Theoretical insights on the reaction pathways for oxygen reduction reaction on phosphorus doped graphene

Bai, Xiaowan; Zhao, Erjun; Li, Kai; Wang, Ying; Jiao, Menggai; He, Feng; Sun, Xiaoxu; Sun, He; Wu, Zhijian

doi:10.1016/j.carbon.2016.04.033

Cited by 64 publications

(39 citation statements)

References 57 publications

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“…The most favorable pathway is a 2 !b 4 !e 1 !f 1 .T he a 2 !b 3 !d 2 !e 2 !f 1 pathway is also energetically competitive. In this work, the rate-determining step in these two competitive pathways is the last step, that is, OH hydrogenation into the second H 2 Ow ith an energy barrier of 0.91 eV.T his value is slightly highert han the calculated energy barrier of 0.80 eV for Pt (111), [39] 0.85 eV for single P-doped divacancy graphene, [40] and 0.88 eV forsingle P-doped monovacancy graphene. [33] Effect of electrodepotentials on the ORR All the above energy barriers and reaction energies are calculated under zero electrode potential, buti nr eality the cathode electrocatalyst for the ORR works under ap ositive electrode potential, therefore, the influence of the externalp otential (U) on the activity and mechanism of the ORR is investigated by employing the methodo fN ørskov et al [41] The free energy diagrams for them ost favorable pathways, that is, OOH hydrogenation into O+ +H 2 O( a 2 !b 4 !e 1 !f 1 )a nd OH+ +OH (a 2 !…”

Section: Hydrogenation Of Oohmentioning

confidence: 69%

“…In this work, the rate‐determining step in these two competitive pathways is the last step, that is, OH hydrogenation into the second H 2 O with an energy barrier of 0.91 eV. This value is slightly higher than the calculated energy barrier of 0.80 eV for Pt (1 1 1), 0.85 eV for single P‐doped divacancy graphene, and 0.88 eV for single P‐doped monovacancy graphene …”

Section: Resultsmentioning

confidence: 99%

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Theoretical Investigation on the Reaction Pathways of the Oxygen Reduction Reaction on Graphene Codoped with Manganese and Phosphorus as a Potential Nonprecious Metal Catalyst

Bai

Zhao

et al. 2016

ChemCatChem

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Nonprecious‐metal‐doped graphene catalysts have been proposed recently as promising candidates to substitute Pt catalysts for the oxygen reduction reaction (ORR) in fuel cells. We codoped Mn and P in divacancy graphene (MnPx, x=1–4) and we studied the stability and the catalytic activity for the ORR. The calculated formation energy indicates that MnP2‐doped divacancy graphene is energetically the most stable. The MnP2 moiety and its adjacent six C atoms are catalytically active sites for the ORR. The kinetically most favorable pathway is the hydrogenation of OOH to form O+H2O, which is a four‐electron process. The rate‐determining step is the second H2O formation, which has an energy barrier of 0.91 eV. The free energy diagrams show that for OOH hydrogenation into O+H2O all of the elementary steps are downhill at potentials of 0.0–0.67 V except for the second H2O formation.

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Section: Hydrogenation Of Oohmentioning

confidence: 69%

Section: Resultsmentioning

confidence: 99%

Theoretical Investigation on the Reaction Pathways of the Oxygen Reduction Reaction on Graphene Codoped with Manganese and Phosphorus as a Potential Nonprecious Metal Catalyst

Bai

Zhao

et al. 2016

ChemCatChem

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“…Green electrochemical devices such as fuel cells and metal–air batteries, operating under acidic or alkaline media, play a crucial role in energy conversion and storage systems, and their output energy capacity is predominantly determined by the cathodic oxygen reduction reaction (ORR) owing to its sluggish kinetics . Although precious Pt‐based catalysts have shown to be high ORR activity, its high cost, scarcity as well as susceptibility to time‐dependent drift, crossover effect, and CO poisoning are prohibitive to large‐scale commercialization . Hence, there is a need to develop either less expensive alternatives or catalysts with higher activity.…”

