Order-to-disorder transition due to entropy in layered and 2D carbides
In compositionally complex materials, there is controversy on the effect of enthalpy versus entropy on the structure and short-range ordering in so-called high-entropy materials. To help address this controversy, we synthesized and probed 40 M<sub>4</sub>AlC<sub>3</sub> layered carbide phases containing two to nine metals and found that short-range ordering from enthalpy was present until the entropy increased enough to achieve complete disordering of the transition metals in their atomic planes. We transformed all of these layered carbide phases into two-dimensional (2D) sheets and showed the effects of the order versus disorder on their surface properties and electronic behavior. This study suggests the key effect that the competition between enthalpy and entropy has on short-range order in multicompositional materials.
Authors
- Brian C. Wyatt (ORCID: https://orcid.org/0000-0002-0425-4791)
- Yinan Yang (ORCID: https://orcid.org/0000-0003-3505-2858)
- Anupma Thakur (ORCID: https://orcid.org/0000-0001-7897-9229)
- Neil Ghosh (ORCID: https://orcid.org/0000-0002-0527-011X)
- Aleksandra Vojvodić (ORCID: https://orcid.org/0000-0002-5584-6711)
- Xianfan Xu (ORCID: https://orcid.org/0000-0003-0580-4625)
- Manushree Tanwar (ORCID: https://orcid.org/0000-0002-7589-0496)
- Annabelle Bedford (ORCID: https://orcid.org/0000-0002-7543-4976)
- Hui Fang (ORCID: https://orcid.org/0000-0002-4024-1234)
- De‐en Jiang (ORCID: https://orcid.org/0000-0001-5167-0731)
- Babak Anasori (ORCID: https://orcid.org/0000-0002-1955-253X)
- Yury G. Gogotsi (ORCID: https://orcid.org/0000-0001-9423-4032)
- Zachary D. Hood (ORCID: https://orcid.org/0000-0002-5720-4392)
- Sixbert P. Muhoza (ORCID: https://orcid.org/0000-0002-9986-4241)
- Srinivasa Kartik Nemani (ORCID: https://orcid.org/0000-0001-5731-8552)
- Sanguk Han
- Francesca Urban (ORCID: https://orcid.org/0000-0003-2109-1370)
- Paweł Piotr Michałowski (ORCID: https://orcid.org/0000-0002-3299-4092)
- Zahra Fakhraai (ORCID: https://orcid.org/0000-0002-0597-9882)
- Tetiana Parker (ORCID: https://orcid.org/0000-0001-5998-2617)
- Bethany G. Wright
- Jin Woo Jang
- Kalpana R. Kamath
- Rebecca Disko
- Yamilée Morency
- Givi Kadagishvili (ORCID: https://orcid.org/0009-0000-1610-8524)
Institutions
- Argonne National Laboratory (US)
- Vanderbilt University (US)
- Purdue University West Lafayette (US)
- Łukasiewicz Research Network (PL)
- Drexel University (US)
- University of Pennsylvania (US)
Publication Details
- Journal
- Science
- Published
- 2025-09-04
- DOI
- https://doi.org/10.1126/science.adv4415
- Citations
- 17
- Primary Topic
- MXene and MAX Phase Materials
- Type
- article
- Field-Weighted Citation Impact
- 8.80