Two cerium complexes with and without manganese ion, [MnCe4(dipic)6(H2O)20][Ce(dipic)3]2·7H2O (dipic = dipicolinate) (1) and [Ce2(H2O)4(O2CMe)6][Ce(H2O)4(NO3)2(O2CMe)]2·2H2O·2MeOH
(2), have been prepared, and their electrocatalytic reactivity for water oxidation has been investigated. Compound 1 is a heterometallic 3d-4f compound which possesses four Ce(IV) ions, two Ce(III) ions, and one Mn(II). Compound 2 is composed of three neutral parts, one
of which is a dinuclear cerium molecule lying on an inversion center, and the other two are symmetric monomer units; the four cerium ions in 2 are all Ce(III). Electrochemical studies of 1 and 2 show that 1 can catalyze water oxidation at the potential ~1.5 V
with an overpotential of ca. 900 mV versus NHE. Control potential electrolysis (CPE) experiments at 1.50 V of 1 displayed a stable current density of 2.5 mA/cm2, and the calculated Faradaic efficiency is 60%. However, no electrocatalytic reactivity
was observed for 2. By comparison experiments, it was found that the electrocatalysis of 1 may result from the cooperative catalytic effect of the 4f cerium ion and 3d transition metal manganese ion.
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Heterometallic 3d-4f compound;
Document Type: Research Article
Key Laboratory of Marine Chemistry Theory and Technology, Ministry of Education, College of Chemistry and Chemical Engineering, Ocean University of China, Qingdao, PR China
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, The Chinese Academy of Sciences, Fuzhou, China
School of Chemistry and Environmental Engineering, Key Laboratory for Green Chemical Process of Ministry of Education, Wuhan Institute of Technology, Wuhan, PR China
May 3, 2018