Nickel(ii) complexes based on dithiolate–polyamine binary ligand systems: crystal structures, hirshfeld surface analysis, theoretical study, and catalytic activity study on photocatalytic hydrogen generation

Adhikari, Suman; Bhattacharjee, Tirtha; Bhattacharjee, Sharmila; Daniliuc, Constantin Gabriel; Frontera, Antonio; Lopato, Eric M.; Bernhard, Stefan

doi:10.1039/d1dt00352f

Title: Nickel(ii) complexes based on dithiolate–polyamine binary ligand systems: crystal structures, hirshfeld surface analysis, theoretical study, and catalytic activity study on photocatalytic hydrogen generation

Journal Article · Tue Mar 16 00:00:00 EDT 2021 · Dalton Transactions

DOI:https://doi.org/10.1039/d1dt00352f· OSTI ID:1853622

^[1]; Bhattacharjee, Tirtha ^[2];

^[1];

^[3];

^[4]; Lopato, Eric M. ^[5];

^[5]

Govt. Degree College, Dharmanagar (India)
Bineswar Brahma Engineering College, Kokrajhar (India)
Westfälische Wilhelms-Univ. Münster (Germany)
Univ. de les Illes Balears, Palma de Mallorca (Spain)
Carnegie Mellon Univ., Pittsburgh, PA (United States)

To ascertain the influence of binary ligand systems [1,1-dicyanoethylene-2,2-dithiolate (i-mnt^-2) and polyamine {tetraen = tris(2-aminoethyl)amine, tren = diethylene triamine and opda = o-phenylenediamine}] on the coordination modes of the Ni(II) metal center and resulting supramolecular architectures, a series of nickel(II) thiolate complexes [Ni(tetraen)(i-mnt)](DMSO) (1), [Ni₂(tren)₂(i-mnt)₂] (2), and [Ni₂(i-mnt)₂(opda)₂]_n (3) have been synthesized in high yield in one step in water and structurally characterized by single crystal X-ray crystallography and spectroscopic techniques. X-ray diffraction studies disclose the diverse i-mnt^-2 coordination to the Ni⁺² center in the presence of active polyamine ligands, forming a slightly distorted octahedral geometry (NiN₄S₂) in 1, square planar (NiS₄) and distorted octahedral geometries (NiN₆) in the bimetallic co-crystallized aggregate of cationic [Ni(tren)₂]⁺² and anionic [Ni(i-mnt)₂]^-2 in 2, and a one dimensional (1D) polymeric chain along the [100] axis in 3, having consecutive square planar (NiS₄) and octahedral (NiN₆) coordination kernels. The N–H···O, N–H···S, N–H···N, N–H···S, N–H···N, and N–H···O type hydrogen bonds stabilize the supramolecular assemblies in 1, 2, and 3 respectively imparting interesting graph-set-motifs. The molecular Hirshfeld surface analyses (HS) and 2D fingerprint plots were utilized for decoding all types of non-covalent contacts in the crystal networks. Atomic HS analysis of the Ni⁺² centers reveals significant Ni–N metal–ligand interactions compared to Ni–S interactions. We have also studied the unorthodox interactions observed in the solid state structures of 1–3 by QTAIM and NBO analyses. Moreover, all the complexes proved to be highly active water reduction co-catalysts (WRC) in a photo-catalytic hydrogen evolution process involving iridium photosensitizers, wherein 2 and 3 having a square planar arrangement around the nickel center(s) – were found to be the most active ones, achieving 1000 and 1119 turnover numbers (TON), respectively.

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Research Organization:: Carnegie Mellon Univ., Pittsburgh, PA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0020392

OSTI ID:: 1853622

Alternate ID(s):: OSTI ID: 1776377

Journal Information:: Dalton Transactions, Vol. 50, Issue 16; ISSN 1477-9226

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

CCDC 2054291: Experimental Crystal Structure Determination Suman, Adhikari,; Tirtha, Bhattacharjee,; Sharmila, Bhattacharjee, https://doi.org/10.5517/ccdc.csd.cc26yng9 The current record is supplemented by this dataset	dataset	January 2021
CCDC 2054290: Experimental Crystal Structure Determination Suman, Adhikari,; Tirtha, Bhattacharjee,; Sharmila, Bhattacharjee, https://doi.org/10.5517/ccdc.csd.cc26ynf8 The current record is supplemented by this dataset	dataset	January 2021
CCDC 2054292: Experimental Crystal Structure Determination Suman, Adhikari,; Tirtha, Bhattacharjee,; Sharmila, Bhattacharjee, https://doi.org/10.5517/ccdc.csd.cc26ynhb The current record is supplemented by this dataset	dataset	January 2021

Title: Nickel(ii) complexes based on dithiolate–polyamine binary ligand systems: crystal structures, hirshfeld surface analysis, theoretical study, and catalytic activity study on photocatalytic hydrogen generation

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