TMN4 complex embedded graphene as bifunctional electrocatalysts for high efficiency OER/ORR

Xue, Zhe; Zhang, Xinyu; Qin, Jiaqian; Liu, Riping

doi:10.1016/j.jechem.2020.07.018

Cited by 145 publications

(97 citation statements)

References 45 publications

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“…To analyze the efficiency of the process of electrochemical oxygen reduction, the overpotential ηORR was calculated as follows 41 where 1.20 is 1/4 of the total free energy change and Δ G i is the free energy change for each stage.…”

Section: Model and Calculation Methodsmentioning

confidence: 99%

Density Functional Theory Study of the Oxygen Reduction Reaction Mechanism on Graphene Doped with Nitrogen and a Transition Metal

et al. 2022

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The active centers of carbon nonplatinum catalysts doped with cobalt, iron, nickel, and copper have been simulated by quantum-chemical density functional theory methods. The thermodynamics of the electrochemical oxygen reduction reaction (ORR) on model catalysts has been determined. It was found that among the studied catalysts, graphene doped with cobalt and iron showed the best properties. A two-state reactivity effect has been found on a cobalt-containing catalyst, and a more detailed reaction mechanism has been proposed, including the stages of charging by an extra electron and association with water. The proposed mechanism explains several effects that have arisen during the modeling in relation to the classical mechanism.

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Section: Model and Calculation Methodsmentioning

confidence: 99%

Density Functional Theory Study of the Oxygen Reduction Reaction Mechanism on Graphene Doped with Nitrogen and a Transition Metal

et al. 2022

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“…5f shows the energy diagrams for the four PCET steps of pristine (blue line) and P-doped (red line) MoS 2 . All of the reaction steps of an ideal catalyst must be as close to 1.23 eV as possible [39]. The energy diagram for the PCET steps of pristine MoS 2 does not display the ideal "staircase" graph.…”

Section: Articles Science China Materialsmentioning

confidence: 98%

Phosphorus-doped MoS2 with sulfur vacancy defects for enhanced electrochemical water splitting

et al. 2021

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MoS 2 is a promising electrocatalyst because of its natural abundance and outstanding electrochemical stability. However, the poor conductivity and low activity limit its catalytic performance; furthermore, MoS 2 is unable to satisfy the requirements of most industrial applications. In this study, to obtain a P-doped MoS 2 catalyst with S vacancy defects, P is inserted into the MoS 2 matrix via a solid phase ion exchange at room temperature. The optimal P-doping amount is 11.4 wt%, and the resultant catalyst delivers excellent electrocatalytic properties for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) with the corresponding overpotentials of 93 and 316 mV at 10 mA cm −2 in an alkaline solution; these values surpass the overpotentials of most previously reported MoS 2 -based materials. Theoretical calculations and results demonstrate that the synergistic effect of the doped P, which forms active centers in the basal plane of MoS 2 , and S vacancy defects caused by P doping intensifies the intrinsic electronic conductivity and electrocatalytic activity of the catalyst. Density functional theory calculations demonstrate that P optimizes the free energy of the MoS 2 matrix for hydrogen adsorption, thereby considerably increasing the intrinsic activity of the doped catalyst for the HER compared with that observed from pristine MoS 2 . The enhanced catalytic activity of P-doped MoS 2 for the OER is attributed to the ability of the doped P which facilitates the adsorption of hydroxyl and hydroperoxy intermediates and reduces the reaction energy barrier. This study provides a new environmentally friendly and convenient solid-phase ion exchange method to improve the electrocatalytic capability of two-dimensional transition-metal dichalcogenides in largescale applications.

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“…The PDOS and charge density difference [60] of intermediates adsorption (Figure S4) on CoP4 indicate that the adsorption attributes to the charges transfer, originating from the hybridization between Co-d and p orbitals of oxygen -containing groups. In the last, the thermodynamic stability of CoP4 catalyst is then evaluated by AIMD simulations in the NVT ensemble (300 K).…”

Section: Highly Reactive Nature Of the Bifunctional Catalystsmentioning

confidence: 99%

Theoretical Inspection of TM-P4C Single-Atom Electrocatalyst: Ultra-High Performance for bifunctional Oxygen Reduction and Evolution Reactions

Zhu

Guan

2021

Preprint

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Developing the cost-effective or even bifunctional electrocatalysts for both oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) with industrially relevant activity is highly desired for metal-air batteries at the current stage. Herein, in this work, the catalytic performances of the single transition metal (TM) atom embeds graphene sheet with the tetra-coordinates Phosphorus (TMP4) for ORR and OER were investigated based on the density functional theory method. The results demonstrate that the most promising ORR and OER catalytic activity can achieved on the CoP4 with the smallest potential gap ∆E and the lowest overpotentials of 0.37 and 0.32 eV among all TMP4 systems, respectively, and the catalytic activity is even better than that of the traditional Pt and IrO2 catalysts. Furthermore, the AIMD calculation was conducted to confirm the thermodynamics stability of CoP4. This work screens out promising candidates for novel graphene-based bifunctional ORR and OER catalysts and provides the theoretical guidance for the development of single-atom catalysts.

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TMN4 complex embedded graphene as bifunctional electrocatalysts for high efficiency OER/ORR

Cited by 145 publications

References 45 publications

Density Functional Theory Study of the Oxygen Reduction Reaction Mechanism on Graphene Doped with Nitrogen and a Transition Metal

Density Functional Theory Study of the Oxygen Reduction Reaction Mechanism on Graphene Doped with Nitrogen and a Transition Metal

Phosphorus-doped MoS2 with sulfur vacancy defects for enhanced electrochemical water splitting

Theoretical Inspection of TM-P4C Single-Atom Electrocatalyst: Ultra-High Performance for bifunctional Oxygen Reduction and Evolution Reactions

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