Non‐3d Metal Modulation of a Cobalt Imidazolate Framework for Excellent Electrocatalytic Oxygen Evolution in Neutral Media

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 [Co4(MO4...

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Published in	Angewandte Chemie International Edition Vol. 58; no. 1; pp. 139 - 143
Main Authors	Xu, Yan‐Tong, Ye, Zi‐Ming, Ye, Jia‐Wen, Cao, Li‐Ming, Huang, Rui‐Kang, Wu, Jun‐Xi, Zhou, Dong‐Dong, Zhang, Xue‐Feng, He, Chun‐Ting, Zhang, Jie‐Peng, Chen, Xiao‐Ming
Format	Journal Article
Language	English
Published	Germany Wiley Subscription Services, Inc 02.01.2019
Edition	International ed. in English
Subjects	Buffer solutions Carbon dioxide Catalysts Coated electrodes Cobalt Computer applications Computer simulation electrocatalysis Electrocatalysts Electronic structure Glassy carbon Heavy metals imidazolate frameworks Metals metal–organic frameworks Modulation Oxygen oxygen evolution reaction Oxygen evolution reactions imidazolate frameworks oxygen evolution reaction cobalt electrocatalysis metal-organic frameworks
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Abstract	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 [Co4(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. Non‐3D for 3D: Introducing non‐3d metal oxide units into a cobalt imidazolate framework results in the drastic enhancement of electrocatalytic performance of the oxygen evolution reaction in neutral media.
AbstractList	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 (MO 4 )(eim) 6 ] (M=Mo or W, Heim=2‐ethylimidazole) having Co(eim) 3 (MO 4 ) 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 CO 2 ‐saturated 0.5 m KHCO 3 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 RuO 2 . 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. 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 [Co4(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. Non‐3D for 3D: Introducing non‐3d metal oxide units into a cobalt imidazolate framework results in the drastic enhancement of electrocatalytic performance of the oxygen evolution reaction in neutral media. 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 [Co4 (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.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 [Co4 (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. 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 [Co4(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. 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 (MO )(eim) ] (M=Mo or W, Heim=2-ethylimidazole) having Co(eim) (MO ) 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 at an overpotential of 210 mV in CO -saturated 0.5 m KHCO electrolyte and 2/10/22 mA cm at overpotential of 388/490/570 mV in phosphate buffer solution) among non-precious metal catalysts and even outperforms RuO . 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.
Author	Cao, Li‐Ming Huang, Rui‐Kang Zhou, Dong‐Dong Zhang, Xue‐Feng Zhang, Jie‐Peng Xu, Yan‐Tong He, Chun‐Ting Wu, Jun‐Xi Ye, Jia‐Wen Chen, Xiao‐Ming Ye, Zi‐Ming
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BackLink	https://www.ncbi.nlm.nih.gov/pubmed/30320948$$D View this record in MEDLINE/PubMed
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Keywords	imidazolate frameworks oxygen evolution reaction cobalt electrocatalysis metal-organic frameworks
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Snippet	Cobalt imidazolate frameworks are classical electrocatalysts for the oxygen evolution reaction (OER) but suffer from the relatively low activity. Here, a...
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SubjectTerms	Buffer solutions Carbon dioxide Catalysts Coated electrodes Cobalt Computer applications Computer simulation electrocatalysis Electrocatalysts Electronic structure Glassy carbon Heavy metals imidazolate frameworks Metals metal–organic frameworks Modulation Oxygen oxygen evolution reaction Oxygen evolution reactions
Title	Non‐3d Metal Modulation of a Cobalt Imidazolate Framework for Excellent Electrocatalytic Oxygen Evolution in Neutral Media
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