TY - JOUR AU - Wang, Yonglin AU - Chen, Kai AU - Zhu, Yunhai AU - Wang, Jiazhi AU - Jiang, Nan AU - Yang, Yingkui PY - 2023 TI - Interwoven Poly(Anthraquinonyl Sulfide) Nanosheets-Decorated Carbon Nanotubes as Core–Sheath Heteroarchitectured Cathodes for Polymer-Based Asymmetrical Full Batteries JO - Energy & Environmental Materials SN - 2575-0348 VL - 6 IS - 5 AB - Organic redox-active polymers provide promising alternatives to metalcontaining inorganic compounds in Li-ion batteries (LIBs), whereas suffer from low actual capacities, poor rate/power capabilities, and inferior cycling stability. Herein, poly(anthraquinonyl sulfide)-coated carbon nanotubes (CNT@PAQS) are readily performed by in situ polymerization to form core–sheath nanostructures. Remarkably, flower-like PAQS nanosheets are interwoven around CNTs to synergistically create robust 3D hierarchical networks with abundant cavities, internal channels, and sufficiently-exposed surfaces/edges, thereby promoting electron transport and making more active sites accessible for electrolytes and guest ions. Apparently, the asfabricated CNT@PAQS cathode delivers the large reversible capacity (200.5 mAh g−1 at 0.05 A g−1), high-rate capability (161.5 mAh g−1 at 5.0 A g−1), and impressive cycling stability (retaining 88.0% over 1000 cycles). In addition, an asymmetric full-battery using CNT@PAQS as a cathode and cyclized polyacrylonitrile-encapsulated CNTs as an anode is assembled that delivers a high energy density of 86.3 Wh kg−1, and retains 81.3% of initial capacity after 1000 cycles. This work opens up an efficient strategy to combine highly conductive and redox-active phases into core–sheath heterostructures to unlock the barrier of high-rate charge storage. The further integration of two polymer-based electrodes into asymmetric full cells would also consolidate the development of low-cost, sustainable, and powerful batteries. UR - https://doi.org/10.1002/eem2.12564 DO - 10.1002/eem2.12564