Exploring the role of electronic structure on photo-catalytic behavior of carbon-nitride polymorphs

Datta, Sujoy; Singh, Prashant; Jana, Debnarayan; Chaudhuri, Chhanda B.; Harbola, Manoj K.; Johnson, Duane D.; Mookerjee, Abhijit

doi:10.1016/j.carbon.2020.04.008

Exploring the role of electronic structure on photo-catalytic behavior of carbon-nitride polymorphs

Journal Article · Sun May 03 00:00:00 EDT 2020 · Carbon

DOI:https://doi.org/10.1016/j.carbon.2020.04.008· OSTI ID:1617025

Datta, Sujoy ^[1]; Singh, Prashant ^[2]; Jana, Debnarayan ^[3]; Chaudhuri, Chhanda B. ^[4]; Harbola, Manoj K. ^[5]; Johnson, Duane D. ^[2]; Mookerjee, Abhijit ^[6]

Univ. of Calcutta, Kolkata (India); Lady Brabourne College, Kolkata (India)
Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
Univ. of Calcutta, Kolkata (India)
Lady Brabourne College, Kolkata (India)
Indian Inst. of Technology, Kanpur (India)
S.N. Bose National Centre for Basic Sciences, Salt Lake City, Kolkata (India)

A fully self-consistent density-functional theory (DFT) with improved functionals is used herein 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 N^th-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.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1617025

Alternate ID(s):: OSTI ID: 1691841

Report Number(s):: IS-J--10,194

Journal Information:: Carbon, Journal Name: Carbon Vol. 168; ISSN 0008-6223

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (67)

