Designing low-cost and high-performance photoelectrodes with improved light harvesting and charge separation rates is significant in photoelectrochemical water splitting.Here,a novel TiO2/Cu2O/Al/Al2O3 photoelectrode ...Designing low-cost and high-performance photoelectrodes with improved light harvesting and charge separation rates is significant in photoelectrochemical water splitting.Here,a novel TiO2/Cu2O/Al/Al2O3 photoelectrode is manufactured by depositing plasmonic nanoparticles of the non-noble metal Al on the surface of a TiO2/Cu2O core/shell heterojunction for the first time.The Al nanoparticles,which exhibit a surface plasmon resonance(SPR)effect and are substantially less expensive than noble metals such as Au and Ag,generate hot electron-hole pairs and amplify the electromagnetic field at the interface under illumination.The as-prepared TiO2/Cu2O/Al/Al2O3 photoelectrodes have an extended absorption range and enhanced carrier separation and transfer.Their photocurrent density of 4.52 mA·cm^-2 at 1.23 V vs.RHE represents an 1.84-fold improvement over that of TiO2/Cu2O.Specifically,the ultrathin Al2O3 passivation layer spontaneously generated on the surface of Al in air could act as a protective layer to significantly increase its stability.In this work,the synergistic effect of the heterojunctions and the SPR effect of the non-noble metal Al significantly improve the photoelectrode performance,providing a novel concept for the design of electrodes with good properties and high practicability.展开更多
The decomposition of Cull nanoparticles in aqueous solution has been successfully developed as a novel method for the preparation of Cu2O nanoparticles. In particular, we found that the decomposition of Cull nanoparti...The decomposition of Cull nanoparticles in aqueous solution has been successfully developed as a novel method for the preparation of Cu2O nanoparticles. In particular, we found that the decomposition of Cull nanoparticles in aqueous solution could be catalyzed by Au colloids, forming CU2O-Au nanocomposites. The composition and structure of the resulting Cu2O-Au nanocomposites have been characterized in detail by inductively coupled plasma atomic emission spectroscopy, powder X-ray diffraction, N2 adsorption-desorption isotherms, infrared spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy and transmission electron microscopy. Their visible-light-driven photocatalytic activity toward various dye molecules has also been investigated. Depending on the Au：Cu ratio, Cu20-Au nanocomposites exhibit different novel nanostructures including a beautiful flower-like nanostructure that consists of polycrystalline Cu2O, amorphous Cu2O and Au colloids. We propose that the rapidly-generated bubbles of H2 during the course of the catalytic decomposition reaction drive the simultaneously-formed Cu2O to form amorphous curved thin foils and might also act as a template to assemble curved thin foils of amorphous Cu2O, polycrystalline Cu2O and Au colloids into uniform nanostructures. A Cu2O-Au nanocomposite with a Cu：Au ratio of 40 exhibits remarkable chemisorption capacity and visible-light-driven photocatalytic activity towards methyl orange and acid orange 7 and is a promising chemisorption-photocatalysis integrated catalyst. The catalytic decomposition of the metal hydride might open up a new approach for the fabrication of other metal/metal oxide nanocomposites with novel nanostructures and properties.展开更多
文摘Designing low-cost and high-performance photoelectrodes with improved light harvesting and charge separation rates is significant in photoelectrochemical water splitting.Here,a novel TiO2/Cu2O/Al/Al2O3 photoelectrode is manufactured by depositing plasmonic nanoparticles of the non-noble metal Al on the surface of a TiO2/Cu2O core/shell heterojunction for the first time.The Al nanoparticles,which exhibit a surface plasmon resonance(SPR)effect and are substantially less expensive than noble metals such as Au and Ag,generate hot electron-hole pairs and amplify the electromagnetic field at the interface under illumination.The as-prepared TiO2/Cu2O/Al/Al2O3 photoelectrodes have an extended absorption range and enhanced carrier separation and transfer.Their photocurrent density of 4.52 mA·cm^-2 at 1.23 V vs.RHE represents an 1.84-fold improvement over that of TiO2/Cu2O.Specifically,the ultrathin Al2O3 passivation layer spontaneously generated on the surface of Al in air could act as a protective layer to significantly increase its stability.In this work,the synergistic effect of the heterojunctions and the SPR effect of the non-noble metal Al significantly improve the photoelectrode performance,providing a novel concept for the design of electrodes with good properties and high practicability.
基金This work was financially supported by the National Natural Science Foundation of China （grant No. 20773113）, the Solar Energy Project of the Chinese Academy of Sciences, the National Basic Research Program of China （No. 2010CB923302）, MOE program for PCSIRT （IRT0756）, the Fundamental Research Funds for the Central Universities （No. WK2060030005）, and the MPG-CAS partner group program.
文摘The decomposition of Cull nanoparticles in aqueous solution has been successfully developed as a novel method for the preparation of Cu2O nanoparticles. In particular, we found that the decomposition of Cull nanoparticles in aqueous solution could be catalyzed by Au colloids, forming CU2O-Au nanocomposites. The composition and structure of the resulting Cu2O-Au nanocomposites have been characterized in detail by inductively coupled plasma atomic emission spectroscopy, powder X-ray diffraction, N2 adsorption-desorption isotherms, infrared spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy and transmission electron microscopy. Their visible-light-driven photocatalytic activity toward various dye molecules has also been investigated. Depending on the Au：Cu ratio, Cu20-Au nanocomposites exhibit different novel nanostructures including a beautiful flower-like nanostructure that consists of polycrystalline Cu2O, amorphous Cu2O and Au colloids. We propose that the rapidly-generated bubbles of H2 during the course of the catalytic decomposition reaction drive the simultaneously-formed Cu2O to form amorphous curved thin foils and might also act as a template to assemble curved thin foils of amorphous Cu2O, polycrystalline Cu2O and Au colloids into uniform nanostructures. A Cu2O-Au nanocomposite with a Cu：Au ratio of 40 exhibits remarkable chemisorption capacity and visible-light-driven photocatalytic activity towards methyl orange and acid orange 7 and is a promising chemisorption-photocatalysis integrated catalyst. The catalytic decomposition of the metal hydride might open up a new approach for the fabrication of other metal/metal oxide nanocomposites with novel nanostructures and properties.
