Citation: Xu Chenyu, Lin Jiayi, Pan Fuqiang, Deng Bowen, Wang Zhihua, Zhou Junhu, Chen Yun, Ma Jingcheng, Gu Zhien, Zhang Yanwei. Photo-thermochemical Cycle for CO₂ Reduction based on Effective Ni ion Substitute-doped TiO₂[J]. Acta Chimica Sinica, ;2017, 75(7): 699-707. doi: 10.6023/A17030083 shu

Photo-thermochemical Cycle for CO₂ Reduction based on Effective Ni ion Substitute-doped TiO₂

Xu Chenyu ^a ,
Lin Jiayi ^a ,
Pan Fuqiang ^a ,
Deng Bowen ^a ,
Wang Zhihua ^a ,
Zhou Junhu ^a ,
Chen Yun ^b ,
Ma Jingcheng ^b ,
Gu Zhien ^b ,
Zhang Yanwei ^a,*,,

a.
State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027
b.
Zhejiang Beilun Power Generation Co., Ningbo 315000

Corresponding author: Zhang Yanwei, zhangyw@zju.edu.cn
Received Date: 2 March 2017

Fund Project: National Natural Science Foundation of China 51276170the Fundamental Research Funds for the Central Universities 2017FZA4014the Innovative Research Groups of the National Natural Science Foundation of China 51621005

Figures(16)

To study the mechanism of the photo-thermochemical cycle (PTC), titanium dioxide (ST) and Ni-doped TiO₂(NT) films were produced using a sol-gel method and applied in the PTC for CO₂ reduction.And commercial P25(PT) has been used as a compared sample.A comparison of CO production shows that Ni-doped TiO₂ performed better than undoped TiO₂ and P25.Average CO production of NT PTCs was 5.30 μmol/g-cat and it was nearly 3.13 times of ST PTCs'CO production and 2.28 times of PT PTCs'.Scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy-dispersive X-ray spectroscopy (EDXS) and X-ray diffraction (XRD) were used to assess the crystal structure and morphology of the films.Ni element could be found in NT by EDXS and inductively coupled plasma-atomic emission spectrometry (ICP-AES), and the mass fraction of Ni was 0.54% and 0.436% which were agreed with experiments.This result of XRD indicated that Ni²⁺ may have high dispersion without significant change in TiO₂ and Ni²⁺ ions were doped into the TiO₂ lattice so that Ni-O-Ti bonds were formed.Photoluminescence (PL), time-resolved PL, UV-visible diffuse reflectance spectra (UV-visible DRS) and X-ray photoelectron spectroscopy (XPS) analyses were also conducted to investigate the charge transfer and reaction mechanisms on the sample surface.The incorporation of Ni into TiO₂ resulted in a weaker PL intensity than that of bare TiO₂, which suggests that the introduction of Ni into TiO₂ effectively suppressed the undesirable recombination of electrons and holes.According to UV-visible DRS results, the Eg of PT is approximately 3.07 eV, which is smaller than that of ST (E_g=3.23 eV) and PT (E_g=3.20 eV).The narrower band gap of NT indicates that NT absorbed light with a wider wavelength range than that absorbed by ST and PT.By XPS patterns, the increase of Ni^+/0 and Ti³⁺ indicated that the VO may have been produced on the bond of Ni-O-Ti after UV illumination, and oxygen vacancies (VO) have been consumed after thermal step in PTC.Density functional theory (DFT) calculations related to the anatase (101) surface of TiO₂ and Ni doped TiO₂ was performed to verify and provide guidance for enhancing the PTC mechanism.Single and second VO formation energy have been calculated.The Ni-doped surface exhibits better performance than the undoped surface in the first step in PTC, because of its lower V_O formation energy which produce more V_O sites.Density of states (DOS) and partial density of states (PDOS) results indicated that narrow energy gap and impurity energy level of Ni-doped TiO₂ may lead to a wider wavelength range of NT.As a result, several key factors of the mechanism have been clarified.
- photo-thermal synergy,
- CO₂ conversion,
- oxygen vacancy,
- Ni substituted doping,
- DFT calculation
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Photo-thermochemical Cycle for CO2 Reduction based on Effective Ni ion Substitute-doped TiO2

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Photo-thermochemical Cycle for CO₂ Reduction based on Effective Ni ion Substitute-doped TiO₂