High-Performance Coral Reef-like Carbon Nitrides: Synthesis and Application in Photocatalysis and Heavy Metal Ion Adsorption Tan, Jeannie Z. Y.; Nursam, Natalita M.; Xia, Fang ACS Applied Materials & Interfaces, Vol. 9, Issue 5 https://doi.org/10.1021/acsami.6b11427	journal	January 2017
Boron- and Fluorine-Containing Mesoporous Carbon Nitride Polymers: Metal-Free Catalysts for Cyclohexane Oxidation Wang, Yong; Zhang, Jinshui; Wang, Xinchen Angewandte Chemie International Edition, Vol. 49, Issue 19 https://doi.org/10.1002/anie.201000120	journal	March 2010
Triazine-Based Graphitic Carbon Nitride: a Two-Dimensional Semiconductor Algara-Siller, Gerardo; Severin, Nikolai; Chong, Samantha Y. Angewandte Chemie International Edition, Vol. 53, Issue 29 https://doi.org/10.1002/anie.201402191	journal	May 2014
Recent Developments in Graphitic Carbon Nitride Based Hydrogels as Photocatalysts Hu, Chechia; Lin, Yan‐Ru; Yang, Hung‐Chun ChemSusChem, Vol. 12, Issue 9 https://doi.org/10.1002/cssc.201802257	journal	November 2018
Ultra fine carbon nitride nanocrystals synthesized by laser ablation in liquid solution Yang, Li; May, Paul W.; Yin, Lei Journal of Nanoparticle Research, Vol. 9, Issue 6 https://doi.org/10.1007/s11051-006-9192-4	journal	January 2007
Is carbon nitride harder than diamond? No, but its girth increases when stretched (negative Poisson ratio) Guo, Yuejin; Goddard, William A. Chemical Physics Letters, Vol. 237, Issue 1-2 https://doi.org/10.1016/0009-2614(95)00267-8	journal	May 1995
First-principle calculation study of tri-s-triazine-based g-C3N4: A review Zhu, Bicheng; Zhang, Liuyang; Cheng, Bei Applied Catalysis B: Environmental, Vol. 224 https://doi.org/10.1016/j.apcatb.2017.11.025	journal	May 2018
Creation of graphene allotropes using patterned defects Lusk, Mark T.; Carr, L. D. Carbon, Vol. 47, Issue 9 https://doi.org/10.1016/j.carbon.2009.04.014	journal	August 2009
Production, properties and potential of graphene Soldano, Caterina; Mahmood, Ather; Dujardin, Erik Carbon, Vol. 48, Issue 8 https://doi.org/10.1016/j.carbon.2010.01.058	journal	July 2010
Ab-initio calculation of electronic and optical properties of nitrogen and boron doped graphene nanosheet Nath, Palash; Chowdhury, Suman; Sanyal, D. Carbon, Vol. 73 https://doi.org/10.1016/j.carbon.2014.02.064	journal	July 2014
Electronic and pseudomagnetic properties of hybrid carbon/boron-nitride nanomaterials via ab-initio calculations and elasticity theory Shayeganfar, Farzaneh; Shahsavari, Rouzbeh Carbon, Vol. 99 https://doi.org/10.1016/j.carbon.2015.12.050	journal	April 2016
Phosphorous-modified bulk graphitic carbon nitride: Facile preparation and application as an acid-base bifunctional and efficient catalyst for CO2 cycloaddition with epoxides Lan, Dong-Hui; Wang, Hong-Tao; Chen, Lang Carbon, Vol. 100 https://doi.org/10.1016/j.carbon.2015.12.098	journal	April 2016
Photocatalysts based on g-C3N4-encapsulating carbon spheres with high visible light activity for photocatalytic hydrogen evolution Li, Kui; Xie, Xin; Zhang, Wei-De Carbon, Vol. 110 https://doi.org/10.1016/j.carbon.2016.09.039	journal	December 2016
Extreme static compression of carbon to terapascal pressures Wu, Hao; Luo, Xudong; Wen, Libin Carbon, Vol. 144 https://doi.org/10.1016/j.carbon.2018.12.004	journal	April 2019
Self-hybridized coralloid graphitic carbon nitride deriving from deep eutectic solvent as effective visible light photocatalysts Yu, Xiang; Fan, Tingting; Chen, Wenwen Carbon, Vol. 144 https://doi.org/10.1016/j.carbon.2018.12.104	journal	April 2019
Band gap of C3N4 in the GW approximation Xu, Yuan; Gao, Shang-Peng International Journal of Hydrogen Energy, Vol. 37, Issue 15 https://doi.org/10.1016/j.ijhydene.2012.04.138	journal	August 2012
First principles phonon calculations in materials science Togo, Atsushi; Tanaka, Isao Scripta Materialia, Vol. 108 https://doi.org/10.1016/j.scriptamat.2015.07.021	journal	November 2015
