Abstract: The electronic structures and redox behavours of the electron donor-acceptor compounds, cyanoethenyl aniline derivatives are investigated by MNDO method in this paper. The frontier orbitals of the compounds result from the interaction between the donor frontier orbital and that of the acceptor. The common oxidizing peaks of these compounds are due to the losing of an electron in N atom of the donor-amino, and the common reducing peaks are brought about by the obtaining of an electron at antibonding orbital of the acceptor-ethenyl. The space effect of the two CH_3 group makes DCEDMA forming a quasi-reversible single electron process. An intermediate stable tert-radical TCEA~(-·) may constitute its redox process.

Key words: MNDO, Donor-acceptor compound, Cyclic voltammogram, Cyanoethenyl aniline derivatives