Research Article

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2018, 11(6): 2897–2908

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https://doi.org/10.1007/s12274-017-1943-2

Ni-doped ZnCo2O4 atomic layers to boost the selectivity in solar-driven reduction of CO2

Katong Liu, Xiaodong Li, Liang Liang, Ju Wu, Xingchen Jiao, Jiaqi Xu, Yongfu Sun (*), and Yi Xie (*)

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Hefei National Laboratory for Physical Sciences at Microscale, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei 230026, China

Keywords: atomic layers, Ni-doped, zinc cobaltite, selectivity of CO2 reduction
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ABSTRACT Regulating the selectivity of CO2 photoreduction is particularly challenging. Herein, we propose ideal models of atomic layers with/without element doping to investigate the effect of doping engineering to tune the selectivity of CO2 photoreduction. Prototypical ZnCo2O4 atomic layers with/without Ni-doping were first synthesized. Density functional theory calculations reveal that introducing Ni atoms creates several new energy levels and increases the density-of-states at the conduction band minimum. Synchrotron radiation photoemission spectroscopy demonstrates that the band structures are suitable for CO2 photoreduction, while the surface photovoltage spectra demonstrate that Ni doping increases the carrier separation efficiency. In situ diffuse reflectance Fourier transform infrared spectra disclose that the CO2− radical is the main intermediate, while temperature-programed desorption curves reveal that the ZnCo2O4 atomic layers with/without Ni doping favor the respective CO and CH4 desorption. The Ni-doped ZnCo2O4 atomic layers exhibit a 3.5-time higher CO selectivity than the ZnCo2O4 atomic layers. This work establishes a clear correlation between elemental doping and selectivity regulation for CO2 photoreduction, opening new possibilities for tailoring solar-driven photocatalytic behaviors.
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Ni-doped ZnCo2O4 atomic layers to boost the selectivity in solar-driven reduction of CO2. Nano Res. 2018, 11(6): 2897–2908 https://doi.org/10.1007/s12274-017-1943-2

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