Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 1, Pages 139-143Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201809144
Keywords
cobalt; electrocatalysis; imidazolate frameworks; metal-organic frameworks; oxygen evolution reaction
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Funding
- NSFC [21731007, 21821003, 21890380, 21473260, 91622109]
- Guangdong Pearl River Talents Program [2017BT01C161]
- National Postdoctoral Program for Innovative Talents [BX201600195]
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Cobalt imidazolate frameworks are classical electrocatalysts for the oxygen evolution reaction (OER) but suffer from the relatively low activity. Here, a non-3d metal modulation strategy is presented for enhancing the OER activity of cobalt imidazolate frameworks. Two isomorphous frameworks [Co-4(MO4)(eim)(6)] (M=Mo or W, Heim=2-ethylimidazole) having Co(eim)(3)(MO4) units and high water stabilities were designed and synthesized. In different neutral media, the Mo-modulated framework coated on a glassy carbon electrode shows the best OER performances (1 mA cm(-2) at an overpotential of 210 mV in CO2-saturated 0.5 m KHCO3 electrolyte and 2/10/22 mA cm(-2) at overpotential of 388/490/570 mV in phosphate buffer solution) among non-precious metal catalysts and even outperforms RuO2. Spectroscopic measurements and computational simulations revealed that the non-3d metals modulate the electronic structure of Co for optimum reactant/product adsorption and tailor the energy of rate-determining step to a more moderate value.
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