DFT investigation of the oxygen reduction reaction over nitrogen (N) doped graphdiyne as an electrocatalyst: the importance of pre-adsorbed OH* and the solvation effect

Literature Information

Publication Date 2023-09-22
DOI 10.1039/D3MA00502J
Impact Factor 0
Authors

Yuelin Wang, Thanh Ngoc Pham, Harry H. Halim, Likai Yan


View Original

Abstract

Searching for novel electrocatalysts that can replace precious platinum for oxygen reduction reaction (ORR) is important for developing fuel cells. Recently, nitrogen (N) doped graphdiyne (GDY) has been synthesized and proved that the ORR electrocatalytic activity catalyzed by N-doped GDY is significantly improved, however, the roles of sp-N (including sp-N1 and sp-N2) and pyridinic (Pyri)-N dopants in mediating the ORR are still unclear. To clarify which sp-N or Pyri-N creates the active site for ORR, we systematically studied the ORR mechanism on sp-N1GDY and pyri-NGDY supported on graphene (G) with the solvation effect, which was performed using density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations. Firstly, we found that the dissociative mechanism is preferred on sp-N1GDY/G and the surface is easily terminated by the OH* intermediates, while the OH* pre-adsorbed surface (sp-N1GDY(OH)/G) prefers the associative mechanism. Pyri-NGDY/G also prefers the associative mechanism without any termination. Then, the solvation effect stabilizes all ORR intermediates in both cases. From the calculated free energy diagram, a model with water solvent gives a more appropriate estimation of the overpotential than the one without the water solvent, and sp-N1GDY/G with OH* pre-adsorbed has a lower overpotential (0.46 V), which is close to the experimental value (0.36 V), compared with Pyri-NGDY/G (0.75 V). Our study provides useful information for understanding the reaction mechanisms of ORR at the solid/liquid interface on the N-doped GDY surface.

Related Literature

Where macro meets micro

R. Stephen Berry, Boris M. Smirnov

2014-01-09 Perspective

DOI: 10.1039/C3CP54550D

Contents list

Front/Back Matter

DOI: 10.1039/C4CP90059F

Back cover

Cover

DOI: 10.1039/C4CP90062F

Structure, fragmentation patterns, and magnetic properties of small cobalt oxide clusters

R. H. Aguilera-del-Toro, A. Vega, L. C. Balbás

2014-08-28 Paper

DOI: 10.1039/C4CP03370A

Sensitivity of local hydration behaviour and conformational preferences of peptides to choice of water model

Divya Nayar, Charusita Chakravarty

2014-02-10 Paper

DOI: 10.1039/C3CP55147D

Unraveling non-covalent interactions within flexible biomolecules: from electron density topology to gas phase spectroscopy

R. Chaudret, B. de Courcy, J. Contreras-García, A. Zehnacker-Rentien, J.-P. Piquemal

2013-10-11 Paper

DOI: 10.1039/C3CP52774C

Bandgap opening/closing of graphene antidot lattices with zigzag-edged hexagonal holes

Shenglin Peng, Zhixiong Yang, Yu Chen, Hui Zou, Xiang Xiong

2014-08-05 Paper

DOI: 10.1039/C4CP02090A

Theoretical investigation on structural and electronic properties of organic dye C258 on TiO2(101) surface in dye-sensitized solar cells

Ping-Ping Sun, Quan-Song Li, Li-Na Yang, Zhu-Zhu Sun, Ze-Sheng Li

2014-08-26 Paper

DOI: 10.1039/C4CP02951H

Ultrafast resonance energy transfer in the umbelliferone–alizarin bichromophore

Pierangelo Fabbrizzi, Luisa Lascialfari, Stefano Cicchi, Malgorzata Biczysko, Fabrizio Santoro

2014-01-23 Paper

DOI: 10.1039/C3CP54609H

You might also like

Compound Q&A

What precautions should be taken when handling 2-Chloro-1,2-bis(4-methylphenyl)ethanone (CAS: 71193-32-3)?

When handling 2-Chloro-1,2-bis(4-methylphenyl)ethanone (CAS: 71193-32-3), it is ...

71193-32-32-Chloro-1,2-bis(4-m...
Compound Q&A

What industries use 4-Ethoxy-3-(5-methyl-4-oxo-7-propyl-1,4-dihydroimidazo[5,1-f][1,2,4]triazin-2-yl)benzenesulfonyl chloride (CAS: 224789-26-8)?

4-Ethoxy-3-(5-methyl-4-oxo-7-propyl-1,4-dihydroimidazo[5,1-f][1,2,4]triazin-2-yl...

224789-26-84-Ethoxy-3-(5-methyl...
Compound Q&A

How should Methyl 3-Oxo-4-Androsten-17-Carboxylate (CAS: 2681-55-2) be stored?

Methyl 3-Oxo-4-Androsten-17-Carboxylate (CAS: 2681-55-2) should be stored in a c...

2681-55-2Methyl 3-Oxo-4-Andro...
Compound Q&A

What are the main uses of (R)-3-Amino-4-(3-hexylphenylamino)-4-oxobutylphosphonic acid (CAS: 909725-61-7)?

(R)-3-Amino-4-(3-hexylphenylamino)-4-oxobutylphosphonic acid is primarily used i...

909725-61-7(R)-3-Amino-4-(3-hex...
Compound Q&A

What regulatory guidelines apply to 2-Methyl-2-propanyl 3-amino-3-carbamoyl-1-azetidinecarboxylate (CAS: 1254120-14-3)?

2-Methyl-2-propanyl 3-amino-3-carbamoyl-1-azetidinecarboxylate (CAS: 1254120-14-...

1254120-14-32-Methyl-2-propanyl ...
Compound Q&A

Are there alternatives to (E)-4-(tert-Butoxy)-4-oxobut-2-enoic acid (CAS: 135355-96-3) in synthesis?

There are alternative reagents that can be used in synthesis instead of (E)-4-(t...

135355-96-3(E)-4-(tert-Butoxy)-...
Compound Q&A

What are the physical and chemical properties of [2-(3-Chlorophenyl)-1,3-thiazol-4-yl]methanol (CAS: 121202-20-8)?

[2-(3-Chlorophenyl)-1,3-thiazol-4-yl]methanol (CAS: 121202-20-8) is a crystallin...

121202-20-8[2-(3-Chlorophenyl)-...
166249-17-8Methyl (2S)-[(4S)-2,...
Compound Q&A

What is the market or research trend for 1-Bromo-2-isocyanatoethane (CAS: 42865-19-0)?

The market for 1-Bromo-2-isocyanatoethane (CAS: 42865-19-0) is driven by its use...

42865-19-01-Bromo-2-isocyanato...
Compound Q&A

What are the main uses of 4-Nitro-D-phenylalanine hydrochloride (CAS: 147065-06-3)?

4-Nitro-D-phenylalanine hydrochloride (CAS: 147065-06-3) is primarily used in re...

147065-06-34-Nitro-D-phenylalan...
Disclaimer
This page provides academic journal information for reference and research purposes only. We are not affiliated with any journal publishers and do not handle publication submissions. For publication-related inquiries, please contact the respective journal publishers directly.
If you notice any inaccuracies in the information displayed, please contact us at support@chemtradehub.com. We will promptly review and address your concerns.