Different mole ratios of TiO2/BiVO4 nanocomposites with effective contacts have are fabricated by putting BiVO4 nanoparticles into the TiO2 sol, followed by thermal treatment at 450 °C. Based on the transient‐state surface photovoltage responses and the atmosphere‐controlled steady‐state surface photovoltage spectra, it is concluded that the photogenerated charge carriers in the TiO2/BiVO4 nanocomposite with a proper mole ratio (5%) display much longer lifetime and higher separation than those in the BiVO4 alone. This is responsible for the unexpected activity for photoelectrochemical oxidation of water, for photocatalytic production of H2, and for photocatalytic degradation of phenol as a model pollutant under visible irradiation. Moreover, it is suggested that the prolonged lifetime and increased separation of photogenerated charges in the fabricated TiO2/BiVO4 nanocomposite is attributed to the unusual spatial transfer of visible‐excited high‐energy electrons of BiVO4 to TiO2. This work will provide feasible routes to synthesize visible‐light responsive nanomaterials for efficient solar utilization.
Herein, we have fabricated rutile TiO2 nanorod-coupled α-Fe2O3 by a wet-chemical process. It is demonstrated that the visible activities for photoelectrochemical water oxidation and for degrading pollutant of α-Fe2O3 are greatly enhanced after coupling a proper amount of rutile nanorods. The enhanced activity is attributed to the prolonged lifetime and improved separation of photogenerated charges mainly by the transient surface photovoltage responses. Interestingly, the observed EPR signals (with g⊥ = 1.963 and g|| = 1.948) of Ti3+ in the fabricated TiO2-Fe2O3 nanocomposite at ultra low temperature (1.8 k) after visible laser excitation, along with the electrochemical impedance spectra and the normalized photocurrent action spectra, testify evidently that the spacial transfers of visible-excited high-energy electrons of α-Fe2O3 to TiO2 could happen. Moreover, it is confirmed that it is more favorable for the uncommon electron transfers of α-Fe2O3 to rutile than to anatase. This is responsible for the much obvious enhancement of visible activity of Fe2O3 after coupling with rutile TiO2, compared with anatase and phase-mixed P25 ones. This work would help us to deeply understand the uncommon photophysical processes, and also provide a feasible route to improve the photocatalytic performance of visible-response semiconductor photocatalyst for water splitting and pollutant degradation.
It is highly desired to enhance the visible-excited charge separation of nanosized BiVO4 for utilization in photocatalysis. Here ZnO/BiVO4 nanocomposites in different molar-ratios are fabricated by simple wet-chemical processes, after synthesis of nanosized BiVO4 and ZnO by hydrothermal methods. It is shown by means of atmosphere-controlled steady-state surface photovoltage spectra and transient-state surface photovoltage responses that the photogenerated charges of resulting nanocomposite shows longer lifetime and higher separation than that of BiVO4 alone. This leads to its superior photoactivities for water oxidation to produce O2 and for colorless pollutant degradation under visible irradiation, with about three times enhancement. Interestingly, it is suggested that the prolonged lifetime and enhanced separation of photogenerated charges in the nanocomposite is attributed to the unusual spatial transfer of visible-excited high-energy electrons, by visible radiation from BiVO4 to ZnO on the basis of the ultralow-temperature electron paramagnetic resonance measurements and the photocurrent action spectra. Moreover, it is clearly demonstrated that the photogenerated charge separation of resulting ZnO/BiVO4 nanocomposite could be further enhanced after introducing the silicate bridges so as to improve the visible photocatalytic activity greatly, attributed to the built bridge favorable to charge transfer. This work would provide a feasible way to enhance the solar energy utilization of visible-response semiconductor photocatalysts.
In this work, we have successfully constructed phosphate bridges in a TiO2-Fe2O3 nanocomposite using wet-chemical processes. Based on FTIR, XPS and TEM measurements it is confirmed that phosphate groups form bridges that effectively connect TiO2 and α-Fe2O3. From steady-state surface photovoltage spectra (SS-SPS) and transient-state surface photovoltage (TS-SPV) measurements in N2, it is clearly demonstrated that the separation and lifetime of the photogenerated charge carriers in the TiO2-Fe2O3 nanocomposite are greatly enhanced by the introduction of the phosphate bridges. As a consequence, the visible light photocatalytic activity in water reduction by methanol and the photoelectrochemical water oxidation were obviously improved after phosphate bridging. It is concluded mainly on the basis of ultra-low-temperature EPR signals, EIS spectra, and the normalized photocurrent action spectra that the photogenerated electrons of α-Fe2O3 under irradiation with visible light would transfer to TiO2 in the nanocomposite, and the built phosphate bridges are favorable for charge transportation, leading to the greatly-increased separation and lifetime of visible-light excited charge carriers. This work provides a feasible route to improve the photoactivity of other visible-response nanocomposites for water splitting.
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