eprintid: 10147056 rev_number: 6 eprint_status: archive userid: 699 dir: disk0/10/14/70/56 datestamp: 2022-04-21 08:57:02 lastmod: 2022-04-21 08:57:02 status_changed: 2022-04-21 08:57:02 type: article metadata_visibility: show sword_depositor: 699 creators_name: Huang, Chun creators_name: Wilson, Matthew D creators_name: Suzuki, Kosuke creators_name: Liotti, Enzo creators_name: Connolley, Thomas creators_name: Magdysyuk, Oxana V creators_name: Collins, Stephen creators_name: Van Assche, Frederic creators_name: Boone, Matthieu N creators_name: Veale, Matthew C creators_name: Lui, Andrew creators_name: Wheater, Rhian-Mair creators_name: Leung, Chu Lun Alex title: 3D Correlative Imaging of Lithium Ion Concentration in a Vertically Oriented Electrode Microstructure with a Density Gradient ispublished: inpress divisions: C05 divisions: F45 divisions: B04 divisions: UCL keywords: density gradient, ion concentration, vertically oriented structure note: © 2022 The Authors. Advanced Science published by Wiley-VCH GmbH This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited. abstract: The performance of Li+ ion batteries (LIBs) is hindered by steep Li+ ion concentration gradients in the electrodes. Although thick electrodes (≥300 µm) have the potential for reducing the proportion of inactive components inside LIBs and increasing battery energy density, the Li+ ion concentration gradient problem is exacerbated. Most understanding of Li+ ion diffusion in the electrodes is based on computational modeling because of the low atomic number (Z) of Li. There are few experimental methods to visualize Li+ ion concentration distribution of the electrode within a battery of typical configurations, for example, coin cells with stainless steel casing. Here, for the first time, an interrupted in situ correlative imaging technique is developed, combining novel, full-field X-ray Compton scattering imaging with X-ray computed tomography that allows 3D pixel-by-pixel mapping of both Li+ stoichiometry and electrode microstructure of a LiNi0.8 Mn0.1 Co0.1 O2 cathode to correlate the chemical and physical properties of the electrode inside a working coin cell battery. An electrode microstructure containing vertically oriented pore arrays and a density gradient is fabricated. It is shown how the designed electrode microstructure improves Li+ ion diffusivity, homogenizes Li+ ion concentration through the ultra-thick electrode (1 mm), and improves utilization of electrode active materials. date: 2022 date_type: published publisher: Wiley official_url: https://doi.org/10.1002/advs.202105723 oa_status: green full_text_type: pub language: eng primo: open primo_central: open_green verified: verified_manual elements_id: 1949773 doi: 10.1002/advs.202105723 medium: Print-Electronic lyricists_name: Leung, Chu Lun Alex lyricists_id: CLALE63 actors_name: Flynn, Bernadette actors_id: BFFLY94 actors_role: owner funding_acknowledgements: EP/S001239/1 [EPSRC]; EP/S001239/2 [EPSRC]; FITG034 [Faraday Institution]; EP/R511559/1 [EPSRC]; EP/R511638/1 [EPSRC]; 19K05519 [MEXT KAKENHI]; [Royal Society]; IEC∖R3∖193017 [Japan Society for the Promotion of Science]; 3G0A0417W [Ghent University Special Research Fund]; 01GC1517 [Ghent University Special Research Fund] full_text_status: public publication: Advanced Science event_location: Germany issn: 2198-3844 citation: Huang, Chun; Wilson, Matthew D; Suzuki, Kosuke; Liotti, Enzo; Connolley, Thomas; Magdysyuk, Oxana V; Collins, Stephen; ... Leung, Chu Lun Alex; + view all <#> Huang, Chun; Wilson, Matthew D; Suzuki, Kosuke; Liotti, Enzo; Connolley, Thomas; Magdysyuk, Oxana V; Collins, Stephen; Van Assche, Frederic; Boone, Matthieu N; Veale, Matthew C; Lui, Andrew; Wheater, Rhian-Mair; Leung, Chu Lun Alex; - view fewer <#> (2022) 3D Correlative Imaging of Lithium Ion Concentration in a Vertically Oriented Electrode Microstructure with a Density Gradient. Advanced Science 10.1002/advs.202105723 <https://doi.org/10.1002/advs.202105723>. (In press). Green open access document_url: https://discovery-pp.ucl.ac.uk/id/eprint/10147056/1/Advanced%20Science%20-%202022%20-%20Huang.pdf