The incomplete sulfur reduction and high ZnS re-oxidation energy barrier along with severe side reactions during the battery cycling compromise the practical application of Zn–S electrochemistry. Herein, a bifunction...The incomplete sulfur reduction and high ZnS re-oxidation energy barrier along with severe side reactions during the battery cycling compromise the practical application of Zn–S electrochemistry. Herein, a bifunctional electrocatalytic sulfur matrix that simultaneously accelerates the sulfur reduction and ZnS oxidation is proposed to realize a highly-efficient Zn–S cell. It is revealed that the N-heteroatom hotspots are more favorable for facilitating the conversion of S to ZnS while the CoO nanocrystal substantially lowers the ZnS activation energy barrier thereby suppressing the formation of disproportionation species(e.g.,SO_(4)^(2-)) and accumulation of inactive ZnS. Accordingly, the Co O anchored on the N-doped carbon-supported sulfur cathode delivers a high Zn^(2+)storage capacity of 1,172 m Ahg^(-1)and outstanding cycling stability with a capacity retention of 71.6% after500 cycles with a high average Coulombic efficiency of 97.8%. Simultaneously, the stable cycling of solid-state Zn–S pouch cells with an energy density of 585 Whkg^(-1)sulfuris also demonstrated. Moreover, the postmortem analysis reveals that the degradation of Zn–S cells is mainly attributed to the limited reversibility of Zn anodes rather than the ZnS decomposition and/or accumulation. The approach to the bidirectional catalysis manipulated the sulfur redox provides a new perspective to realize the theoretical potentials of Zn–S cells.展开更多
以ZnCl_(2)为硬模板和锌源,三聚氰胺和硫脲为氮源和硫源,废弃生物质橘子皮为碳源,通过高温烧结和后续蚀刻处理制备出硫化锌纳米点与三维N-S共掺杂炭纳米片的纳米复合材料(ZnS/NS-CN)。当应用于锂离子电池时,ZnS/NSCN表现出较高的可逆容...以ZnCl_(2)为硬模板和锌源,三聚氰胺和硫脲为氮源和硫源,废弃生物质橘子皮为碳源,通过高温烧结和后续蚀刻处理制备出硫化锌纳米点与三维N-S共掺杂炭纳米片的纳米复合材料(ZnS/NS-CN)。当应用于锂离子电池时,ZnS/NSCN表现出较高的可逆容量(0.1 A g^(−1)下,循环300次后容量仍有853.5 mAh g^(−1)),优异的长期循环稳定性(5 A g^(−1)下,循环1000次后,容量保持率为70.1%)和优异的倍率性能。此外,在0.5~4 V下组装和测试的ZnS/NS-CN//LiNiCoMnO2全电池表现出优异的电池性能(在0.2 C下循环150次后容量为140.4 mAh g^(−1),能量密度为132.4 Wh kg^(−1))。展开更多
制备了Mn掺杂Zn-In-S量子点并研究了Zn/In的量比和反应温度对其发光性质的影响。在Mn掺杂的Zn-In-S量子点的发光谱中观测到一个600 nm发光带。通过改变Zn/In的量比,掺杂量子点的吸收带隙可从3.76 e V(330 nm)调谐到2.82 e V(440 nm),但6...制备了Mn掺杂Zn-In-S量子点并研究了Zn/In的量比和反应温度对其发光性质的影响。在Mn掺杂的Zn-In-S量子点的发光谱中观测到一个600 nm发光带。通过改变Zn/In的量比,掺杂量子点的吸收带隙可从3.76 e V(330 nm)调谐到2.82 e V(440 nm),但600 nm发光峰的波长只有略微移动。这些掺杂量子点的最长荧光寿命为2.14 ms。当反应温度从200℃增加到230℃时,掺杂量子点的发光强度增加并达到最大值;而继续升高温度至260℃时,发光强度迅速减弱。此外,测量了Mn掺杂Zn-In-S量子点的变温发光光谱。发现随着温度的升高,发光峰位发生蓝移,发光强度明显下降。分析认为,Mn掺杂Zn-In-S量子点的600 nm发光来自于Mn2+离子的4T1和6A1之间的辐射复合。展开更多
基金financially supported by the Natural Scientific Foundation of China (22109001, 22208335)Postdoctoral Fellowship Program of CPSF (GZB20230950)+1 种基金the Hefei National Laboratory for Physical Sciences at the Microscale (KF2020106)the support provided by the Collaborative Innovation Center of Suzhou Nano Science and Technology (NANO-CIC)。
文摘The incomplete sulfur reduction and high ZnS re-oxidation energy barrier along with severe side reactions during the battery cycling compromise the practical application of Zn–S electrochemistry. Herein, a bifunctional electrocatalytic sulfur matrix that simultaneously accelerates the sulfur reduction and ZnS oxidation is proposed to realize a highly-efficient Zn–S cell. It is revealed that the N-heteroatom hotspots are more favorable for facilitating the conversion of S to ZnS while the CoO nanocrystal substantially lowers the ZnS activation energy barrier thereby suppressing the formation of disproportionation species(e.g.,SO_(4)^(2-)) and accumulation of inactive ZnS. Accordingly, the Co O anchored on the N-doped carbon-supported sulfur cathode delivers a high Zn^(2+)storage capacity of 1,172 m Ahg^(-1)and outstanding cycling stability with a capacity retention of 71.6% after500 cycles with a high average Coulombic efficiency of 97.8%. Simultaneously, the stable cycling of solid-state Zn–S pouch cells with an energy density of 585 Whkg^(-1)sulfuris also demonstrated. Moreover, the postmortem analysis reveals that the degradation of Zn–S cells is mainly attributed to the limited reversibility of Zn anodes rather than the ZnS decomposition and/or accumulation. The approach to the bidirectional catalysis manipulated the sulfur redox provides a new perspective to realize the theoretical potentials of Zn–S cells.
文摘以ZnCl_(2)为硬模板和锌源,三聚氰胺和硫脲为氮源和硫源,废弃生物质橘子皮为碳源,通过高温烧结和后续蚀刻处理制备出硫化锌纳米点与三维N-S共掺杂炭纳米片的纳米复合材料(ZnS/NS-CN)。当应用于锂离子电池时,ZnS/NSCN表现出较高的可逆容量(0.1 A g^(−1)下,循环300次后容量仍有853.5 mAh g^(−1)),优异的长期循环稳定性(5 A g^(−1)下,循环1000次后,容量保持率为70.1%)和优异的倍率性能。此外,在0.5~4 V下组装和测试的ZnS/NS-CN//LiNiCoMnO2全电池表现出优异的电池性能(在0.2 C下循环150次后容量为140.4 mAh g^(−1),能量密度为132.4 Wh kg^(−1))。