Section: Introductionmentioning

confidence: 99%

Sustainable and Atomically Dispersed Iron Electrocatalysts Derived from Nitrogen‐ and Phosphorus‐Modified Woody Biomass for Efficient Oxygen Reduction

Liu

Gan

et al. 2018

Adv Materials Inter

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Development of low‐cost, efficient, and robust electrocatalysts to replace precious platinum catalysts for oxygen reduction reaction (ORR) is urgent to boost the applications of green energy devices such as fuel cells and metal–air batteries. Herein, a low‐cost, simple, and easy‐to‐scale method to develop sustainable and cost‐effective ORR carbocatalysts via impregnation followed by pyrolysis of different renewable woody biomass is reported. Aberration‐corrected high‐angle annular dark field scanning transmission electron microscopy, X‐ray photoelectron spectroscopy, and X‐ray absorption near edge structure measurements show that the nitrogen‐ and phosphorus‐promoted atomically dispersed iron is mainly responsible for the high ORR activity. Moreover, by a mimic of the natural pine materials derived Fe‐based electrocatalyst, introducing external Fe precursor into the biomass can generate targeted well dispersed Fe complex catalysts, which is not very much dependent on the biomass types. The insights revealed here can shed new light on the development of sustainable and cost‐effective ORR carbocatalysts from biomass.

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“…The scenario is different for PC 4 G and OPC 4 G motifs in which both the P‐ and C‐sites can similarly attract *OH and effectively contribute to the ORR process. For PC 4 G, the kinetically most favorable reaction pathway is shown to be the hydrogenation of O 2 molecule to form OOH followed by a further hydrogenation of OOH, resulting in H 2 O + O formation …”

Section: Nonmetallic Electrocatalystsmentioning

confidence: 99%

Oxygen Reduction Reactions on Single‐ or Few‐Atom Discrete Active Sites for Heterogeneous Catalysis

Sharifi

Gracia‐Espino

Chen

et al. 2019

Advanced Energy Materials

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The oxygen reduction reaction (ORR) is of great importance in energy‐converting processes such as fuel cells and in metal–air batteries and is vital to facilitate the transition toward a nonfossil dependent society. The ORR has been associated with expensive noble metal catalysts that facilitate the O2 adsorption, dissociation, and subsequent electron transfer. Single‐ or few‐atom motifs based on earth‐abundant transition metals, such as Fe, Co, and Mo, combined with nonmetallic elements, such as P, S, and N, embedded in a carbon‐based matrix represent one of the most promising alternatives. Often these are referred to as single atom catalysts; however, the coordination number of the metal atom as well as the type and nearest neighbor configuration has a strong influence on the function of the active sites, and a more adequate term to describe them is metal‐coordinated motifs. Despite intense research, their function and catalytic mechanism still puzzle researchers. They are not molecular systems with discrete energy states; neither can they fully be described by theories that are adapted for heterogeneous bulk catalysts. Here, recent results on single‐ and few‐atom electrocatalyst motifs are reviewed with an emphasis on reports discussing the function and the mechanism of the active sites.

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Theoretical insights on the reaction pathways for oxygen reduction reaction on phosphorus doped graphene

Cited by 64 publications

References 57 publications

Theoretical Investigation on the Reaction Pathways of the Oxygen Reduction Reaction on Graphene Codoped with Manganese and Phosphorus as a Potential Nonprecious Metal Catalyst

Theoretical Investigation on the Reaction Pathways of the Oxygen Reduction Reaction on Graphene Codoped with Manganese and Phosphorus as a Potential Nonprecious Metal Catalyst

Sustainable and Atomically Dispersed Iron Electrocatalysts Derived from Nitrogen‐ and Phosphorus‐Modified Woody Biomass for Efficient Oxygen Reduction

Oxygen Reduction Reactions on Single‐ or Few‐Atom Discrete Active Sites for Heterogeneous Catalysis

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