Bis(aminothiolato)nickel nanosheet as a redox switch for conductivity and an electrocatalyst for the hydrogen evolution reaction

Xinsen Sun, Kuo Hui Wu, Ryota Sakamoto, Tetsuro Kusamoto, Hiroaki Maeda, Xiaojuan Ni, Wei Jiang, Feng Liu, Sono Sasaki, Hiroyasu Masunaga, Hiroshi Nishihara

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95 Scopus citations

Abstract

A π-conjugated coordination nanosheet comprising bis(aminothiolato)nickel (NiAT) moieties was synthesized by the reaction of Ni(acac)2 with 1,3,5-triaminobenzene-2,4,6-trithiol at liquid-liquid and gas-liquid interfaces. The sheet thickness could be controlled down to a single layer (0.6 nm). Selected area electron diffraction and grazing incidence X-ray diffraction analyses indicated the formation of a flat crystalline sheet with a kagome lattice stacked in a staggered alignment. NiAT was reversibly interconverted to a bis(iminothiolato)nickel (NiIT) nanosheet by the chemical 2H+-2e- reaction, which was accompanied by a drastic change in electrical conductivity from 3 × 10-6 to 1 × 10-1 S cm-1. This change in conductivity was explained by the difference in band structures between NiAT and NiIT. NiAT acted as an efficient electrocatalyst for the hydrogen evolution reaction, showing strong acid durability and an onset overpotential of -0.15 V.

Original languageEnglish (US)
Pages (from-to)8078-8085
Number of pages8
JournalChemical Science
Volume8
Issue number12
DOIs
StatePublished - 2017
Externally publishedYes

Bibliographical note

Funding Information:
This work is supported by JST-CREST “Development of Atomic or Molecular Two-Dimensional Functional Films and Creation of Fundamental Technologies for Their Applications” (JPMJCR15F2) and JSPS KAKENHI Grant Numbers JP15H00862, JP15J06673, JP15K13654, JP16H00900, JP16H00957, JP26220801, JP26708005, JP17H05354, JP17H03028. Work at Utah is supported by US Department of Energy (Grant No. DE FG02-04ER46148). The synchrotron radiation experiments were performed at BL45XU in SPring-8 with the approval of RIKEN (Proposal No. 20160041). XPS measurements were conducted at Advanced Characterization Nanotechnology Platform of the University of Tokyo, supported by “Nanotechnology Platform” of the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan. We acknowledge NERSC and CHPC at the University of Utah for providing the computing resources.

Publisher Copyright:
© 2017 The Royal Society of Chemistry.

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