications.Here the design of sp^(2)carbon-based polyphenylene(PPH)with high lithium-ion uptakes and long-term stability is reported.Linear-PPH(L-PPH)exceeds the performance of crosslink-PPH(C-PPH),due to the fact that it has an ordered lamellar structure,promoting the Li^(+)intercalation/deintercalation channel.The L-PPH cell shows a clear charge and discharge plateau at 0.35 and 0.15 V vs.Li^(+)/Li,respectively,which is absent in the C-PPH cell.The Li^(+)storage capacity of L-PPH is five times that of the C-PPH.The reversible storage capacity is further improved to 261 m Ah g;by functionalizing the L-PPH with the–SO_(3)H groups.In addition,the Li-intercalated structures of C-PPH and L-PPH are investigated via near-edge X-ray absorption fine structure(NEXAFS),suggesting the high reversible Li^(+)–C=C bond interaction at L-PPH.This strategy,based on new insight into sp^(2)functional groups,is the first step toward a molecular understanding of the structure storage-capacity relationship in sp^(2)carbon-based polymer.