STM-electroluminescence from clustered C3N4 nanodomains synthesized via green chemistry process Andrade, E. P.; Costa, B. B. A.; Chaves, C. R. Ultrasonics Sonochemistry, Vol. 40 https://doi.org/10.1016/j.ultsonch.2017.08.021	journal	January 2018
Graphitic Carbon Nitride (g-C ₃ N ₄ )-Based Photocatalysts for Artificial Photosynthesis and Environmental Remediation: Are We a Step Closer To Achieving Sustainability? Ong, Wee-Jun; Tan, Lling-Lling; Ng, Yun Hau Chemical Reviews, Vol. 116, Issue 12 https://doi.org/10.1021/acs.chemrev.6b00075	journal	May 2016
Band Engineering of Carbon Nitride Monolayers by N-Type, P-Type, and Isoelectronic Doping for Photocatalytic Applications Makaremi, Meysam; Grixti, Sean; Butler, Keith T. ACS Applied Materials & Interfaces, Vol. 10, Issue 13 https://doi.org/10.1021/acsami.8b01729	journal	March 2018
Powder Synthesis and Characterization of Amorphous Carbon Nitride Khabashesku, Valery N.; Zimmerman, John L.; Margrave, John L. Chemistry of Materials, Vol. 12, Issue 11 https://doi.org/10.1021/cm000328r	journal	November 2000
Polymer Semiconductors for Artificial Photosynthesis: Hydrogen Evolution by Mesoporous Graphitic Carbon Nitride with Visible Light Wang, Xinchen; Maeda, Kazuhiko; Chen, Xiufang Journal of the American Chemical Society, Vol. 131, Issue 5 https://doi.org/10.1021/ja809307s	journal	February 2009
A Strategy of Enhancing the Photoactivity of g-C ₃ N ₄ via Doping of Nonmetal Elements: A First-Principles Study Ma, Xinguo; Lv, Yanhui; Xu, Jing The Journal of Physical Chemistry C, Vol. 116, Issue 44 https://doi.org/10.1021/jp308334x	journal	October 2012
Elasticity and constitution of the Earth's interior Birch, Francis Journal of Geophysical Research, Vol. 57, Issue 2 https://doi.org/10.1029/JZ057i002p00227	journal	June 1952
Limiting and realizable efficiencies of solar photolysis of water Bolton, James R.; Strickler, Stewart J.; Connolly, John S. Nature, Vol. 316, Issue 6028, p. 495-500 https://doi.org/10.1038/316495a0	journal	August 1985
A stable compound of helium and sodium at high pressure Dong, Xiao; Oganov, Artem R.; Goncharov, Alexander F. Nature Chemistry, Vol. 9, Issue 5 https://doi.org/10.1038/nchem.2716	journal	February 2017
A metal-free polymeric photocatalyst for hydrogen production from water under visible light Wang, Xinchen; Maeda, Kazuhiko; Thomas, Arne Nature Materials, Vol. 8, Issue 1 https://doi.org/10.1038/nmat2317	journal	November 2008
The phase diagram and hardness of carbon nitrides Dong, Huafeng; Oganov, Artem R.; Zhu, Qiang Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep09870	journal	May 2015
Chemical synthesis of turbostratic carbon nitride, containing C–N crystallites, at atmospheric pressure Qiu, Yu; Gao, Lian Chem. Commun., Issue 18 https://doi.org/10.1039/B307086G	journal	January 2003
A general framework for the assessment of solar fuel technologies Herron, Jeffrey A.; Kim, Jiyong; Upadhye, Aniruddha A. Energy & Environmental Science, Vol. 8, Issue 1 https://doi.org/10.1039/C4EE01958J	journal	January 2015
Linear and nonlinear optical properties for AA and AB stacking of carbon nitride polymorph (C ₃ N ₄ ) Reshak, A. H.; Khan, Saleem Ayaz; Auluck, S. RSC Adv., Vol. 4, Issue 23 https://doi.org/10.1039/C4RA00388H	journal	January 2014
Engineering heterogeneous semiconductors for solar water splitting Li, Xin; Yu, Jiaguo; Low, Jingxiang Journal of Materials Chemistry A, Vol. 3, Issue 6 https://doi.org/10.1039/C4TA04461D	journal	January 2015
A tunable and sizable bandgap of a g-C ₃ N ₄ /graphene/g-C ₃ N ₄ sandwich heterostructure: a van der Waals density functional study Dong, M. M.; He, C.; Zhang, W. X. Journal of Materials Chemistry C, Vol. 5, Issue 15 https://doi.org/10.1039/C7TC00386B	journal	January 2017
Spinel photocatalysts for environmental remediation, hydrogen generation, CO ₂ reduction and photoelectrochemical water splitting Chandrasekaran, Sundaram; Bowen, Chris; Zhang, Peixin Journal of Materials Chemistry A, Vol. 6, Issue 24 https://doi.org/10.1039/C8TA03669A	journal	January 2018
