Regulating the Spin State of FeIII by Atomically Anchoring on Ultrathin Titanium Dioxide for Efficient Oxygen Evolution Electrocatalysis.
Guoqiang ShenRongrong ZhangLun PanFang HouYingjie ZhaoZeyu ShenWenbo MiChengxiang ShiQingfa WangXiangwen ZhangJi-Jun ZouPublished in: Angewandte Chemie (International ed. in English) (2019)
Ferric oxides and (oxy)hydroxides, although plentiful and low-cost, are rarely considered for oxygen evolution reaction (OER) owing to the too high spin state (eg filling ca. 2.0) suppressing the bonding strength with reaction intermediates. Now, a facile adsorption-oxidation strategy is used to anchor FeIII atomically on an ultrathin TiO2 nanobelt to synergistically lower the spin state (eg filling ca. 1.08) to enhance the adsorption with oxygen-containing intermediates and improve the electro-conductibility for lower ohmic loss. The electronic structure of the catalyst is predicted by DFT calculation and perfectly confirmed by experimental results. The catalyst exhibits superior performance for OER with overpotential 270 mV @10 mA cm-2 and 376 mV @100 mA cm-2 in alkaline solution, which is much better than IrO2 /C and RuO2 /C and is the best iron-based OER catalyst free of active metals such as Ni, Co, or precious metals.
Keyphrases
- room temperature
- metal organic framework
- visible light
- low cost
- density functional theory
- reduced graphene oxide
- ionic liquid
- highly efficient
- transition metal
- single molecule
- human health
- health risk
- carbon dioxide
- aqueous solution
- quantum dots
- health risk assessment
- signaling pathway
- risk assessment
- protein kinase
- molecular dynamics
- gold nanoparticles
- mass spectrometry
- iron deficiency
- electron transfer
- high resolution
- high speed