Heteroepitaxial Growth of Narrow Band Gap Carbon-Rich Carbon Nitride Using In Situ Polymerization to Empower Sunlight-Driven Photoelectrochemical Water SplittingClick to copy article linkArticle link copied!
- Narendra Chaulagain*Narendra Chaulagain*Email: [email protected]Department of Electrical and Computer Engineering, University of Alberta, 9211-116 St NW, Edmonton, AB T6G 1H9, CanadaMore by Narendra Chaulagain
- Kazi M. AlamKazi M. AlamDepartment of Electrical and Computer Engineering, University of Alberta, 9211-116 St NW, Edmonton, AB T6G 1H9, CanadaMore by Kazi M. Alam
- John C. GarciaJohn C. GarciaDepartment of Electrical and Computer Engineering, University of Alberta, 9211-116 St NW, Edmonton, AB T6G 1H9, CanadaMore by John C. Garcia
- Damini VrushabendrakumarDamini VrushabendrakumarDepartment of Electrical and Computer Engineering, University of Alberta, 9211-116 St NW, Edmonton, AB T6G 1H9, CanadaMore by Damini Vrushabendrakumar
- Julian E. HegerJulian E. HegerTUM School of Natural Sciences, Chair for Functional Materials, Physics Department, Technical University of Munich, James-Franck-Str. 1, 85748 Garching, GermanyMore by Julian E. Heger
- Guangjiu PanGuangjiu PanTUM School of Natural Sciences, Chair for Functional Materials, Physics Department, Technical University of Munich, James-Franck-Str. 1, 85748 Garching, GermanyMore by Guangjiu Pan
- Navneet KumarNavneet KumarDepartment of Electrical and Computer Engineering, University of Alberta, 9211-116 St NW, Edmonton, AB T6G 1H9, CanadaMore by Navneet Kumar
- Md. Masud RanaMd. Masud RanaDepartment of Electrical and Computer Engineering, University of Alberta, 9211-116 St NW, Edmonton, AB T6G 1H9, CanadaMore by Md. Masud Rana
- Harshitha RajashekharHarshitha RajashekharDepartment of Electrical and Computer Engineering, University of Alberta, 9211-116 St NW, Edmonton, AB T6G 1H9, CanadaMore by Harshitha Rajashekhar
- Riley W. HooperRiley W. HooperDepartment of Chemistry, University of Alberta, 11337 Saskatchewan Drive NW, Edmonton, AB T6G 2G2, CanadaMore by Riley W. Hooper
- Saeid KamalSaeid KamalDepartment of Chemistry, University of British Columbia, 2036 Main Mall, Vancouver Campus, Vancouver, BC V6T 1Z1, CanadaMore by Saeid Kamal
- Vladimir K. MichaelisVladimir K. MichaelisDepartment of Chemistry, University of Alberta, 11337 Saskatchewan Drive NW, Edmonton, AB T6G 2G2, CanadaMore by Vladimir K. Michaelis
- Alkiviathes MeldrumAlkiviathes MeldrumDepartment of Physics, University of Alberta, 11335 Saskatchewan Drive NW, Edmonton, AB T6G 2H5, CanadaMore by Alkiviathes Meldrum
- Peter Müller-BuschbaumPeter Müller-BuschbaumTUM School of Natural Sciences, Chair for Functional Materials, Physics Department, Technical University of Munich, James-Franck-Str. 1, 85748 Garching, GermanyMore by Peter Müller-Buschbaum
- Karthik Shankar*Karthik Shankar*Email: [email protected]Department of Electrical and Computer Engineering, University of Alberta, 9211-116 St NW, Edmonton, AB T6G 1H9, CanadaMore by Karthik Shankar
Abstract
We describe an in situ-polymerized conformal thin layer coating of narrow band gap carbon-rich carbon nitride (NBG-CRCN) on titania nanorod arrays to design a binary semiconductor heterojunction photocatalyst. The in situ polymerization creates a strong interaction between the TiO2 nanorod substrate and the carbon nitride film, which prevents leaching of CRCN in liquid electrolytes. A unique aspect of our work is developing an easy and inexpensive technique for the heteroepitaxial growth of mechanically and photochemically stable carbon nitride thin films with intimate contact at the CN:TNR heterojunction interface. This method aids in overcoming one of the main problems with carbon nitride (CN), namely, the inability to produce an evenly distributed CN coating on a substrate. The synthesized NBG-CRCN@TNR extends the visible light absorption to 700 nm (Eg = 1.7 eV) and red-shifts the photoluminescence (PL) emission peak to 580 nm. The peak shifts and broadening in the Raman spectra of the NBG-CRCN@TNR hybrid compared to those in TNR confirm an unusually strong interaction between TiO2 and NBG-CRCN. An easy and inexpensive technique to heteroepitaxially grow CRCN (002) on rutile TiO2 (110) is confirmed by advanced characterization. High-resolution transmission electron microscopy (HRTEM), selected-area electron diffraction (SAED), and grazing-incidence wide-angle X-ray scattering (GIWAXS) suggest the heteroepitaxial growth of (002) CRCN on rutile TiO2 (110). Under AM1.5G solar illumination, the NBG-CRCN@TNR hybrid shows superior performance in photoelectrochemical water splitting, generating a photocurrent density as high as 4.3 mA cm–2 in 1 M KOH under 0.6 V external bias, rising to 8.4 mA cm–2 in the presence of a hole scavenger (methanol). An impressive hydrogen evolution rate of 26.51 μmol h–1 with 88.12% Faradaic efficiency is recorded. Establishing a high-quality interface between g-C3N4 and titania permits effective charge carrier separation, leading to enhanced photocatalytic activity.
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