Immobilization of an Amphiphilic Molecular Cobalt Catalyst on Carbon Black for Ligand-Assisted Water Oxidation

被引：18

作者：

Baydoun, Habib ^{[1
]}

Burdick, Jordyn ^{[1
]}

Thapa, Bishnu ^{[1
]}

Wickramasinghe, Lanka ^{[1
]}

Li, Da ^{[1
]}

Niklas, Jens ^{[2
]}

Poluektov, Oleg G. ^{[2
]}

Schlegel, H. Bernhard ^{[1
]}

Verani, Claudio N. ^{[1
]}

机构：

[1] Wayne State Univ, Dept Chem, 5101 Cass Ave, Detroit, MI 48202 USA

[2] ANL, Chem Sci & Engn Div, Lemont, IL 60439 USA

来源：

INORGANIC CHEMISTRY | 2018年 / 57卷 / 16期

基金：

美国国家科学基金会;

关键词：

OXYGEN EVOLUTION REACTION; DENSITY-FUNCTIONAL THEORY; MULTIPLE ACTIVE OXIDANTS; LANGMUIR-BLODGETT-FILMS; CONTINUUM SOLVATION; FREE-ENERGIES; IRON(III); COMPLEX; INTERMEDIATE; POTENTIALS;

D O I：

10.1021/acs.inorgchem.7b03252

中图分类号：

O61 [无机化学];

学科分类号：

070301 ; 081704 ;

摘要：

We have prepared the amphiphilic molecular catalyst [Co-III(L-OC18)(pyrr)(2)]ClO4 (1), where L-OC18 is the deprotonated form of N,N'-[4,5-bis(octadecyloxy)-1,2-phenylene]dipicolinamide. Species 1 can be anchored onto a carbon black support to yield the assembly 1@CB, which can catalyze water oxidation at an affordable onset overpotential of 0.32 V, with a current density of 10 mA/cm(2) at 0.37 V. Moreover, 1@CB displays TOF = 3850 h(-1). A mechanism is proposed based on the experimental and density-functional-theory-calculated data.

引用

页码：9748 / 9756

页数：9

共 60 条

[1] Synthesis and characterization of trans-[Co(III)(bpb)(amine)2]X (X = NCS, ClO4).: X-ray crystal structure of trans-[Co(III)(bpb)(pyrrolidine)2]NCS.0.5H2O containing intermolecular N-H•••O=C hydrogen-bonding [J].