Proceedings of MATSUS23 & Sustainable Technology Forum València (STECH23) (MATSUS23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.310
Publication date: 22nd December 2022
Solar driven photoelectrochemical (PEC) reduction to produce chemical fuel is a promising strategy for solar energy harvesting, which could address the intermittent and dispersed supply of solar energy and provide a high-density solar energy storage method in the form of chemical bonds. PEC CO2 reduction, converting CO2 into value-added chemical, has attracted significant attention because of its potential to capture and reduce the massive emission of CO2. Another desirable PEC application is NH3 synthesis from NOx reduction reaction (NOxRR), which provides not only a promising alternative to the conventional energy-intensive NH3 production process, but a sustainable solution for balancing the global nitrogen cycle by restoring ammonia from wastewater.
Kesterite Cu2ZnSnS4 (CZTS)-based photocathodes have attracted increasing research interest due to its excellent light harvesting capability, earth-abundance, and environmental-friendliness. After constructing p–n junction with CdS buffer layer, CZTS photocathode exhibits robust charge separation efficiency, which can enable an energetic photoinduced reaction driving force to power the PEC reactions. This work will present the strategies we applied to achieve high PEC reduction performance and controllable PEC reduction selectivity in both CO2 and NOx reduction.
In CO2 reduction, by introducing heat treatment (HT) strategy on CZTS/CdS photocathodes, interface charge transfer optimization and surficial S vacancy engineering have been simultaneously realized (Figure 1). HT improves the CZTS/CdS heterojunction interface by introducing elemental inter-diffusion between Cd in CdS and Cu/Zn in CZTS, leading to a more favorable p-n junction with enlarged built-in potential, prolonged carrier lifetime and suppressed charge recombination.
In NOx reduction for NH3 production, the uniquely designed CZTS photocathode by loading defect engineered TiOx cocatalyst enables selective NH3 production from NOxRR, yielding up to 89.1% Faradaic efficiency (FE) with a remarkable positive onset potential (Figure 2). By tailoring the amount of surface defective Ti3+ species, the adsorption of reactant NO3− and NO2 intermediate is significantly promoted while the full coverage of TiOx also suppresses NO2− liberation as a by-product, contributing to high NH3 selectivity.
The authors acknowledge the facilities and the scientific and technical assistance of Microscopy Australia at the Electron Microscope Unit (EMU) and other characterization facilities within the Mark Wainwright Analytical Centre (MWAC) at UNSW Sydney. The work was supported by the Australian Research Council (ARC) Training Centre for the Global Hydrogen Economy (IC200100023). X.H. acknowledges the Australian Research Council (ARC) Future Fellowship Programme (FT190100756). K.S. acknowledges the Australian Centre for Advanced Photovoltaics (ACAP) postdoctoral fellowship programme (RG172864-B). Responsibility for the views, information, or advice expressed herein is not accepted by the Australian Government. The authors acknowledge Dr. Bingqiao Xie for the valuable discussion on the reaction mechanism, and Dr. Zhipeng Ma, Jing Sun, and Chen Han for the assistance with calibration process.
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