High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials

Lu, Zhiyi; Chen, Guangxu; Siahrostami, Samira; Chen, Zhihua; Li, Kai; Xie, Jin; Liao, Lei; Wu, Tong; Lin, Dingchang; Liu, Yayuan; Jaramillo, Thomas F.; Nørskov, Jens K.; Cui, Yi

doi:10.1038/s41929-017-0017-x

Cited by 1,180 publications

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“…[8] It is the doping-induced charge transfer from carbon atoms to their adjacent nitrogen atoms, changing the chemisorption mode of O 2 and weakening the OO bond for improving the ORR performance of VA-NCNT. [4,5,7] Since then, C-MFCs have been demonstrated to catalyze hydrogen evolution reaction (HER) for the production of clean fuel (H 2 ) from photo-/electrochemical water-splitting, ORR in fuel cells for energy generation/conversion, [10] and oxygen evolution reaction (OER) in metal-air batteries for energy storage, [7] two-electron transfer ORR to generate H 2 O 2 (an energy carrier and green oxidizer), [13] CO 2 reduction reaction (CO 2 RR) for the direct conversion of CO 2 into fuel, [14] N 2 reduction reaction (NRR) for synthesis of NH 3 under ambient environment, [15] and for the renewable energy generation/conversion from water driven by sunlight. [4,5,7] Since then, C-MFCs have been demonstrated to catalyze hydrogen evolution reaction (HER) for the production of clean fuel (H 2 ) from photo-/electrochemical water-splitting, ORR in fuel cells for energy generation/conversion, [10] and oxygen evolution reaction (OER) in metal-air batteries for energy storage, [7] two-electron transfer ORR to generate H 2 O 2 (an energy carrier and green oxidizer), [13] CO 2 reduction reaction (CO 2 RR) for the direct conversion of CO 2 into fuel, [14] N 2 reduction reaction (NRR) for synthesis of NH 3 under ambient environment, [15] and for the renewable energy generation/conversion from water driven by sunlight.…”

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Doping of Carbon Materials for Metal‐Free Electrocatalysis

2018

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Owning to the multiple advantages, including earth abundance, low-cost, high electronic conductivity, structure tenability at the molecular and morphological levels, and strong tolerance to acidic/alkaline media, [6] carbon nanomaterials have the great potential as metal alternatives for highly efficient metal-free catalysis. While metal alloys often suffer from segregation problems, heteroatom-doped carbonbased metal-free catalysts (C-MFCs) with covalent chemical bonds between the carbon and dopant atoms have no segregation issue, leading to a good operational stability. For metal catalysts, the catalytic activities strictly rely on metal element attributes. However, the catalytic active sites on C-MFCs can be modulated by introducing different dopants and structural defects, [8] providing powerful means for creating a large variety of highly efficient, multifunctional catalysts for various reactions. [5] Furthermore, 3D carbon architectures can be constructed from advanced nanocarbons, including carbon nanotubes (CNTs) and graphene sheets, [9,10] to further improve the performance of C-MFCs. Of particular interest, efficient 3D porous C-MFCs exhibit a large surface area with abundant available exposed active sites, excellent conductivity, high electrolyte diffusibility, and good mechanical property [11,12] -essentially impossible for metal catalysts.Great progress has been achieved since the first C-MFC with heteroatom-doping (i.e., vertically aligned N-doped CNT array, VA-NCNT) was developed as a metal-free catalyst for oxygen reduction reaction (ORR) by Dai and co-workers in 2009. [8] It is the doping-induced charge transfer from carbon atoms to their adjacent nitrogen atoms, changing the chemisorption mode of O 2 and weakening the OO bond for improving the ORR performance of VA-NCNT. [8] This groundbreaking work then launched a large number of research activities worldwide. [4,5,7] Since then, C-MFCs have been demonstrated to catalyze hydrogen evolution reaction (HER) for the production of clean fuel (H 2 ) from photo-/electrochemical water-splitting, ORR in fuel cells for energy generation/conversion, [10] and oxygen evolution reaction (OER) in metal-air batteries for energy storage, [7] two-electron transfer ORR to generate H 2 O 2 (an energy carrier and green oxidizer), [13] CO 2 reduction reaction (CO 2 RR) for the direct conversion of CO 2 into fuel, [14] N 2 reduction reaction (NRR) for synthesis of NH 3 under ambient environment, [15] and for the renewable energy generation/conversion from water driven by sunlight. [16] Carbon atoms in the graphitic carbon skeleton can be replaced by heteroatoms with different electronegative from that of the carbon atom (i.e., heteroatom doping) to modulate the charge distribution over the carbon network. The charge modulation can be achieved via direct charge transfer with an electron acceptor/donor (i.e., charge transfer doping) or through introduction of defects (i.e., defective doping). Various doping strategies, including heteroatom doping, charge-transfer dopi...

