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Exploring the role of electronic structure on photo-catalytic behavior of carbon-nitride (C3N4) polymorphs
Carbon
  • Sujoy Datta, University of Calcutta and Lady Brabourne College
  • Prashant Singh, Ames Laboratory
  • Debnarayan Jana, University of Calcutta
  • Chhanda B. Chaudhuri, Lady Brabourne College
  • Manoj K. Harbola, Indian Institute of Technology
  • Duane D. Johnson, Iowa State University and Ames Laboratory
  • Abhijit Mookerjee, S. N. Bose National Centre for Basic Sciences
Document Type
Article
Publication Version
Accepted Manuscript
Publication Date
5-3-2020
DOI
10.1016/j.carbon.2020.04.008
Abstract

A fully self-consistent density-functional theory (DFT) with improved functionals is used to provide a comprehensive account of structural, electronic, and optical properties of C3N4 polymorphs. Using our recently developed van Leeuwen-Baerends (vLB) corrected local-density approximation (LDA), we implemented LDA + vLB within full-potential Nth-order muffin-tin orbital (FP-NMTO) method and show that it improves structural properties and band gaps compared to semi-local functionals (LDA/GGA). We demonstrate that the LDA + vLB predicts band-structure and work-function for well-studied 2D-graphene and bulk-Si in very good agreement with experiments, and more exact hybrid functional (HSE) calculations as implemented in the Quantum-Espresso (QE) package. The structural and electronic-structure (band gap) properties of C3N4 polymorphs calculated using FP-NMTO-LDA + vLB is compared with more sophisticated hybrid-functional calculations. We also perform detailed investigation of photocatalytic behavior using QE-HSE method of C3N4 polymorphs through work-function, band (valence and conduction) position with respect to water reduction and oxidation potential. Our results show γ-C3N4 as the best candidate for photocatalysis among all the C3N4 polymorphs but it is dynamically unstable at ‘zero’ pressure. We show that γ-C3N4 can be stabilized under hydrostatic-pressure, which improves its photocatalytic behavior relative to water reduction and oxidation potentials.

Comments

This is a manuscript of the article Datta, Sujoy, Prashant Singh, Debnarayan Jana, Chhanda B. Chaudhuri, Manoj K. Harbola, Duane D. Johnson, and Abhijit Mookerjee. "Exploring the role of electronic structure on photo-catalytic behavior of carbon-nitride polymorphs." Carbon (2020). DOI: 10.1016/j.carbon.2020.04.008. Posted with permission.

Creative Commons License
Creative Commons Attribution-NonCommercial-No Derivative Works 4.0 International
Copyright Owner
Elsevier Ltd.
Language
en
File Format
application/pdf
Citation Information
Sujoy Datta, Prashant Singh, Debnarayan Jana, Chhanda B. Chaudhuri, et al.. "Exploring the role of electronic structure on photo-catalytic behavior of carbon-nitride (C3N4) polymorphs" Carbon (2020)
Available at: http://works.bepress.com/duane_johnson/143/