eprintid: 10194590
rev_number: 8
eprint_status: archive
userid: 699
dir: disk0/10/19/45/90
datestamp: 2024-07-16 13:38:27
lastmod: 2024-07-16 13:38:27
status_changed: 2024-07-16 13:38:27
type: article
metadata_visibility: show
sword_depositor: 699
creators_name: Büchner, Carina
creators_name: Kubitza, Niels
creators_name: Malik, Ali M
creators_name: Jamboretz, John
creators_name: Riaz, Aysha A
creators_name: Zhu, Yujiang
creators_name: Schlueter, Christoph
creators_name: McCartney, Martha R
creators_name: Smith, David J
creators_name: Regoutz, Anna
creators_name: Rohrer, Jochen
creators_name: Birkel, Christina S
title: Chemical Conversions within the Mo–Ga–C System: Layered Solids with Variable Ga Content
ispublished: pub
divisions: UCL
divisions: B04
divisions: C06
divisions: F56
note: This version is the author-accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
abstract: Layered carbides are fascinating compounds due to their enormous structural and chemical diversity, as well as their potential to possess useful and tunable functional properties. Their preparation, however, is challenging and forces synthesis scientists to develop creative and innovative strategies to access high-quality materials. One unique compound among carbides is Mo₂Ga₂C. Its structure is related to the large and steadily growing family of 211 MAX phases that crystallize in a hexagonal structure (space group P6₃/mmc) with alternating layers of edge-sharing M₆X octahedra and layers of the A-element. Mo₂Ga₂C also crystallizes in the same space group, with the difference that the A-element layer is occupied by two A-elements, here Ga, that sit right on top of each other (hence named “221” compound). Here, we propose that the Ga content in this compound is variable between 2:2, 2:1, and 2: ≤1 (and 2:0) Mo/Ga ratios. We demonstrate that one Ga layer can be selectively removed from Mo₂Ga₂C without jeopardizing the hexagonal P6₃/mmc structure. This is realized by chemical treatment of the 221 phase Mo₂Ga₂C with a Lewis acid, leading to the “conventional” 211 MAX phase Mo₂GaC. Upon further reaction with CuCl₂, more Ga is removed and replaced with Cu (instead of fully exfoliating into the Ga-free Mo₂CTx MXene), leading to Mo₂Ga₁₋ₓCuₓC still crystallizing with space group P6₃/mmc, however, with a significantly larger c-lattice parameter. Furthermore, 211 Mo₂GaC can be reacted with Ga to recover the initial 221 Mo₂Ga₂C. All three reaction pathways have not been reported previously and are supported by powder X-ray diffraction (PXRD), electron microscopy, X-ray spectroscopy, and density functional theory (DFT) calculations.
date: 2024-04-29
date_type: published
publisher: RSC
official_url: https://doi.org/10.1021/acs.inorgchem.4c00107
full_text_type: other
language: eng
verified: verified_manual
elements_id: 2269871
doi: 10.1021/acs.inorgchem.4c00107
medium: Print-Electronic
lyricists_name: Regoutz, Anna
lyricists_id: AREGO48
actors_name: Regoutz, Anna
actors_id: AREGO48
actors_role: owner
funding_acknowledgements: NNCI-ECCS-1542160 [University College London]; I-20221270 [University College London]; NHR4CES [University College London]; [Federal Ministry of Education and Research]
full_text_status: restricted
publication: Inorganic Chemistry
volume: 63
number: 17
pagerange: 7725-7734
pages: 10
event_location: United States
issn: 2052-1553
citation:        Büchner, Carina;    Kubitza, Niels;    Malik, Ali M;    Jamboretz, John;    Riaz, Aysha A;    Zhu, Yujiang;    Schlueter, Christoph;                     ... Birkel, Christina S; + view all <#>        Büchner, Carina;  Kubitza, Niels;  Malik, Ali M;  Jamboretz, John;  Riaz, Aysha A;  Zhu, Yujiang;  Schlueter, Christoph;  McCartney, Martha R;  Smith, David J;  Regoutz, Anna;  Rohrer, Jochen;  Birkel, Christina S;   - view fewer <#>    (2024)    Chemical Conversions within the Mo–Ga–C System: Layered Solids with Variable Ga Content.                   Inorganic Chemistry , 63  (17)   pp. 7725-7734.    10.1021/acs.inorgchem.4c00107 <https://doi.org/10.1021/acs.inorgchem.4c00107>.      
 
document_url: https://discovery.ucl.ac.uk/id/eprint/10194590/1/Mo2Ga2C_Birkel_rev.pdf