Acetylenic linkage dependent electronic and optical behaviour of morphologically distinct ‘-ynes’ Jana, Susmita; Bandyopadhyay, Arka; Jana, Debnarayan Physical Chemistry Chemical Physics, Vol. 21, Issue 25 https://doi.org/10.1039/C9CP01914F	journal	January 2019
Stability and electronic property investigations of the graphitic C3N4 system showing an orthorhombic unit cell Mattesini, Maurizio; Matar, Samir F.; Etourneau, Jean Journal of Materials Chemistry, Vol. 10, Issue 3 https://doi.org/10.1039/a908903i	journal	January 2000
Crystal facet engineering of semiconductor photocatalysts: motivations, advances and unique properties Liu, Gang; Yu, Jimmy C.; Lu, Gao Qing (Max) Chemical Communications, Vol. 47, Issue 24 https://doi.org/10.1039/c1cc10665a	journal	January 2011
Graphene/g-C3N4 bilayer: considerable band gap opening and effective band structure engineering Li, Xinru; Dai, Ying; Ma, Yandong Physical Chemistry Chemical Physics, Vol. 16, Issue 9 https://doi.org/10.1039/c3cp54592j	journal	January 2014
Detailed Balance Limit of Efficiency of p‐n Junction Solar Cells Shockley, William; Queisser, Hans J. Journal of Applied Physics, Vol. 32, Issue 3, p. 510-519 https://doi.org/10.1063/1.1736034	journal	March 1961
Efficient hybrid density functional calculations in solids: Assessment of the Heyd–Scuseria–Ernzerhof screened Coulomb hybrid functional Heyd, Jochen; Scuseria, Gustavo E. The Journal of Chemical Physics, Vol. 121, Issue 3, p. 1187-1192 https://doi.org/10.1063/1.1760074	journal	July 2004
The Compressibility of Media under Extreme Pressures Murnaghan, F. D. Proceedings of the National Academy of Sciences, Vol. 30, Issue 9 https://doi.org/10.1073/pnas.30.9.244	journal	September 1944
Deriving accurate work functions from thin-slab calculations Fall, C. J.; Binggeli, N.; Baldereschi, A. Journal of Physics: Condensed Matter, Vol. 11, Issue 13 https://doi.org/10.1088/0953-8984/11/13/006	journal	January 1999
Hardness and thermal stability of cubic silicon nitride Jiang, J. Z.; Kragh, F.; Frost, D. J. Journal of Physics: Condensed Matter, Vol. 13, Issue 22 https://doi.org/10.1088/0953-8984/13/22/111	journal	May 2001
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials Giannozzi, Paolo; Baroni, Stefano; Bonini, Nicola Journal of Physics: Condensed Matter, Vol. 21, Issue 39, Article No. 395502 https://doi.org/10.1088/0953-8984/21/39/395502	journal	September 2009
Advanced capabilities for materials modelling with Quantum ESPRESSO Giannozzi, P.; Andreussi, O.; Brumme, T. Journal of Physics: Condensed Matter, Vol. 29, Issue 46 https://doi.org/10.1088/1361-648X/aa8f79	journal	October 2017
Simple correction to bandgap problems in IV and III–V semiconductors: an improved, local first-principles density functional theory Datta, Sujoy; Singh, Prashant; Chaudhuri, Chhanda B. Journal of Physics: Condensed Matter, Vol. 31, Issue 49 https://doi.org/10.1088/1361-648X/ab34ad	journal	September 2019
Exchange-correlation potential with correct asymptotic behavior van Leeuwen, R.; Baerends, E. J. Physical Review A, Vol. 49, Issue 4 https://doi.org/10.1103/PhysRevA.49.2421	journal	April 1994
Exact results for the charge and spin densities, exchange-correlation potentials, and density-functional eigenvalues Almbladh, C. -O.; von Barth, U. Physical Review B, Vol. 31, Issue 6 https://doi.org/10.1103/PhysRevB.31.3231	journal	March 1985
Calculated quasiparticle band gap of β- C 3 N 4 Corkill, Jennifer L.; Cohen, Marvin L. Physical Review B, Vol. 48, Issue 23 https://doi.org/10.1103/PhysRevB.48.17622	journal	December 1993
Optical properties of β- C 3 N 4 and its pressure dependence Yao, Hongyu; Ching, W. Y. Physical Review B, Vol. 50, Issue 15 https://doi.org/10.1103/PhysRevB.50.11231	journal	October 1994
