Noncovalent Immobilization of a Pyrene-Modified Cobalt Corrole on Carbon Supports for Enhanced Electrocatalytic Oxygen Reduction and Oxygen Evolution in Aqueous Solutions

Lei, Haitao; Liu, Chengyu; Wang, Zhaojun; Zhang, Zongyao; Zhang, Meining; Chang, Xingmao; Zhang, Wei; Cao, Rui

doi:10.1021/acscatal.6b01579

Cited by 175 publications

(150 citation statements)

References 87 publications

(129 reference statements)

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“…By comparison, it is obvious that the increase in the reduction current was because of the reduction of oxygen catalyzed by the Cu-SOCBP/C-modified electrode. Thus, it is preliminarily concluded that Cu-SOCBP/C has electrocatalytic activity for ORR, and this is consistent with the Cu-N x -enriched structure [17,21].…”

Section: Cyclic Voltammetry Of the Catalystsupporting

confidence: 63%

“…Figure 5a shows two CV curves of the Cu-SOCBP/C catalyst in a medium of 0.1 M PBS (pH = 7); one saturated with O 2 , and one saturated with N 2 . The CV curve recorded in the N 2 atmosphere shows a pair of irreversible redox peaks at 0.55 V/0.50 V, and these can be ascribed to the redox reaction process of Cu + /Cu 2+ ; this further confirmed the immobilization of copper ions within the catalyst [17,21]. In contrast, when N 2 was replaced by O 2 as the bubbling gas, it was observed that both the oxidation current and reduction current increased substantially.…”

Section: Cyclic Voltammetry Of the Catalystmentioning

confidence: 72%

“…Transition metal complexes generally have favorable catalytic activity for ORR, and the dispersion, deposition, or doping of these catalysts on carbon support materials substantially enhances ORR activity because of the performance improvements of many aspects of the catalysts. These aspects include high dispersion, conductivity, and an enhanced rate of mass transfer, such as charge transfer, oxygen uptake, and hydrogen uptake on the active site of the catalyst [21][22][23][24]. This type of modified catalyst is generally designated as Me-N x /C, where Me represents the complexed metal ions, N x refers to nitrogen atoms with complexing ability, and C refers to carbon materials as the supporters of the supramolecule complex.…”

Section: Introductionmentioning

confidence: 99%

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Carbon-Supported Copper-Based Nitrogen-Containing Supramolecule as an Efficient Oxygen Reduction Reaction Catalyst in Neutral Medium

Zhao

Chu

et al. 2018

Catalysts

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Abstract:In this work, a nitrogen-containing bidentate ligand named 5,5 -(9-octyl-9H-carbazole-2,7-diyl)bis(1,10-phenanthroline) (OCBP) was synthesized as a nitrogen precursor for making an oxygen reduction catalyst. The 1,10-phenanthroline unit provides a coordination site for copper ions, and the resulting Cu-N x unit may be responsible for the catalytic activities of the catalyst. Carbon black was selected as a support to improve the electroconductibility of the resulting catalyst. The metallo-supramolecule (Cu-SOCBP) was dispersed on the surface of Vulcan XC-72 carbon and was used as a catalyst (designated as Cu-SOCBP/C) for the oxygen reduction reaction (ORR). The microscope structure and surface components of the catalyst were acquired via scanning electron microscopy and X-ray photoelectron spectroscopy, as well as X-ray powder diffraction. The electrochemical property and ORR mechanism of Cu-SOCBP/C were analyzed using a variety of electroanalytical methods including cyclic voltammetry, electrochemical impedance spectroscopy, and linear sweep voltammetry. These results show that Cu-SOCBP/C was successfully synthesized and that ORR was achieved mainly via a four-electron transfer process to water. Thus, Cu-SOCBP/C was an effective catalyst and might have potential application as a cathodic catalyst in microbial fuel cells, which operate in an aqueous medium.

