We first report that photoelectrochemical （PEC） performance of electrochemically hydrogenated TiO2 nanotube arrays （TNTAs） as high-efficiency photoanodes for solar water splitting could be well tuned by designing ...We first report that photoelectrochemical （PEC） performance of electrochemically hydrogenated TiO2 nanotube arrays （TNTAs） as high-efficiency photoanodes for solar water splitting could be well tuned by designing and adjusting the phase structure and composition of TNTAs. Among various TNTAs annealed at different temperature ranging from 300 to 700℃, well-crystallized single anatase （A） phase TNTAs-400 photoanode shows the best photoresponse properties and PEC performance due to the favor- able crystallinity, grain size and tubular structures. After electrochemical hydrogenation （EH）. anatase- rutile （A-R） mixed phase EH-TNTAs-600 photoanode exhibits the highest photoactivity and PEC perfor- mance for solar water splitting. Under simulated solar illumination, EH-TNTAs-600 achieves the best photoconversion efficiency of up to 1.52% and maximum H2 generation rate of 40.4 ~mol h i cm-2, our- stripping other EH-TNTAs photoanodes. Systematic studies reveal that the signigicantly enhanced PEC performance for A-R mixed phaes EH-TNTAs-600 photoanode could be attributed to the synergy of A-R mixed phases and intentionally introduced Ti3~ （oxygen vacancies） which enhances the photoactivity over both UV and visible-light regions, and boosts both charge separation and transfer efficiencies. These findings provide new insight and guidelines for the construction of highly efficient TiO2-based devices for the application of solar water splitting.展开更多
基金supported by the National Natural Science Foundation of China(51402078,21702041,and 11674354)the National Basic Research Program of China(2014CB660815)the Fundamental Research Funds for the Central Universities(JZ2016HGTB0711,JZ2016HGTB0719,and JZ2017HGPA0167)
文摘We first report that photoelectrochemical （PEC） performance of electrochemically hydrogenated TiO2 nanotube arrays （TNTAs） as high-efficiency photoanodes for solar water splitting could be well tuned by designing and adjusting the phase structure and composition of TNTAs. Among various TNTAs annealed at different temperature ranging from 300 to 700℃, well-crystallized single anatase （A） phase TNTAs-400 photoanode shows the best photoresponse properties and PEC performance due to the favor- able crystallinity, grain size and tubular structures. After electrochemical hydrogenation （EH）. anatase- rutile （A-R） mixed phase EH-TNTAs-600 photoanode exhibits the highest photoactivity and PEC perfor- mance for solar water splitting. Under simulated solar illumination, EH-TNTAs-600 achieves the best photoconversion efficiency of up to 1.52% and maximum H2 generation rate of 40.4 ~mol h i cm-2, our- stripping other EH-TNTAs photoanodes. Systematic studies reveal that the signigicantly enhanced PEC performance for A-R mixed phaes EH-TNTAs-600 photoanode could be attributed to the synergy of A-R mixed phases and intentionally introduced Ti3~ （oxygen vacancies） which enhances the photoactivity over both UV and visible-light regions, and boosts both charge separation and transfer efficiencies. These findings provide new insight and guidelines for the construction of highly efficient TiO2-based devices for the application of solar water splitting.
