Robust Interfacial Effect in Multi-interface Environment through Hybrid Reconstruction Chemistry for Enhanced Energy Storage
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- Northwestern Polytechnical University, Xi'an, Shaanxi (China)
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Nanjing University of Science and Technology, Nanjing (China)
Electrochemical-oxidation-driven reconstruction has emerged as an efficient approach for developing advanced materials, but the reconstructed microstructure still faces challenges including inferior conductivity, unsatisfying intrinsic activity, and active-species dissolution. In this report we present hybrid reconstruction chemistry that synergistically couples electrochemical oxidation with electrochemical polymerization (EOEP) to overcome these constraints. During the EOEP process, the metal hydroxides undergo rapid reconstruction and dynamically couple with polypyrrole (PPy), resulting in an interface-enriched microenvironment. We observe that the interaction between PPy and the reconstructed metal center (i.e., Mn > Ni, Co) is strongly correlated. Theoretical calculation results demonstrate that the strong interaction between Mn sites and PPy breaks the intrinsic limitation of MnO2, rendering MnO2 with a metallic property for fast charge transfer and enhancing the ion-adsorption dynamics. Operando Raman measurement confirms the promise of EOEP-treated Mn(OH)2 (E-MO/PPy) to stably work under a 1.2 V potential window. The tailored E-MO/PPy exhibits a high capacitance of 296 F g–1 at a large current density of 100 A g–1. Here our strategy presents breakthroughs in upgrading the electrochemical reconstruction technique, which enables both activity and kinetics engineering of electrode materials for better performance in energy-related fields.
- Research Organization:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Organization:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC); National Key Research and Development Program of China; Central Universities; Natural Science Basic Research Plan in Shaanxi Province of China; China Postdoctoral Science Foundation; Young Talent Fund of Association for Science and Technology in Shaanxi, China; Northwestern Polytechnical University; Nanjing University of Science and Technology; Natural Science Foundation of Jiangsu Province
- Grant/Contract Number:
- AC02-05CH11231; 52202301; 22375161; 22275148; 2018YFB1900201; D5000210607; 2022JQ-143; 2022M722587, 2022TQ0256; 20230620; 2023T014; TSXK2022D002; BK20220929
- OSTI ID:
- 2279007
- Journal Information:
- ACS Nano, Vol. 17, Issue 24; ISSN 1936-0851
- Publisher:
- American Chemical Society (ACS)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
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