Juncao Bian

Efficient Emission Facilitated by Multiple Energy Level Transitions in Uniform Graphitic Carbon Nitride Films Deposited by Thermal Vapor Condensation

Graphitic carbon nitride (g-CN) films are important components of optoelectronic devices, but current techniques for their production, such as drop casting and spin coating, fail to deliver uniform and pinhole-free g-CN films on solid substrates. Here, versatile, cost-effective, and large-area growth of uniform and pinhole-free g-CN films is achieved by using a thermal vapor condensation method under atmospheric pressure. A comparison of the X-ray diffraction and Fourier transform infrared data with the calculated infrared spectrum confirmed the graphitic build-up of films composed of tri-s-triazine units. These g-CN films possess multiple active energy states including π*, π, and lone-pair states, which facilitate their efficient (6% quantum yield in the solid state) photoluminescence, as confirmed by both experimental measurements and theoretical calculations.

Graphitic Carbon Nitride Film: An Emerging Star for Catalytic and Optoelectronic Applications

Graphitic carbon nitride (g-CN) is a unique organic semiconductor that has been widely applied as a visible-light-driven photocatalyst. However, these applications are primarily based on g-CN powders. Applications of g-CN in devices are hindered because of difficulties associated with the synthesis of high-quality g-CN films. This work reviews the latest advances in g-CN films. The deposition methods are summarized and the structural, optical, and electronic properties of g-CN films and their applications in catalysis, solar cells, and light-emitting diodes are outlined. Moreover, the challenges remaining in this field are also discussed.

C=C π Bond Modified Graphitic Carbon Nitride Films for Enhanced Photoelectrochemical Cell Performance

Applications of graphitic carbon nitride (g-CN) in photoelectrochemical and optoelectronic devices are still hindered due to the difficulties in synthesis of g-CN films with tunable chemical, physical and catalytic properties. Herein we present a general method to alter the electronic and photoelectrochemical properties of g-CN films by annealing. We found that N atoms can be removed from the g-CN networks after annealing treatment. Assisted by theoretical calculations, we confirm that upon appropriate N removal, the adjacent C atoms will form new C=C π bonds. Detailed calculations demonstrate that the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) are located at the structure unit with C=C π bonds and the electrons are more delocalized. Valence band X-ray photoelectron spectroscopy spectra together with optical absorption spectra unveil that the structure changes result in the alteration of the g-CN energy levels and position of band edges. Our results show that the photocurrent density of the annealed g-CN film is doubled compared with the pristine one, thanks to the better charge separation and transport within the film induced by the new C=C π bonds. An ultrathin TiO2 film (2.2 nm) is further deposited on the g-CN film as stabilizer and the photocurrent density is kept at 0.05 mA cm-2 at 1.23 V versus reversible hydrogen electrode after two-cycle stability assessment. This work enables the applications of g-CN films in many electronic and optoelectronic devices.