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Section: Cyclic Voltammetry Of the Catalystsupporting

confidence: 63%

Section: Cyclic Voltammetry Of the Catalystmentioning

confidence: 72%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Carbon-Supported Copper-Based Nitrogen-Containing Supramolecule as an Efficient Oxygen Reduction Reaction Catalyst in Neutral Medium

Zhao

Chu

et al. 2018

Catalysts

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“…[64][65][66][67] This is because existing cobalt molecular catalysts perform very well in organic solvents when reducing CO 2 ; however, in aqueous environments, cobalt selectively promotes proton reduction and generates HER. [71][72][73] These loading methods typically involve either physically Adv. [71][72][73] These loading methods typically involve either physically Adv.…”

Section: Cobalt-based Catalystsmentioning

confidence: 99%

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO₂ by Molecular Catalysts

Elouarzaki

Kannan

Jose

et al. 2019

Advanced Energy Materials

153

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provides a promising alternative to hydrocarbon sources for petrochemical feedstock. Thanks to the electrochemical nature of the CO 2 conversion to fuels and chemicals, the electrical energy invested to convert CO 2 in the form of a chemical fuel can be stored and redistributed using established supply chains for future use. Additionally, the integration of renewable energy systems (green electricity) into the grid can potentially create a carbon neutral energy cycle, and when driven by solar energy, offers a completely renewable energy cycle or negative carbon technology. Converting CO 2 electrochemically into compounds with high energy densities, such as alcohols (methanol, ethanol), formates, and CO, represents a form of energy storage and is also adaptable to demand response or energy arbitrage technologies. [3][4][5][6][7] The recoverable energy density of the chemicals that can be converted from CO 2 is substantially higher than most battery technologies.Given CO 2 electroreduction's immense economic and environmental potential, it has been the subject of much research activity over the past decades. [8][9][10][11] One of the greatest challenges of reducing CO 2 in an electrochemical cell is overcoming the immense energy barrier required to do so; the single electron reduction of CO 2 to CO 2 −˙, a common step in many CO 2 reduction mechanisms, requires an applied potential of −1.97 V measured versus standard hydrogen electrode (SHE). To alleviate this problem, many catalytic cathodes have been developed to avoid this intermediate and to reroute the reduction mechanism through alternate pathways requiring much lower applied potentials (a necessity if CO 2 electroreduction is to be implemented at industrial scale). [12][13][14] However, despite the low potentials offered by catalytic electrodes, the cost of electrodes is not always viable when upscaled to industrial levels. [15,16] Therefore, recent research trends in electrocatalytic reduction of CO 2 have been shifting toward the development of molecular catalysts that can exist as either solutes in electrolytes or can be surface-confined on electrodes. [13,16] The tunable nature and electronic characteristics of molecular catalysts give access to a large variety of catalysts with high activity, selectivity, and durability, as well as their ability to be integrated into sophisticated nanoassemblies. [17][18][19] Thanks to the aforementioned proprieties, performing CO 2 reduction using molecularly defined compounds offer several advantages compared to classical solid-state counterparts. Molecular catalysts usually exhibit well-defined homogeneous and/or CO 2 reduction using molecular catalysts is a key area of study for achieving electrical-to-chemical energy storage and feedstock chemical synthesis. Compared to classical metallic solid-state catalysts, these molecular catalysts often result in high performance and selectivity, even under unfavorable aqueous environments. This review considers the recent state-of-the-art molecular catalysts for CO 2 electro...

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“…

Twod ifferentm ethods were used to immobilize Co corroles on carbon nanotubes (CNTs) through covalent bonds. [34][35][36][37][38] Covalent immobilizationi su seful to improvec atalyst stabilitya nd performance and benefitst he recycling of electrocatalysts. For both HER andO ER in all solutions, the hybrids obtained by attaching Co corroles on CNTst hrough amidation coupling showedb etter performance.

