Facile and accelerated production of RuO2 monolayers via a dual-step intercalation process

Se Yun Kim; Weon Ho Shin; Doh Won Jung; Dong-Su Ko; Jong Wook Roh; Sungwoo Hwang; Jongmin Lee; Kimoon Lee; Hee Jung Park; Chan Kwak; Sang-il Kim; Hyung Mo Jeong; Kyu Hyoung Lee; Hyun Sik Kim

doi:10.1039/C9QI01678C

Facile and accelerated production of RuO₂ monolayers via a dual-step intercalation process†

Se Yun Kim,

‡*^a Weon Ho Shin,

‡^b Doh Won Jung,^a Dong-Su Ko,^c Jong Wook Roh,^d Sungwoo Hwang,^a Jongmin Lee,^a Kimoon Lee,

^e Hee Jung Park,^f Chan Kwak,^a Sang-il Kim,

^g Hyung Mo Jeong,^h Kyu Hyoung Leeⁱ and Hyun Sik Kim*^j

Author affiliations

* Corresponding authors

^a Inorganic Material Lab, Samsung Advanced Institute of Technology, Suwon, Republic of Korea
E-mail: seyuni.kim@samsung.com

^b Department of Electronic Materials Engineering, Kwangwoon University, Seoul, Republic of Korea

^c Autonomous Material Development Lab, Samsung Advanced Institute of Technology, Suwon, Republic of Korea

^d School of Nano & Materials Science and Engineering, Kyungpook National University, Sangju, Republic of Korea

^e Department of Physics, Kunsan National University, Gunsan, Republic of Korea

^f Department of Materials Science and Engineering, Dankook University, Cheonan, Republic of Korea

^g Department of Materials Science and Engineering, University of Seoul, Seoul 02504, Republic of Korea

^h School of Mechanical Engineering, Sungkyunkwan University, Suwon 16419, Republic of Korea

ⁱ Department of Materials Science and Engineering, Yonsei University, Seoul, Republic of Korea

^j Department of Materials Science and Engineering, Hongik University, Seoul 04066, Republic of Korea
E-mail: hyunsik.kim@hongik.ac.kr

Abstract

Tetrabutylammonium ions (TBA⁺) have commonly been used to exfoliate RuO₂ into monolayers via ion exchange reactions. However, the low production yield of RuO₂ exfoliation, which originates from the large molecular size of TBA⁺, limits wider utilisation of RuO₂ monolayers in optoelectronic applications. We introduce a rapid and efficient dual-step exfoliation process beginning with intercalation of small organic molecules (tetramethylammonium ions) into RuO₂, which is followed by the addition of TBA⁺ as a second intercalant to realize RuO₂ monolayer production. Our dual-step intercalation process increases the RuO₂ monolayer exfoliation yield from 9.9% to 60% after 14 days. Density functional theory calculations reveal that the activation energy of dual-step intercalation is much lower than that of direct intercalation of TBA⁺ ions into the RuO₂ structure. The experimental and theoretical results of dual-step intercalation suggest that it is a facile and general approach for the production of metal oxide monolayers, and could widen the use of metal oxide monolayer nanosheets.

Inorganic Chemistry Frontiers

Facile and accelerated production of RuO₂ monolayers via a dual-step intercalation process†

Abstract

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Facile and accelerated production of RuO₂ monolayers via a dual-step intercalation process

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