Malonodinitrile, benzoylacetonitrile, and ethyl benzoylacetate were deprotonated in situ by (BuLi)-Bu-n to give the reactive carbanions (RRHC(-))-R-2-H-3 (R-2/R-3 = CN/CN, CN/COPh, CO2Et/COPh), which nucleophilically attack the C=N bond of the nitrilium clusters (Ph4P)[B10H9NCR1] (R-1 = Me, Et). This reaction results in generation of push-pull alkenes bearing closo-decaborate clusters, [B10H9NHC(R-1)=(CRR3)-R-2](2) (6 examples; up to 97% isolated yields). These species were isolated as the bis-tetraphenylposhphonium salts and were characterized by H-1 and B-11 NMR, HR ESI+/- -MS, and also by single-crystal X-ray diffraction. (C) 2017 Elsevier B.V. All rights reserved.