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confidence: 99%

Doping of Carbon Materials for Metal‐Free Electrocatalysis

2018

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“…However, their OER activity and stability under the OER conditions are not yet reported, which is essential for the bifunctional performance of the catalyst. On the other hand, oxygen‐doped carbon nanotubes are reported to be a highly selective catalyst for peroxide formation during the ORR in neutral media . To improve the ORR selectivity a further reduction of hydrogen peroxide can be ensured by engineering the loading, morphology, and composition of the catalyst …”

Section: Resultsmentioning

confidence: 99%

Designing Aqueous Organic Electrolytes for Zinc–Air Batteries: Method, Simulation, and Validation

Clark

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Iruin

et al. 2020

Advanced Energy Materials

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Aqueous zinc–air batteries (ZABs) are a low‐cost, safe, and sustainable technology for stationary energy storage. ZABs with pH‐buffered near‐neutral electrolytes have the potential for longer lifetime compared to traditional alkaline ZABs due to the slower absorption of carbonates at nonalkaline pH values. However, existing near‐neutral electrolytes often contain halide salts, which are corrosive and threaten the precipitation of ZnO as the dominant discharge product. This paper presents a method for designing halide‐free aqueous ZAB electrolytes using thermodynamic descriptors to computationally screen components. The dynamic performance of a ZAB with one possible halide‐free aqueous electrolyte based on organic salts is simulated using an advanced method of continuum modeling, and the results are validated by experiments. X‐ray diffraction, scanning electron microscopy, and energy dispersive X‐ray spectroscopy measurements of Zn electrodes show that ZnO is the dominant discharge product, and operando pH measurements confirm the stability of the electrolyte pH during cell cycling. Long‐term full cell cycling tests are performed, and rotating ring disk electrode measurements elucidate the mechanism of oxygen reduction reaction and oxygen evolution reaction. The analysis shows that aqueous electrolytes containing organic salts could be a promising field of research for zinc‐based batteries, due to their Zn2+ chelating and pH buffering properties. The remaining challenges including the electrochemical stability of the electrolyte components are discussed.

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“…They have undergone rapid development in recent decades and are replacing some traditional ceramic fabrication methods. [21] The oxidized carbon materials can be obtained by chemical oxidation, in which functional groups containing oxygen atoms are generated. The wet chemical methodc an be used to mix heteroatoms with 3D graphene gels having high surfacea rea and porous structure.…”

Section: Ball Millingmentioning

confidence: 99%

Progress in Nonmetal‐Doped Graphene Electrocatalysts for the Oxygen Reduction Reaction

et al. 2019

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Owing to energy shortages and environmental pollution, green energy sources such as polymer electrolyte fuel cells and metal–air batteries play a more and more important role, whereby the oxygen reduction reaction (ORR) is the rate‐determining step. Development of high‐efficiency and stable catalysts to facilitate the ORR is of importance. Graphene is a new type of material with two‐dimensional structure and high surface area, which has wide‐ranging applications in many fields. However, graphene with zero band gap shows low electrocatalytic activity toward the ORR. Introduction of nonmetal atoms can change the electronic arrangement, generate active sites, and further improve the catalytic activity of graphene. Some nonmetal‐doping strategies (e.g., N, S, and P doping) can promote ORR activity. Herein, the recent development of nonmetal‐doped graphene catalysts for ORR is reviewed. Some common synthetic methods for nonmetal‐doped graphene materials are summarized, and the active sites and possible reaction mechanisms for ORR on various nonmetal‐doped graphene catalysts are discussed.

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High-efficiency oxygen reduction to hydrogen peroxide catalysed by oxidized carbon materials

Cited by 1,180 publications

References 41 publications

Doping of Carbon Materials for Metal‐Free Electrocatalysis

Doping of Carbon Materials for Metal‐Free Electrocatalysis

Designing Aqueous Organic Electrolytes for Zinc–Air Batteries: Method, Simulation, and Validation

Progress in Nonmetal‐Doped Graphene Electrocatalysts for the Oxygen Reduction Reaction

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