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The high photocatalytic efficiency and stability of LaNiO₃/g-C₃N₄ heterojunction nanocomposites for photocatalytic water splitting to hydrogen.

ABSTRACT: A binary direct Z-scheme LaNiO₃/g-C₃N₄ nanocomposite photocatalyst consisted with LaNiO₃ nanoparticles and g-C₃N₄ nanosheets was successfully synthesized by means of mechanical mixing and solvothermal methods in order to improve the photocatalytic water splitting activity. The as-prepared materials were characterized by powder X-ray diffraction (XRD), Scanning Electron microscope (SEM), Transmission Electron microscope (TEM), X-ray photoelectron spectroscope (XPS), Fourier Transform Infrared Spectroscopy (FT-IR) and N₂ adsorption-desorption experiments, respectively, demonstrating the formation of interfacial interaction and heterogeneous structure in LaNiO₃/g-C₃N₄ nanocomposites. Under UV-light irradiation, the LaNiO₃/g-C₃N₄ samples which without the addition of any noble metal as co-catalyst behaved enhanced photocatalytic water splitting activity compared with pure LaNiO₃ and g-C₃N₄, owing to the Z-scheme charge carrier transfer pathway. Especially, the LaNiO₃/70%g-C₃N₄ nanocomposite reach an optimal yield of up to 3392.50 µmol g^-1 in 5 h and held a maximum H₂ evolution rate of 678.5 µmol h^-1 g^-1 that was 5 times higher than that of pure LaNiO₃.

SUBMITTER: Ye C

PROVIDER: S-EPMC7596961 | biostudies-literature | 2020 Oct

REPOSITORIES: biostudies-literature

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The high photocatalytic efficiency and stability of LaNiO3/g-C3N4 heterojunction nanocomposites for photocatalytic water splitting to hydrogen.

Ye Changyu C Wang Rui R Wang Haoyu H Jiang Fubin F

BMC chemistry 20201029 1

A binary direct Z-scheme LaNiO3/g-C3N4 nanocomposite photocatalyst consisted with LaNiO3 nanoparticles and g-C3N4 nanosheets was successfully synthesized by means of mechanical mixing and solvothermal methods in order to improve the photocatalytic water splitting activity. The as-prepared materials were characterized by powder X-ray diffraction (XRD), Scanning Electron microscope (SEM), Transmission Electron microscope (TEM), X-ra ...[more]

PMID: 33292406

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Project description:By photodeposition of CrOx on SrTiO3-based semiconductors doped with aliovalent Mg(II) and functionalized with Ni/NiOx catalytic nanoparticles (economically significantly more viable than commonly used Rh catalysts), an increase in apparent quantum yield (AQYs) from ∼10 to 26% in overall water splitting was obtained. More importantly, deposition of CrOx also significantly enhances the stability of Ni/NiO nanoparticles in the production of hydrogen, allowing sustained operation, even in intermittent cycles of illumination. In situ elemental analysis of the water constituents during or after photocatalysis by inductively coupled plasma mass spectrometry/optical emission spectrometry shows that after CrOx deposition, dissolution of Ni ions from Ni/NiOx-Mg:SrTiO3 is significantly suppressed, in agreement with the stabilizing effect observed, when both Mg dopant and CrOx are present. State-of-the-art electron microscopy and energy-dispersive X-ray spectroscopy (EDX) and electron energy-loss spectroscopy (EELS) analyses demonstrate that upon preparation, CrOx is photodeposited in the vicinity of several, but not all, Ni/NiOx particles. This implies the formation of a Ni-Cr mixed metal oxide, which is highly effective in water reduction. Inhomogeneities in the interfacial contact, evident from differences in contact angles between Ni/NiOx particles and the Mg:SrTiO3 semiconductor, likely affect the probability of reduction of Cr(VI) species during synthesis by photodeposition, explaining the observed inhomogeneity in the spatial CrOx distribution. Furthermore, by comparison with undoped SrTiO3, Mg-doping appears essential to provide such favorable interfacial contact and to establish the beneficial effect of CrOx. This study suggests that the performance of semiconductors can be significantly improved if inhomogeneities in interfacial contact between semiconductors and highly effective catalytic nanoparticles can be resolved by (surface) doping and improved synthesis protocols.

Dataset Information

The high photocatalytic efficiency and stability of LaNiO₃/g-C₃N₄ heterojunction nanocomposites for photocatalytic water splitting to hydrogen.

Publications

The high photocatalytic efficiency and stability of LaNiO<sub>3</sub>/g-C<sub>3</sub>N<sub>4</sub> heterojunction nanocomposites for photocatalytic water splitting to hydrogen.

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