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Tailoring the electrochemical activity of magnesium chromium oxide towards Mg batteries through control of size and crystal structure

Hu, L; Johnson, ID; Kim, S; Nolis, GM; Freeland, JW; Yoo, HD; Fister, TT; ... Cabana, J; + view all (2019) Tailoring the electrochemical activity of magnesium chromium oxide towards Mg batteries through control of size and crystal structure. Nanoscale , 11 (2) pp. 639-646. 10.1039/c8nr08347a. Green open access

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Abstract

Chromium oxides with the spinel structure have been predicted to be promising high voltage cathode materials in magnesium batteries. Perennial challenges involving the mobility of Mg2+ and reaction kinetics can be circumvented by nano-sizing the materials in order to reduce diffusion distances, and by using elevated temperatures to overcome activation energy barriers. Herein, ordered 7 nm crystals of spinel-type MgCr2O4 were synthesized by a conventional batch hydrothermal method. In comparison, the relatively underexplored Continuous Hydrothermal Flow Synthesis (CHFS) method was used to make highly defective sub-5 nm MgCr2O4 crystals. When these materials were made into electrodes, they were shown to possess markedly different electrochemical behavior in a Mg2+ ionic liquid electrolyte, at moderate temperature (110 °C). The anodic activity of the ordered nanocrystals was attributed to surface reactions, most likely involving the electrolyte. In contrast, evidence was gathered regarding the reversible bulk deintercalation of Mg2+ from the nanocrystals made by CHFS. This work highlights the impact on electrochemical behavior of a precise control of size and crystal structure of MgCr2O4. It advances the understanding and design of new cathode materials for Mg-based batteries.

Type: Article
Title: Tailoring the electrochemical activity of magnesium chromium oxide towards Mg batteries through control of size and crystal structure
Location: England
Open access status: An open access version is available from UCL Discovery
DOI: 10.1039/c8nr08347a
Publisher version: https://doi.org/10.1039/c8nr08347a
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10064870
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