With the proliferation of energy storage and power applications, electric vehicles particularly, solid-state batteries are considered as one of the most promising strategies to address the ever-increasing safety conce...With the proliferation of energy storage and power applications, electric vehicles particularly, solid-state batteries are considered as one of the most promising strategies to address the ever-increasing safety concern and high energy demand of power devices. Here, we demonstrate the Al4B2O9 nanorods-modified poly(ethylene oxide) (PEO)-based solid polymer electrolyte (ASPE) with high ionic conductivity, wide electrochemical window, decent mechanical property and nonflammable performance. Specifically, because of the longer-range ordered Li+ transfer channels conducted by the interaction between Al4B2O9 nanorods and PEO, the optimal ASPE (ASPE-1) shows excellent ionic conductivity of 4.35×10^−1 and 3.1×10^−1 S cm^−1 at 30 and 60℃, respectively. It also has good electrochemical stability at 60℃ with a decomposition voltage of 5.1 V. Besides, the assembled LiFePO4//Li cells show good cycling performance, delivering 155 mA h g−1 after 300 cycles at 1 C under 60℃, and present excellent low temperature adaptability, retaining over 125 mA h g^−1 after 90 cycles at 0.2 C under 30℃. These results verify that the addition of Al4B2O9 nanorods can effectively promote the integrated performance of solid polymer electrolyte.展开更多
Solid-state lithium-metal-batteries(SSLMBs)using garnet Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO)as the solid electrolyte are expected to conquer the safety concerns of high energy Li batteries with organic liquid e...Solid-state lithium-metal-batteries(SSLMBs)using garnet Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO)as the solid electrolyte are expected to conquer the safety concerns of high energy Li batteries with organic liquid electrolytes owing to its nonflammable nature and good mechanical strength.However,the poor interfacial contact between the Li anode and LLZTO greatly restrains the practical applications of the electrolyte,because large polarization,dendritic Li formation and penetration can occur at the interfaces.Here,an effective method is proposed to improve the wettability of the LLZTO toward lithium and reduce the interfacial resistance by engineering universal lithiophilic interfacial layers.Thanks to the in-situ formed lithiophilic and ionic conductive Co/Li_(2)O interlayers,the symmetric Li/CoO-LLZTO/Li batteries present much smaller overpotential,ultra-low areal specific resistance(ASR,12.3 X cm^(2)),high critical current density(CCD,1.1 mA cm^(-2)),and outstanding cycling performance(1696 h at a current density of 0.3 mA cm^(-2))at 25℃.Besides,the solid-state Li/CoO-LLZTO/LFP cells deliver an excellent electrochemical performance with a high coulombic efficiency of~100%and a long cycling time over 185 times.Surprisingly,the high-voltage(4.6 V)solid state Li/CoO-LLZTO/Li_(1.4)Mn_(0.6)Ni_(0.2)Co_(0.2)O_(2.4)(LMNC622)batteries can also realize an ultra-high specific capacity(232.5 mAh g-1)under 0.1 C at 25℃.This work paves an effective way for practical applications of the dendrite-free SSLMBs.展开更多
基金financially supported by the National Natural Science Foundation of China (52072196, 52002199, 52002200, and 52102106)the Major Basic Research Program of Natural Science Foundation of Shandong Province (ZR2020ZD09)+4 种基金the Natural Science Foundation of Shandong Province (ZR2019BEM042 and ZR2020QE063)the Innovation and Technology Program of Shandong Province (2020KJA004)the Open Project of Chemistry Department of Qingdao University of Science and Technology (QUSTHX201813)the Postdoctoral Innovation Project of Shandong Province (202101020)Taishan Scholars Program of Shandong Province (ts201511034)。
基金financially supported by the National Natural Science Foundation of China (51804344)the Huxiang Youth Talent Support Program (2019RS2002)+2 种基金the Innovation and Entrepreneurship Project of Hunan Province,China (2018GK5026)the Innovation-Driven Project of Central South University (2020CX027)Guangdong Yang Fan Plan for Postdoctor Program
文摘With the proliferation of energy storage and power applications, electric vehicles particularly, solid-state batteries are considered as one of the most promising strategies to address the ever-increasing safety concern and high energy demand of power devices. Here, we demonstrate the Al4B2O9 nanorods-modified poly(ethylene oxide) (PEO)-based solid polymer electrolyte (ASPE) with high ionic conductivity, wide electrochemical window, decent mechanical property and nonflammable performance. Specifically, because of the longer-range ordered Li+ transfer channels conducted by the interaction between Al4B2O9 nanorods and PEO, the optimal ASPE (ASPE-1) shows excellent ionic conductivity of 4.35×10^−1 and 3.1×10^−1 S cm^−1 at 30 and 60℃, respectively. It also has good electrochemical stability at 60℃ with a decomposition voltage of 5.1 V. Besides, the assembled LiFePO4//Li cells show good cycling performance, delivering 155 mA h g−1 after 300 cycles at 1 C under 60℃, and present excellent low temperature adaptability, retaining over 125 mA h g^−1 after 90 cycles at 0.2 C under 30℃. These results verify that the addition of Al4B2O9 nanorods can effectively promote the integrated performance of solid polymer electrolyte.
基金supported by the National Natural Science Foundation of China (21603019 and 201503025)Program for the Hundred Talents Program of Chongqing University。
文摘Solid-state lithium-metal-batteries(SSLMBs)using garnet Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO)as the solid electrolyte are expected to conquer the safety concerns of high energy Li batteries with organic liquid electrolytes owing to its nonflammable nature and good mechanical strength.However,the poor interfacial contact between the Li anode and LLZTO greatly restrains the practical applications of the electrolyte,because large polarization,dendritic Li formation and penetration can occur at the interfaces.Here,an effective method is proposed to improve the wettability of the LLZTO toward lithium and reduce the interfacial resistance by engineering universal lithiophilic interfacial layers.Thanks to the in-situ formed lithiophilic and ionic conductive Co/Li_(2)O interlayers,the symmetric Li/CoO-LLZTO/Li batteries present much smaller overpotential,ultra-low areal specific resistance(ASR,12.3 X cm^(2)),high critical current density(CCD,1.1 mA cm^(-2)),and outstanding cycling performance(1696 h at a current density of 0.3 mA cm^(-2))at 25℃.Besides,the solid-state Li/CoO-LLZTO/LFP cells deliver an excellent electrochemical performance with a high coulombic efficiency of~100%and a long cycling time over 185 times.Surprisingly,the high-voltage(4.6 V)solid state Li/CoO-LLZTO/Li_(1.4)Mn_(0.6)Ni_(0.2)Co_(0.2)O_(2.4)(LMNC622)batteries can also realize an ultra-high specific capacity(232.5 mAh g-1)under 0.1 C at 25℃.This work paves an effective way for practical applications of the dendrite-free SSLMBs.