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Anchored Mediator Enabling Shuttle‐Free Redox Mediation in Lithium‐Oxygen Batteries
Author(s) -
Ko Youngmin,
Park Hyunji,
Lee Kyunam,
Kim Sung Joo,
Park Hyeokjun,
Bae Youngjoon,
Kim Jihyeon,
Park Soo Young,
Kwon Ji Eon,
Kang Kisuk
Publication year - 2020
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201916682
Subject(s) - redox , anode , oxygen , lithium (medication) , polymer , materials science , chemistry , methacrylate , chemical engineering , inorganic chemistry , polymerization , electrode , organic chemistry , medicine , engineering , endocrinology
Abstract Redox mediators (RMs) are considered an effective countermeasure to reduce the large polarization in lithium‐oxygen batteries. Nevertheless, achieving sufficient enhancement of the cyclability is limited by the trade‐offs of freely mobile RMs, which are beneficial for charge transport but also trigger the shuttling phenomenon. Here, we successfully decoupled the charge‐carrying redox property of RMs and shuttling phenomenon by anchoring the RMs in polymer form, where physical RM migration was replaced by charge transfer along polymer chains. Using PTMA (poly(2,2,6,6‐tetramethyl‐1‐piperidinyloxy‐4‐yl methacrylate)) as a polymer model system based on the well‐known RM tetramethylpiperidinyloxyl (TEMPO), it is demonstrated that PTMA can function as stationary RM, preserving the redox activity of TEMPO. The efficiency of RM‐mediated Li 2 O 2 decomposition remains remarkably stable without the consumption of oxidized RMs or degradation of the lithium anode, resulting in an improved performance of the lithium‐oxygen cell.