Surface energies, work functions, and surface relaxations of low-index metallic surfaces from first principles Singh-Miller, Nicholas E.; Marzari, Nicola Physical Review B, Vol. 80, Issue 23 https://doi.org/10.1103/PhysRevB.80.235407	journal	December 2009
Elastic and structural instability of cubic Sn 3 N 4 and C 3 N 4 under pressure Pradhan, Gopal K.; Kumar, Anil; Deb, S. K. Physical Review B, Vol. 82, Issue 14 https://doi.org/10.1103/PhysRevB.82.144112	journal	October 2010
Variations in the work function of doped single- and few-layer graphene assessed by Kelvin probe force microscopy and density functional theory Ziegler, D.; Gava, P.; Güttinger, J. Physical Review B, Vol. 83, Issue 23 https://doi.org/10.1103/PhysRevB.83.235434	journal	June 2011
Necessary and sufficient elastic stability conditions in various crystal systems Mouhat, Félix; Coudert, François-Xavier Physical Review B, Vol. 90, Issue 22 https://doi.org/10.1103/PhysRevB.90.224104	journal	December 2014
Interpolation across a muffin-tin interstitial using localized linear combinations of spherical waves Nohara, Yoshiro; Andersen, O. K. Physical Review B, Vol. 94, Issue 8 https://doi.org/10.1103/PhysRevB.94.085148	journal	August 2016
Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces Perdew, John P.; Ruzsinszky, Adrienn; Csonka, Gábor I. Physical Review Letters, Vol. 100, Issue 13 https://doi.org/10.1103/PhysRevLett.100.136406	journal	April 2008
Lattice Instability during Solid-Solid Structural Transformations under a General Applied Stress Tensor: Example of Si I → Si II with Metallization Zarkevich, Nikolai A.; Chen, Hao; Levitas, Valery I. Physical Review Letters, Vol. 121, Issue 16 https://doi.org/10.1103/PhysRevLett.121.165701	journal	October 2018
Band Offsets in Lattice-Matched Heterojunctions: A Model and First-Principles Calculations for GaAs/AlAs Baldereschi, Alfonso; Baroni, Stefano; Resta, Raffaele Physical Review Letters, Vol. 61, Issue 6 https://doi.org/10.1103/PhysRevLett.61.734	journal	August 1988
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Interesting Physical Properties of the New Spinel Phase of Si 3 N 4 and C 3 N 4 Mo, Shang-Di; Ouyang, Lizhi; Ching, W. Y. Physical Review Letters, Vol. 83, Issue 24 https://doi.org/10.1103/PhysRevLett.83.5046	journal	December 1999
Oxygen chemisorption and oxide formation on Si(111) and Si(100) surfaces Hollinger, G.; Himpsel, F. J. Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 1, Issue 2 https://doi.org/10.1116/1.572199	journal	April 1983
Experimental estimation of the band gap in silicon and germanium from the temperature–voltage curve of diode thermometers Precker, Jürgen W.; da Silva, Marcı́lio A. American Journal of Physics, Vol. 70, Issue 11 https://doi.org/10.1119/1.1512658	journal	November 2002
Low-Compressibility Carbon Nitrides Teter, D. M.; Hemley, R. J. Science, Vol. 271, Issue 5245 https://doi.org/10.1126/science.271.5245.53	journal	January 1996
ELECTRONIC STRUCTURE OF SIX PHASES OF C ₃ N ₄ : A THEORETICAL APPROACH Molina, B.; Sansores, L. E. Modern Physics Letters B, Vol. 13, Issue 06n07 https://doi.org/10.1142/S0217984999000269	journal	March 1999
Materials for Photo-Electrochemical Water Splitting Meda, L.; Abbondanza, L. Reviews in Advanced Sciences and Engineering, Vol. 2, Issue 3 https://doi.org/10.1166/rase.2013.1034	journal	September 2013
Third-Generation TB-LMTO Andersen, O. K.; Arcangeli, C.; Tank, R. W. MRS Proceedings, Vol. 491 https://doi.org/10.1557/PROC-491-3	journal	January 1997
Photocatalytic Water Splitting—The Untamed Dream: A Review of Recent Advances Jafari, Tahereh; Moharreri, Ehsan; Amin, Alireza Molecules, Vol. 21, Issue 7 https://doi.org/10.3390/molecules21070900	journal	July 2016

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36 MATERIALS SCIENCE
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photocatalysis
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Exploring the role of electronic structure on photo-catalytic behavior of carbon-nitride polymorphs

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