…”

mentioning

confidence: 99%

Convenient Immobilization of Cobalt Corroles on Carbon Nanotubes through Covalent Bonds for Electrocatalytic Hydrogen and Oxygen Evolution Reactions

Lei

et al. 2019

ChemSusChem

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Twod ifferentm ethods were used to immobilize Co corroles on carbon nanotubes (CNTs) through covalent bonds. The resulting CNTse ngineered with Co corroles were used as electrocatalysts for the hydrogen evolutionr eaction (HER) and the oxygen evolution reaction (OER) in aqueous solutions of pH 0, 7, and 14. For both HER andO ER in all solutions, the hybrids obtained by attaching Co corroles on CNTst hrough amidation coupling showedb etter performance. This is likely because the large surface area and good electricalc onductivity of CNTsc an be well preserved during the amidationr eactionu nder mild conditions.The development of inexpensive, efficient, and robust electrocatalysts for the hydrogen evolutionr eaction (HER) and the oxygen evolution reaction( OER) has attracted increasing interest because of their appealing applicationsi nn ew energy technologies. [1][2][3] During the last decade,avariety of molecular complexes based on earth-abundant transition-metal elements including Mn, [4][5][6][7] Fe, [8][9][10][11][12][13][14] Co, [15][16][17][18][19][20][21] Ni, [22][23][24][25][26][27][28] and Cu [29][30][31][32][33] have been identified as catalystsf or these two reactions. To make these well-designed molecular catalysts useful in practice, they need to be immobilizedo ne lectrode materials. [34][35][36][37][38] Covalent immobilizationi su seful to improvec atalyst stabilitya nd performance and benefitst he recycling of electrocatalysts. [39][40][41][42][43] Despite these progresses,h owever, convenient methods for covalenti mmobilization under mild conditions are still needed.Carbon nanotubes (CNTs) are broadly used as supports for electrochemical applications because of their large surface areas and good electrical conductivities. [37,[44][45][46][47][48][49] Thep resence of abundant carboxyl groups on the surface of oxidized CNTsprovides ideal sites to attach catalystm olecules bearing amine groups through the amidation reaction. The resulting amide bonds tolerateb oth acidic and basic media and have sufficient stabilityu nder reductive and oxidative conditions. These features make CNTsp romising electrode materials for molecular engineering. However, the direct reaction of carboxyl and amine groupst of orm amide bonds is challenging. Therefore, carboxyl groups are usually converted to acyl chloride groups for subsequent amidation reaction.Herein, we report the convenient immobilization of Co corroles on CNTst hrough amidation coupling under mild conditions. Co corroles have been shown to be highly active and stable as catalysts for HERa nd OER under various conditions, [3,19] andt hust hey were chosen as model complexes in this work. The resulting hybrid can catalyze both HER and OER in aqueous solutionso fp H0,7 ,a nd 14. Compared with the traditional amidation by activating carboxyl groups with sulfinyl dichloride (SOCl 2 ), the directa midation coupling is simpler and more straightforward, and the resulting hybrid shows much better performance. This work is significant to showt he importance of the co...

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Noncovalent Immobilization of a Pyrene-Modified Cobalt Corrole on Carbon Supports for Enhanced Electrocatalytic Oxygen Reduction and Oxygen Evolution in Aqueous Solutions

Cited by 175 publications

References 87 publications

Carbon-Supported Copper-Based Nitrogen-Containing Supramolecule as an Efficient Oxygen Reduction Reaction Catalyst in Neutral Medium

Carbon-Supported Copper-Based Nitrogen-Containing Supramolecule as an Efficient Oxygen Reduction Reaction Catalyst in Neutral Medium

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO₂ by Molecular Catalysts

Convenient Immobilization of Cobalt Corroles on Carbon Nanotubes through Covalent Bonds for Electrocatalytic Hydrogen and Oxygen Evolution Reactions

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Noncovalent Immobilization of a Pyrene-Modified Cobalt Corrole on Carbon Supports for Enhanced Electrocatalytic Oxygen Reduction and Oxygen Evolution in Aqueous Solutions

Cited by 175 publications

References 87 publications

Carbon-Supported Copper-Based Nitrogen-Containing Supramolecule as an Efficient Oxygen Reduction Reaction Catalyst in Neutral Medium

Carbon-Supported Copper-Based Nitrogen-Containing Supramolecule as an Efficient Oxygen Reduction Reaction Catalyst in Neutral Medium

Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO2 by Molecular Catalysts

Convenient Immobilization of Cobalt Corroles on Carbon Nanotubes through Covalent Bonds for Electrocatalytic Hydrogen and Oxygen Evolution Reactions

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Recent Trends, Benchmarking, and Challenges of Electrochemical Reduction of CO₂ by Molecular Catalysts