Copper-coordinated cellulose ion conductors for solid-state batteries

Chunpeng Yang, Qisheng Wu, Weiqi Xie, Xin Zhang, Alexandra Brozena, Jin Zheng, Mounesha N. Garaga, Byung Hee Ko, Yimin Mao, Shuaiming He, Yue Gao, Pengbo Wang, Madhusudan Tyagi, Feng Jiao, Robert Briber, Paul Albertus, Chunsheng Wang, Steven Greenbaum, Yan-Yan Hu, Akira Isogai, Martin Winter, Kang Xu, Yue Qi () and Liangbing Hu ()
Additional contact information
Chunpeng Yang: University of Maryland
Qisheng Wu: Brown University
Weiqi Xie: University of Maryland
Xin Zhang: University of Maryland
Alexandra Brozena: University of Maryland
Jin Zheng: Florida State University
Mounesha N. Garaga: City University of New York
Byung Hee Ko: University of Delaware
Yimin Mao: University of Maryland
Shuaiming He: University of Maryland
Yue Gao: University of Maryland
Pengbo Wang: Florida State University
Madhusudan Tyagi: University of Maryland
Feng Jiao: University of Delaware
Robert Briber: University of Maryland
Paul Albertus: University of Maryland
Chunsheng Wang: University of Maryland
Steven Greenbaum: City University of New York
Yan-Yan Hu: Florida State University
Akira Isogai: The University of Tokyo
Martin Winter: Institute of Physical Chemistry, University of Münster
Kang Xu: Army Research Laboratory
Yue Qi: Brown University
Liangbing Hu: University of Maryland

Nature, 2021, vol. 598, issue 7882, 590-596

Abstract: Abstract Although solid-state lithium (Li)-metal batteries promise both high energy density and safety, existing solid ion conductors fail to satisfy the rigorous requirements of battery operations. Inorganic ion conductors allow fast ion transport, but their rigid and brittle nature prevents good interfacial contact with electrodes. Conversely, polymer ion conductors that are Li-metal-stable usually provide better interfacial compatibility and mechanical tolerance, but typically suffer from inferior ionic conductivity owing to the coupling of the ion transport with the motion of the polymer chains1–3. Here we report a general strategy for achieving high-performance solid polymer ion conductors by engineering of molecular channels. Through the coordination of copper ions (Cu2+) with one-dimensional cellulose nanofibrils, we show that the opening of molecular channels within the normally ion-insulating cellulose enables rapid transport of Li+ ions along the polymer chains. In addition to high Li+ conductivity (1.5 × 10−3 siemens per centimetre at room temperature along the molecular chain direction), the Cu2+-coordinated cellulose ion conductor also exhibits a high transference number (0.78, compared with 0.2–0.5 in other polymers2) and a wide window of electrochemical stability (0–4.5 volts) that can accommodate both the Li-metal anode and high-voltage cathodes. This one-dimensional ion conductor also allows ion percolation in thick LiFePO4 solid-state cathodes for application in batteries with a high energy density. Furthermore, we have verified the universality of this molecular-channel engineering approach with other polymers and cations, achieving similarly high conductivities, with implications that could go beyond safe, high-performance solid-state batteries.

Date: 2021
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DOI: 10.1038/s41586-021-03885-6

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