Flexible and robust bimetallic covalent organic frameworks for the reversible switching of electrocatalytic oxygen evolution activity

Gao, Zhengming; Yu, Zhengkun; Huang, Yuxing; He, Xiangqing; Su, Xuemin; Xiao, Longhui; Yu, Yixin; Huang, Xinhui; Luo, Feng

doi:10.1039/c9ta14023a

Cited by 55 publications

(33 citation statements)

References 53 publications

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“…The electrocatalytic performance of Co‐TpBpy was also moderate; the overpotential reached 400 mV at only 1 mA cm −2 [17b] . Co 0.5 V 0.5 @COF‐SO 3 ( η = 318 mV for 10 mA cm −2 ) [7b] was excellent an electrocatalyst in COFs. Although the overpotential of Co@COF‐Pyr was higher than Co 0.5 V 0.5 @COF‐SO 3 , its TOF value (0.1 s −1 ) was slightly better than Co 0.5 V 0.5 @COF‐SO 3 (0.098 s −1 ).…”

Section: Resultsmentioning

confidence: 95%

Pyrimidine‐Functionalized Covalent Organic Framework and its Cobalt Complex as an Efficient Electrocatalyst for Oxygen Evolution Reaction

et al. 2021

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A pyrimidine‐modified covalent organic framework (COF‐Pyr) was designed to be synthesized via the Povarov reaction. The nitrogen atom on the pyrimidine showed excellent coordination ability to metal ions. Their stable metal composite material (Co@COF‐Pyr) exhibited remarkable performance for electrocatalytic oxygen evolution reaction (OER) in 1.0 m KOH aqueous solution. The overpotential was 450 mV at 10 mA cm−2. The Co@COF‐Pyr with large specific surface area (392 m2 g−1) and regular crystal structure provided free passage for H2O to move and make them fully contact with the uniformly dispersed cobalt ions on the surface. Thus, the turnover frequency of Co@COF‐Pyr was 0.1 s−1 at the overpotential of 370 mV, which was higher than most reported OER catalysts. This work provided a new way to design and prepare nitrogen‐containing heterocyclic functionalized COFs. They can be combined with metal ions to expand the application of COFs in the field of electrocatalysis.

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Section: Resultsmentioning

confidence: 95%

Pyrimidine‐Functionalized Covalent Organic Framework and its Cobalt Complex as an Efficient Electrocatalyst for Oxygen Evolution Reaction

et al. 2021

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“…The electrocatalytic properties of Ni‐HXR, Fe‐HXR, NiFe‐HXR, NiFeO x and commercial IrO 2 benchmark toward OER were examined in 1.0 M KOH electrolyte using a typical three‐electrode setup [19] . As well known, the overpotential at the current density of 10 mA cm −2 is a crucial parameter to evaluate the OER activity of electrocatalysts.…”

Section: Methodsmentioning

confidence: 99%

Enhancing One‐Dimensional Charge Transport in Metal‐organic Framework Hexagonal Nanorods for Electrocatalytic Oxygen Evolution

et al. 2021

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Metal‐organic frameworks (MOFs) have exhibited huge potential in electrocatalytic fields. However, the intrinsic low conductivity and the blockage of metal active sites by organic linkers still seriously hinder their large‐scale application. In this study, as a proof of principle, constructing cofacial π–π stacking in the terminal ligand (4,4′‐bipyridine) of a Ni/Fe‐chain‐based MOF to fabricate strong π–π interaction, in combination with unique hexagonal nanorod (HXR) structure, is found to be an effective strategy to enhance one‐dimensional charge carrier efficiency and thus achieve excellent activity in the oxygen evolution reaction (OER). The approach yields a high turnover frequency (4.54 s−1) in well‐designed bimetallic chain‐based MOFs (NiFe‐HXR) at an overpotential of 350 mV, which is about 8.7 and 34.9 times higher than those in Ni‐HXR (0.52 s−1) and IrO2 (0.13 s−1), respectively. This work effectively combines “through‐bond” channel in chain‐based structure of NiFe‐HXR and “through‐space” transport between face‐to‐face terminal ligands, thus resulting in outstanding OER activity. This strategy of modulating the structure chemistry and morphology of MOFs to promote the OER may open a new perspective to synthesize MOFs for energy‐relevant electrochemical reactions.

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“…Starting with a great contribution from Luo and coworkers, flexible and robust Co/V‐incorporated bimetallic COFs (defined as Co x V 1− x @COF‐SO 3 ) were synthesized and used as efficient OER electrocatalysts via a convenient and efficient cation‐exchange strategy ( Figure a). [ 81 ] The obtained Co 0.5 V 0.5 @COF‐SO 3 catalyst showed a morphology of the uniform nanofiber (Figure 12b). As a result, the optimized bimetallic Co 0.5 V 0.5 @COF‐SO 3 exhibited the lowest Tafel slope of 62 mV dec −1 and a high TOF value (0.098 s −1 ) at the overpotential of 300 mV, all of which are superior to those of monometallic COFs (Figure 12c–e).…”

Section: Cof‐based Electrocatalysts For Efficient Oermentioning

confidence: 99%

Section: Cof‐based Electrocatalysts For Efficient Oermentioning

confidence: 99%

Covalent Organic Frameworks for Efficient Energy Electrocatalysis: Rational Design and Progress

Zhang

Zhu

Schmidt

et al. 2021

Adv Energy and Sustain Res

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An efficient catalyst with a precisely designed and predictable structure is highly desired to optimize its performance and understand the mechanism beyond the catalytic activity. Covalent organic frameworks (COFs), as an emerging class of framework materials linked by strong covalent bonds, simultaneously allow precise structure design with predictable synthesis and show advantages of large surface areas, tunable pore sizes, and unique molecular architectures. Although the research on COF‐based electrocatalysts is at an early age, significant progress has been made. Herein, the recent significant progress in the design and synthesis of COFs as highly efficient electrocatalysts for the oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER) is summarized. Design principles for COFs as efficient electrocatalysts are discussed by considering essential factors for catalyzing the OER, ORR, and HER processes at the molecular level. Herein, a summary on the in‐depth understanding of the catalytic mechanism and kinetics limitations of COFs provides a general instruction for further exploring their vast potential for designing highly efficient electrocatalysts.

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Flexible and robust bimetallic covalent organic frameworks for the reversible switching of electrocatalytic oxygen evolution activity

Abstract: Reversible switching of OER performance is designed for the first time in COF materials through convenient phase transformation via ion exchange. This also facilitates to enhance atom utilization efficiency.

Cited by 55 publications

References 53 publications

Pyrimidine‐Functionalized Covalent Organic Framework and its Cobalt Complex as an Efficient Electrocatalyst for Oxygen Evolution Reaction

Pyrimidine‐Functionalized Covalent Organic Framework and its Cobalt Complex as an Efficient Electrocatalyst for Oxygen Evolution Reaction

Enhancing One‐Dimensional Charge Transport in Metal‐organic Framework Hexagonal Nanorods for Electrocatalytic Oxygen Evolution

Covalent Organic Frameworks for Efficient Energy Electrocatalysis: Rational Design and Progress

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