journal article·2024-11-12

Selective Hydride Interstitials Induced in a High-Entropy Lanthanide Oxyhydride

Yuvraj Vaishnav, Rohit K. Rai, Walid Al Maksoud, Fumitaka Takeiri, Shusaku Hayama, Hiroshi Yaguchi, Samy Ould-Chikh, Marcell Toth, Raza Ullah Shah Bacha, Bambar Davaasuren, Maxim Avdeev, Genki Kobayashi, Yoji Kobayashi

Chemistry of Materials· Volume 36· Issue 21
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Abstract

High-entropy materials have gained significant interest in many applications, but structural investigations of the effect on anions in the crystal structure are still scarce. Here, we study the effect of multicomponent cation disorder in the case of mixed-anion compounds. The distribution of mixed anions among various coordination sites is important given their implications for properties such as ionic conductivity and bulk diffusion in catalysis. Structural analysis in the fluorite-type (La,Ce,Pr,Nd,Y)H 1.5 O 0.75 reveals that the disordered cationic effects create new interstitial sites, occupied selectively by hydride despite oxide and hydride disorder in other compositions and sites. In contrast, single-lanthanide oxyhydrides of analogous anion content, such as LaH 1.5 O 0.75, or SmH 2 O 0.5 lack the complex interstitial structure. Hydride ion conductivity measurements and bond valence sum energy maps show a considerably low activation energy of hydride migration due to the additional interstitial sites induced by high entropy. Such interstitials can be crucial in applications that involve hydride ion diffusion, such as ammonia synthesis catalysis and solid-state ionics, as further high-entropy compositions are explored.
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Research context

OpenAlex topics: Nuclear Materials and Properties · Hydrogen Storage and Materials · Catalysis and Oxidation Reactions

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Affiliations

KAUST Catalysis Center (KCC), Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal 23955-6900, Saudi Arabia

Chemistry Program, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal 23955-6900, Saudi Arabia

Center for Renewable Energy and Storage Technologies (CREST), Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology, Thuwal 23955-6900, Saudi Arabia

Solid State Chemistry Laboratory, Cluster for Pioneering Research (CPR), RIKEN, Wako 351-0198, Japan

Department of Chemistry, Kindai University, Osaka 577-8502, Japan

Diamond Light Source Ltd., Harwell Science and Innovation Campus, Didcot, Oxfordshire OX11 0DE, United Kingdom

Core Laboratories, King Abdullah University of Science and Technology, Thuwal 23955-6900, Saudi Arabia

Australian Nuclear Science and Technology Organisation, New Illawarra Rd, Lucas Heights, NSW 2234, Australia

School of Chemistry, The University of Sydney, Sydney 2006, Australia

Funding

King Abdullah University of Science and Technology

References (37)

Show source-provided references
1. 10.1103/PhysRevB.25.642510.1103/PhysRevB.25.6425 ↗
2. 10.1088/0022-3719/14/4/00810.1088/0022-3719/14/4/008 ↗
3. 10.1039/f2987830107310.1039/f29878301073 ↗
4. 10.1038/physci246044a010.1038/physci246044a0 ↗
5. 10.1088/0022-3719/17/22/01110.1088/0022-3719/17/22/011 ↗
6. 10.1098/rspa.1987.004510.1098/rspa.1987.0045 ↗
7. 10.1038/s41586-023-05815-010.1038/s41586-023-05815-0 ↗
8. 10.1021/acsaem.8b0007710.1021/acsaem.8b00077 ↗
9. 10.1038/ncomms191310.1038/ncomms1913 ↗
10. 10.1038/s41467-019-10492-710.1038/s41467-019-10492-7 ↗
11. 10.1021/acs.chemmater.9b0196810.1021/acs.chemmater.9b01968 ↗
12. 10.1002/aenm.20200372310.1002/aenm.202003723 ↗
13. 10.1021/jacs.8b0618710.1021/jacs.8b06187 ↗
14. 10.1080/21663831.2016.122043310.1080/21663831.2016.1220433 ↗
15. 10.1038/ncomms948510.1038/ncomms9485 ↗
16. 10.1002/adma.20180623610.1002/adma.201806236 ↗
17. 10.1016/0022-4596(84)90226-310.1016/0022-4596(84)90226-3 ↗
18. 10.1021/acs.chemmater.6b0521810.1021/acs.chemmater.6b05218 ↗
19. 10.1021/jacs.7b1036110.1021/jacs.7b10361 ↗
20. 10.1016/0167-2738(80)90034-X10.1016/0167-2738(80)90034-X ↗
21. 10.1016/0022-4596(83)90118-410.1016/0022-4596(83)90118-4 ↗
22. 10.1007/BF0061545910.1007/BF00615459 ↗
23. 10.1088/0022-3719/4/18/01610.1088/0022-3719/4/18/016 ↗
24. 10.1038/nmat330210.1038/nmat3302 ↗
25. 10.1021/acs.chemmater.7b0224010.1021/acs.chemmater.7b02240 ↗
26. 10.1002/adma.1990002030410.1002/adma.19900020304 ↗
27. 10.1021/jacs.1c1135310.1021/jacs.1c11353 ↗
28. 10.1039/b915141a10.1039/b915141a ↗
29. 10.1016/0167-2738(81)90110-710.1016/0167-2738(81)90110-7 ↗
30. 10.1006/jcat.1996.026810.1006/jcat.1996.0268 ↗
31. 10.1038/nchem.259510.1038/nchem.2595 ↗
32. 10.1002/aenm.20180177210.1002/aenm.201801772 ↗
33. 10.1021/jacs.9b1072610.1021/jacs.9b10726 ↗
34. 10.1111/jace.1668910.1111/jace.16689 ↗
35. 10.1107/S002188981300353110.1107/S0021889813003531 ↗
36. 10.1107/S160057751800897410.1107/S1600577518008974 ↗
37. 10.1107/S205252061801571810.1107/S2052520618015718 ↗