Journal
CHEMICAL SCIENCE
Volume 8, Issue 12, Pages 8078-8085Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c7sc02688a
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Funding
- JST-CREST Development of Atomic or Molecular Two-Dimensional Functional Films and Creation of Fundamental Technologies for Their Applications [JPMJCR15F2]
- JSPS KAKENHI [JP15H00862, JP15J06673, JP15K13654, JP16H00900, JP16H00957, JP26220801, JP26708005, JP17H05354, JP17H03028]
- US Department of Energy [DE FG02-04ER46148]
- Nanotechnology Platform of the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan
- U.S. Department of Energy (DOE) [DE-FG02-04ER46148] Funding Source: U.S. Department of Energy (DOE)
- Grants-in-Aid for Scientific Research [26708005, 15K13654, 16H00957] Funding Source: KAKEN
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A pi-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 x 10 (6) to 1 x 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.
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