THESIS
2020
xxvii, 182 pages : illustrations ; 30 cm
Abstract
Solar water splitting using photoelectrochemical (PEC) cells has emerged as one of the
most promising routes to produce hydrogen as a clean and renewable fuel source. The
functional semiconductor materials and efficient nanostructures are the key to realizing the
green hydrogen economy. My thesis research is directed at designing and constructing
sustainable semiconductor materials and nanostructures for efficient and stable solar water
splitting.
Firstly, I developed new functional photoelectrodes and heterogeneous composites to
boost the solar water splitting, including (1) the design and fabrication of the p-type ZnPbO
3
and n-type Zn
2PbO
4 as the new photoelectrodes for water reduction and oxidation,
respectively. Additionally, it was the first time that unassisted solar wate...[
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Solar water splitting using photoelectrochemical (PEC) cells has emerged as one of the
most promising routes to produce hydrogen as a clean and renewable fuel source. The
functional semiconductor materials and efficient nanostructures are the key to realizing the
green hydrogen economy. My thesis research is directed at designing and constructing
sustainable semiconductor materials and nanostructures for efficient and stable solar water
splitting.
Firstly, I developed new functional photoelectrodes and heterogeneous composites to
boost the solar water splitting, including (1) the design and fabrication of the p-type ZnPbO
3
and n-type Zn
2PbO
4 as the new photoelectrodes for water reduction and oxidation,
respectively. Additionally, it was the first time that unassisted solar water splitting was
realized by combining the CoPi/Zn
2PbO
4 photoanode and the MoS
2/ZnPbO
3 photocathode. (2)
the configuration of BiVO
4/BiFeO
3 composite with regulable polarization electric field, which
achieved with synergistic ferroelectric and piezoelectric effects, accelerating the interfacial
charge separation and transfer in heterojunction structure for PEC applications.
Secondly, I applied various strategies to fabricate the nanostructured photoelectrodes to
high performance and stability hybrid PEC systems, including (1) the novel strategy to extend
the cocatalyst loading from 1D to 3D from the photoabsorbing semiconductor (PAS) in a cross-linked conducting polymer network. This scheme has been proved to greatly increase
the redox reaction sites without decreasing the light absorption and effectively prohibit charge
recombination. (2) in-situ growth strategy to form the intertwined nanointerfaces with
uniform, continuous, fully engaged connection of the adjacent constituents. Meanwhile, the
charge transfer direction has been further enforced through band structure tuning to make the
photogenerated holes efficiently transfer through the nanointerfaces.
In my thesis, various efficient and stable photoelectrodes have been developed with
unique material properties and nanostructures for the excellent performance of solar water
splitting. The chemicals, possible reaction mechanisms and factors that may affect the final
PEC performance have been systematically investigated. Overall, these works shed light on
designing and fabricating the sustainable semiconductor materials and nanostructures for the
next-generation photoelectrodes and devices.
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