Superstructured mesocrystals through multiple inherent molecular interactions for highly reversible sodium ion batteries

Xiaoling Qiu; Xiaoling Wang; Yunxiang He; Jieying Liang; Kang Liang; Blaise L Tardy; Joseph J Richardson; Ming Hu; Hao Wu; Yun Zhang; Orlando J Rojas; Ian Manners; Junling Guo

doi:10.1126/sciadv.abh3482

Superstructured mesocrystals through multiple inherent molecular interactions for highly reversible sodium ion batteries

Sci Adv. 2021 Sep 10;7(37):eabh3482. doi: 10.1126/sciadv.abh3482. Epub 2021 Sep 8.

Authors

Xiaoling Qiu¹, Xiaoling Wang^{1

2}, Yunxiang He¹, Jieying Liang³, Kang Liang³, Blaise L Tardy⁴, Joseph J Richardson⁵, Ming Hu⁶, Hao Wu¹, Yun Zhang¹, Orlando J Rojas⁷, Ian Manners⁸, Junling Guo^{1

2

9}

Affiliations

¹ BMI Center for Biomass Materials and Nanointerfaces, College of Biomass Science and Engineering, College of Materials Science and Engineering, Sichuan University, Chengdu Sichuan 610065, China.
² Harvard John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA.
³ School of Chemical Engineering, University of New South Wales, Sydney, New South Wales 2052, Australia.
⁴ Department of Bioproducts and Biosystems, School of Chemical Engineering, Aalto University, 02150 Espoo, Finland.
⁵ Department of Materials Engineering, School of Engineering, The University of Tokyo, Tokyo 113-8656, Japan.
⁶ School of Physics and Materials Science, East China Normal University, Shanghai 200241, China.
⁷ Bioproducts Institute, Departments of Chemical and Biological Engineering, Chemistry, and Wood Science, The University of British Columbia, Vancouver, BC, Canada.
⁸ Department of Chemistry, University of Victoria, Victoria, BC V8W 3V6, Canada.
⁹ State Key Laboratory of Polymer Materials Engineering, Sichuan University, Chengdu, Sichuan 610065, China.

Abstract

Soft structures in nature, such as supercoiled DNA and proteins, can organize into complex hierarchical architectures through multiple noncovalent molecular interactions. Identifying new classes of natural building blocks capable of facilitating long-range hierarchical structuring has remained an elusive goal. We report the bottom-up synthesis of a hierarchical metal-phenolic mesocrystal where self-assembly proceeds on different length scales in a spatiotemporally controlled manner. Phenolic-based coordination complexes organize into supramolecular threads that assemble into tertiary nanoscale filaments, lastly packing into quaternary mesocrystals. The hierarchically ordered structures are preserved after thermal conversion into a metal-carbon hybrid framework and can impart outstanding performance to sodium ion batteries, which affords a capability of 72.5 milliampere hours per gram at an ultrahigh rate of 200 amperes per gram and a 90% capacity retention over 15,000 cycles at a current density of 5.0 amperes per gram. This hierarchical structuring of natural polyphenols is expected to find widespread applications.