Metastable hexagonal close-packed palladium hydride in liquid cell TEM

Jaeyoung Hong, Jee-Hwan Bae, Hyesung Jo, Hee-Young Park, Sehyun Lee, Sung Jun Hong, Hoje Chun, Min Kyung Cho, Juyoung Kim, Joodeok Kim, Yongju Son, Haneul Jin, Jin-Yoo Suh, Sung-Chul Kim, Ha-Kyung Roh, Kyu Hyoung Lee, Hyung-Seok Kim, Kyung Yoon Chung, Chang Won Yoon, Kiryeong Lee, Seo Hee Kim, Jae-Pyoung Ahn, Hionsuck Baik, Gyeung Ho Kim, Byungchan Han, Sungho Jin, Taeghwan Hyeon, Jungwon Park, Chang Yun Son (), Yongsoo Yang (), Young-Su Lee (), Sung Jong Yoo () and Dong Won Chun ()
Additional contact information
Jaeyoung Hong: Korea Institute of Science and Technology
Jee-Hwan Bae: Korea Institute of Science and Technology
Hyesung Jo: Korea Advanced Institute of Science and Technology
Hee-Young Park: Korea Institute of Science and Technology
Sehyun Lee: Korea Institute of Science and Technology
Sung Jun Hong: Yonsei University
Hoje Chun: Yonsei University
Min Kyung Cho: Korea Institute of Science and Technology
Juyoung Kim: Korea Institute of Science and Technology
Joodeok Kim: Institute for Basic Science (IBS)
Yongju Son: Institute for Basic Science (IBS)
Haneul Jin: Korea Institute of Science and Technology
Jin-Yoo Suh: Korea Institute of Science and Technology
Sung-Chul Kim: Korea Institute of Science and Technology
Ha-Kyung Roh: Korea Institute of Science and Technology
Kyu Hyoung Lee: Yonsei University
Hyung-Seok Kim: Korea Institute of Science and Technology
Kyung Yoon Chung: Korea Institute of Science and Technology
Chang Won Yoon: Korea Institute of Science and Technology
Kiryeong Lee: Korea Institute of Science and Technology
Seo Hee Kim: Korea Institute of Science and Technology
Jae-Pyoung Ahn: Korea Institute of Science and Technology
Hionsuck Baik: Korea Basic Science Institute
Gyeung Ho Kim: Korea Institute of Science and Technology
Byungchan Han: Yonsei University
Sungho Jin: University of California San Diego
Taeghwan Hyeon: Institute for Basic Science (IBS)
Jungwon Park: Institute for Basic Science (IBS)
Chang Yun Son: Pohang University of Science and Technology
Yongsoo Yang: Korea Advanced Institute of Science and Technology
Young-Su Lee: Korea Institute of Science and Technology
Sung Jong Yoo: Korea Institute of Science and Technology
Dong Won Chun: Korea Institute of Science and Technology

Nature, 2022, vol. 603, issue 7902, 631-636

Abstract: Abstract Metastable phases—kinetically favoured structures—are ubiquitous in nature1,2. Rather than forming thermodynamically stable ground-state structures, crystals grown from high-energy precursors often initially adopt metastable structures depending on the initial conditions, such as temperature, pressure or crystal size1,3,4. As the crystals grow further, they typically undergo a series of transformations from metastable phases to lower-energy and ultimately energetically stable phases1,3,4. Metastable phases sometimes exhibit superior physicochemical properties and, hence, the discovery and synthesis of new metastable phases are promising avenues for innovations in materials science1,5. However, the search for metastable materials has mainly been heuristic, performed on the basis of experiences, intuition or even speculative predictions, namely ‘rules of thumb’. This limitation necessitates the advent of a new paradigm to discover new metastable phases based on rational design. Such a design rule is embodied in the discovery of a metastable hexagonal close-packed (hcp) palladium hydride (PdHx) synthesized in a liquid cell transmission electron microscope. The metastable hcp structure is stabilized through a unique interplay between the precursor concentrations in the solution: a sufficient supply of hydrogen (H) favours the hcp structure on the subnanometre scale, and an insufficient supply of Pd inhibits further growth and subsequent transition towards the thermodynamically stable face-centred cubic structure. These findings provide thermodynamic insights into metastability engineering strategies that can be deployed to discover new metastable phases.

Date: 2022
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DOI: 10.1038/s41586-021-04391-5

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