Abstract
A novel 2D ultrathin Ag/AgI-δ-Bi2O3 photocatalyst was constructed by a facile hydrothermal and in situ photodeposition method, which presented a uniform nanosheet structure with an average height of 6 nm. Its composition, morphology and light-harvesting properties were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), transmission electron microscopy (TEM), UV–vis spectrophotometer (UV–vis) and photoluminescence (PL) measurements in detail. The Ag/AgI-δ-Bi2O3 nanocomposites showed an excellent photocatalytic nitrogen fixation performance of 420 μmol L−1 g−1 h−1 in water without any sacrificial agent. The introduction of Ag/AgI nanoparticles caused the morphology modification of δ-Bi2O3, a higher concentration of oxygen vacancy, and the construction of a plasmon sensitized heterojunction, resulting in enhanced light absorption, improved separation efficiency of charge carriers and strong N2 absorption and activation ability, which are responsible for the superior photocatalytic performance of Ag/AgI-δ-Bi2O3.
Highlights
Ammonia (NH3) is one of the most important chemical products due to its role in natural biological processes as a hydrogen carrier and for the synthesis of many nitrogenous compounds [1]
We developed a facile hydrothermal method to synthesize δ-Bi2O3 microcrystals at a low temperature, and a Ag/AgI-δ-Bi2O3 photocatalyst was further prepared via a precipitation and photoreduction route, which was used as the photocatalyst for nitrogen fixation which achieved remarkably improved N2 photoconversion activity compared to that of a pure δ-Bi2O3 photocatalyst
The surface chemical composition of the as-prepared sample was measured by X-ray photoelectron spectroscopy (XPS)
Summary
Ammonia (NH3) is one of the most important chemical products due to its role in natural biological processes as a hydrogen carrier and for the synthesis of many nitrogenous compounds [1]. It has been reported that the presence of oxygen vacancies can promote light harvesting and charge carrier separation efficiency, especially improving the adsorption and activation ability of N2 in the photocatalytic nitrogen fixation reaction [6,19,20]. The new plasmon resonance photocatalyst silver/silver halides (Ag/AgX, X = Cl, Br, I) attracted much attention when combined with other semiconductor photocatalytic materials, because Ag/AgX hybrid materials dramatically increase visible light utilization and promote photogenerated charge separation [24,25,26]. The combination of δ-Bi2O3 and Ag/AgX composites could provide new opportunities for developing highly efficient visible-light driven nitrogen fixation photocatalysts due to the LSPR effect and the heterostructure. The mechanism of photocatalytic nitrogen fixation of the Ag/AgI-δ-Bi2O3 photocatalyst was proposed according to the results of systematic analysis, such as photoluminescence (PL), alternating current (AC) impedance, photocurrent response, and fluorescence life and DMPO (5,5-dimethyl-1-pyrroline-N-oxide)–electron spin resonance (ESR)
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