Low-Cost One-Step Fabrication of Highly Conductive ZnO:Cl Transparent Thin Films with Tunable Photocatalytic Properties via Aerosol-Assisted Chemical Vapor Deposition

Arreerat Jiamprasertboon; Sebastian C Dixon; Sanjayan Sathasivam; Michael J Powell; Yao Lu; Theeranun Siritanon; Claire J Carmalt

doi:10.1021/acsaelm.9b00190

Low-Cost One-Step Fabrication of Highly Conductive ZnO:Cl Transparent Thin Films with Tunable Photocatalytic Properties via Aerosol-Assisted Chemical Vapor Deposition

ACS Appl Electron Mater. 2019 Aug 27;1(8):1408-1417. doi: 10.1021/acsaelm.9b00190. Epub 2019 Jun 3.

Authors

Arreerat Jiamprasertboon^{1

2}, Sebastian C Dixon², Sanjayan Sathasivam², Michael J Powell², Yao Lu³, Theeranun Siritanon¹, Claire J Carmalt²

Affiliations

¹ School of Chemistry, Institute of Science, Suranaree University of Technology, 111 University Avenue, Muang, Nakhon Ratchasima, 30000, Thailand.
² Materials Chemistry Centre, Department of Chemistry, University College London, 20 Gordon Street, London, WC1H 0AJ, U.K.
³ Department of Mechanical Engineering, University College London, London, WC1E 7JE, U.K.

Abstract

Low-cost, high-efficiency, and high quality Cl-doped ZnO (ZnO:Cl) thin films that can simultaneously function as transparent conducting oxides (TCOs) and photocatalysts are described. The films have been fabricated by a facile and inexpensive solution-source aerosol-assisted chemical vapor deposition technique using NH₄Cl as an effective, cheap, and abundant source of Cl. Successful Cl_O substitutional doping in the ZnO films was evident from powder X-ray diffraction, X-ray photoelectron spectroscopy, and time-of-flight secondary ion mass spectrometry results, while scanning electron microscopy reveals the impact of Cl doping on the ZnO thin film morphology. All ZnO:Cl films deposited were transparent and uncolored; optical transmittance in the visible region (400-700 nm) exceeded 80% for depositions using 5-20 mol % Cl. Optimal electrical properties were achieved when using 5 mol % Cl with a minimum measured resistivity of (2.72 ± 0.04) × 10^-3 Ω·cm, in which the charge carrier concentration and mobility were measured at (8.58 ± 0.16) × 10¹⁹ cm^-3 and 26.7 ± 0.1 cm² V^-1 s^-1 respectively, corresponding to a sheet resistance (R _sh) of 41.9 Ω□^-1 at a thickness of 650 nm. In addition to transparent conducting properties, photocatalytic behavior of stearic acid degradation in the ZnO:Cl films was also observed with an optimal Cl concentration of 7 mol % Cl, with the highest formal quantum efficiency (ξ) measured at (1.63 ± 0.03) × 10^-4 molecule/photon, while retaining a visible transparency of 80% and resistivity ρ = (9.23 ± 0.13) × 10^-3 Ω·cm. The dual functionality of ZnO:Cl as both a transparent conductor and an efficient photocatalyst is a unique combination of properties making this a particularly unusual material.