Heterometallic Benzenehexathiolato Coordination Nanosheets: Periodic Structure Improves Crystallinity and Electrical Conductivity

Ryojun Toyoda, Naoya Fukui, Dionisius H.L. Tjhe, Ekaterina Selezneva, Hiroaki Maeda, Cédric Bourgès, Choon Meng Tan, Kenji Takada, Yuanhui Sun, Ian Jacobs, Kazuhide Kamiya, Hiroyasu Masunaga, Takao Mori, Sono Sasaki, Henning Sirringhaus, Hiroshi Nishihara

Research output: Contribution to journalArticlepeer-review

6 Citations (Scopus)

Abstract

Coordination nanosheets are an emerging class of 2D, bottom-up materials having fully π-conjugated, planar, graphite-like structures with high electrical conductivities. Since their discovery, great effort has been devoted to expand the variety of coordination nanosheets; however, in most cases, their low crystallinity in thick films hampers practical device applications. In this study, mixtures of nickel and copper ions are employed to fabricate benzenehexathiolato (BHT)-based coordination nanosheet films, and serendipitously, it is found that this heterometallicity preferentially forms a structural phase with improved film crystallinity. Spectroscopic and scattering measurements provide evidence for a bilayer structure with in-plane periodic arrangement of copper and nickel ions with the NiCu2BHT formula. Compared with homometallic films, heterometallic films exhibit more crystalline microstructures with larger and more oriented grains, achieving higher electrical conductivities reaching metallic behaviors. Low dependency of Seebeck coefficient on the mixing ratio of nickel and copper ions supports that the large variation in the conductivity data is not caused by change in the intrinsic properties of the films. The findings open new pathways to improve crystallinity and to tune functional properties of 2D coordination nanosheets.

Original languageEnglish
Article number2106204
JournalAdvanced Materials
Volume34
Issue number13
DOIs
Publication statusPublished - 1 Apr 2022

Keywords

  • 2D polymers
  • benzenehexathiolato metal complexes
  • coordination nanosheets
  • electrical conductivities
  • heterometallicity

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