Lead oxides (PbO, 1 ≤ ≤ 2) are promising high-capacity and low-cost anodes for lithium ion batteries (LIBs). However, the huge lithiation-induced volume expansion of conventional large-sized PbO particles leads to severe electrode pulverization with poor cycling stability. Herein, a rare mixed-valence PbO with a unique hierarchical architecture of nanoparticle-assembled interconnected hollow spheres (denoted PbO NAHSs) is crafted by introducing polyvinylpyrrolidone (PVP) into the solution of generating β-PbO microspheres (MSs), which is exploited for the first time as a potential advanced anode material for LIBs. Notably, an intriguing PVP-driven dissolution-recrystallization transformation process converting β-PbO MSs into PbO NAHSs is revealed by PVP-concentration and reaction-time control experiments, demonstrating the dual function of PVP as a mild reducing agent combined with it being a morphology regulator for the construction of PbO NAHSs. Furthermore, a self-sacrificial templating mechanism is demonstrated for yielding the interconnected hollow structure of PbO NAHSs. Remarkably, PbO NAHSs deliver stable capacities of 561 and 453 mA h g after 100 and 200 cycles at 50 and 500 mA g, respectively, in sharp contrast to the performance of β-PbO MSs (52 and 43 mA h g). Structural and electrochemical measurements of the cycled electrodes indicate that the hollow and nanoarchitectural structure of PbO NAHSs enables their superior cycling and rate capabilities, benefiting from the effectively buffered volume expansion and shortened lithium storage distance, respectively. As such, this work highlights a robust PVP-assisted strategy to fabricate rare mixed-valence PbO NAHSs with outstanding electrochemical reactivity and mechanical robustness for lithium storage and various potential applications.
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http://dx.doi.org/10.1039/d4nr04763j | DOI Listing |
Nanoscale
December 2024
Key Laboratory of Advanced Energy Storage and Conversion of Wenzhou, Key Laboratory of Carbon Materials of Zhejiang Province, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou 325035, P. R. China.
Lead oxides (PbO, 1 ≤ ≤ 2) are promising high-capacity and low-cost anodes for lithium ion batteries (LIBs). However, the huge lithiation-induced volume expansion of conventional large-sized PbO particles leads to severe electrode pulverization with poor cycling stability. Herein, a rare mixed-valence PbO with a unique hierarchical architecture of nanoparticle-assembled interconnected hollow spheres (denoted PbO NAHSs) is crafted by introducing polyvinylpyrrolidone (PVP) into the solution of generating β-PbO microspheres (MSs), which is exploited for the first time as a potential advanced anode material for LIBs.
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