The new mono-and dicopper (II) complexes [Cu (H3L1)(NCS)](1) and [Cu2 (μ-HL2) 2 (NCS) 2](2) were easily self-assembled from Cu (CH3COO) 2· H2O, NaNCS, NaOH and N, N, N′, N′-tetrakis (2-hydroxyethyl) ethylenediamine (H4L1) or N-ethyldiethanolamine (H2L2), respectively. They were fully characterized by IR spectroscopy, ESI-MS (±), elemental and single-crystal X-ray diffraction analyses, and applied as homogeneous catalysts for (i) the ...