作为微电子器件的理想电源,全固态薄膜锂电池(TFB)已经被广泛地研究了几十年,并开始进入商业化应用。然而,目前关于失效TFB的回收与再利用的研究几乎没有,这将会阻碍TFB的可持续发展。本工作针对因金属锂负极失效而造成电池失效的TFB,...作为微电子器件的理想电源,全固态薄膜锂电池(TFB)已经被广泛地研究了几十年,并开始进入商业化应用。然而,目前关于失效TFB的回收与再利用的研究几乎没有,这将会阻碍TFB的可持续发展。本工作针对因金属锂负极失效而造成电池失效的TFB,提出了一种简单的基于最常见LiCoO_(2)(LCO)/LiPON/LiTFB(F-TFB)的直接回收再利用的方法。研究发现,F-TFB中的金属锂负极薄膜在循环过程会被部分氧化从而造成电池失效。我们提出利用无水乙醇溶液有效地溶解并去除F-TFB上失效的金属锂负极部分,从而快速地回收底层的LCO/LiPON薄膜。结构分析和表面分析结果表明,回收的LCO/LiPON薄膜中的LCO正极的晶体结构、LCO/LiPON的界面结构以及LiPON电解质的表面保持完好,使其再利用成为了可能。进一步地,我们在回收的LCO/LiPON薄膜上依次沉积了LiPON和Li薄膜,构建得到了电化学性能恢复的LCO/LiPON/LiTFB,并获得了与新制备的TFB相一致的比容量(0.223 m Ah·cm^(-2))、良好的倍率性能和循环寿命(500次循环后容量保持率为77.3%)。这种简单而有效的回收再利用方法有望延长固态电池的使用寿命,减少能源和资源消耗,促进固态电池的可持续发展。展开更多
Compared with the planar two-dimensional(2D)all-solid-state thin film batteries(TFBs),threedimensional(3D)all-solid-state TFBs with interdigitated contact between electrode and electrolyte possess great advantage in a...Compared with the planar two-dimensional(2D)all-solid-state thin film batteries(TFBs),threedimensional(3D)all-solid-state TFBs with interdigitated contact between electrode and electrolyte possess great advantage in achieving both high energy and power densities.Herein,we report a facile fabrication of vertically aligned oxygen-deficient a-MoO3-x nanoflake arrays(3D MO_(x))using metal Mo target by direct current(DC)magnetron sputtering.By utilizing the 3D MO_(x)cathode,amorphous lithium phosphorus oxynitride solid electrolyte,and lithium thin film anode,3D solid-state TFBs have been successfully fabricated,exhibiting high specific capacity(266 mAh g^(-1)at 50 mA g^(-1)),good rate performance(110 mAh g^(-1)at 1000mA g^(-1)),and excellent cycle performance(92.7%capacity retention after 1000 cycles)in comparison with the 2D TFBs using the planar MO_(x)thin film as cathode.The superior electrochemical performance of the 3D TFBs can be attributed to the 3D architecture of the cathode,maximizing the cathode/electrolyte interface while retaining the short Lit diffusion length.The charge/discharge measurements of the 3D MO_(x)cathode in liquid electrolyte,however,exhibit fast capacity fading,demonstrating the advantage of using transition metal oxide as cathode in solid-state batteries.展开更多
Layered lithium manganese-rich oxides are promising cathode materials for lithium-ion batteries(LIBs),due to the low-cost,abundant manganese source,and large theoretical capacity.However,these layered lithium manganes...Layered lithium manganese-rich oxides are promising cathode materials for lithium-ion batteries(LIBs),due to the low-cost,abundant manganese source,and large theoretical capacity.However,these layered lithium manganese-rich oxides,e.g.,monoclinic-LiMn0_(2),suffer from poor cycle performance and rate performance because of fast structural degradation with the irreversible layered-to-spinel phase transition and sluggish electrode kinetics during cycling[1,2].展开更多
文摘作为微电子器件的理想电源,全固态薄膜锂电池(TFB)已经被广泛地研究了几十年,并开始进入商业化应用。然而,目前关于失效TFB的回收与再利用的研究几乎没有,这将会阻碍TFB的可持续发展。本工作针对因金属锂负极失效而造成电池失效的TFB,提出了一种简单的基于最常见LiCoO_(2)(LCO)/LiPON/LiTFB(F-TFB)的直接回收再利用的方法。研究发现,F-TFB中的金属锂负极薄膜在循环过程会被部分氧化从而造成电池失效。我们提出利用无水乙醇溶液有效地溶解并去除F-TFB上失效的金属锂负极部分,从而快速地回收底层的LCO/LiPON薄膜。结构分析和表面分析结果表明,回收的LCO/LiPON薄膜中的LCO正极的晶体结构、LCO/LiPON的界面结构以及LiPON电解质的表面保持完好,使其再利用成为了可能。进一步地,我们在回收的LCO/LiPON薄膜上依次沉积了LiPON和Li薄膜,构建得到了电化学性能恢复的LCO/LiPON/LiTFB,并获得了与新制备的TFB相一致的比容量(0.223 m Ah·cm^(-2))、良好的倍率性能和循环寿命(500次循环后容量保持率为77.3%)。这种简单而有效的回收再利用方法有望延长固态电池的使用寿命,减少能源和资源消耗,促进固态电池的可持续发展。
基金This work was supported by National Natural Science Foundation of China(No.51572129,51772154,51811530100)International S&T Cooperation Program of China(No.2016YFE0111500)+1 种基金Natural Science Foundation of Jiangsu Province(No.BK20170036)SEM and XRD experiment was performed at the Materials Characterization Facility of Nanjing University of Science and Technology.
文摘Compared with the planar two-dimensional(2D)all-solid-state thin film batteries(TFBs),threedimensional(3D)all-solid-state TFBs with interdigitated contact between electrode and electrolyte possess great advantage in achieving both high energy and power densities.Herein,we report a facile fabrication of vertically aligned oxygen-deficient a-MoO3-x nanoflake arrays(3D MO_(x))using metal Mo target by direct current(DC)magnetron sputtering.By utilizing the 3D MO_(x)cathode,amorphous lithium phosphorus oxynitride solid electrolyte,and lithium thin film anode,3D solid-state TFBs have been successfully fabricated,exhibiting high specific capacity(266 mAh g^(-1)at 50 mA g^(-1)),good rate performance(110 mAh g^(-1)at 1000mA g^(-1)),and excellent cycle performance(92.7%capacity retention after 1000 cycles)in comparison with the 2D TFBs using the planar MO_(x)thin film as cathode.The superior electrochemical performance of the 3D TFBs can be attributed to the 3D architecture of the cathode,maximizing the cathode/electrolyte interface while retaining the short Lit diffusion length.The charge/discharge measurements of the 3D MO_(x)cathode in liquid electrolyte,however,exhibit fast capacity fading,demonstrating the advantage of using transition metal oxide as cathode in solid-state batteries.
基金the National Natural Science Foundation of China(51972174,51772154,and 51702164)Natural Science Foundation of Jiangsu Province(BK20170036 and BK20170844)the Six Talent Peaks Project of Jiangsu Province(2018-XNY-025)。
文摘Layered lithium manganese-rich oxides are promising cathode materials for lithium-ion batteries(LIBs),due to the low-cost,abundant manganese source,and large theoretical capacity.However,these layered lithium manganese-rich oxides,e.g.,monoclinic-LiMn0_(2),suffer from poor cycle performance and rate performance because of fast structural degradation with the irreversible layered-to-spinel phase transition and sluggish electrode kinetics during cycling[1,2].
