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The role of phase impurities and lattice defects on the electron dynamics and photochemistry of CuFeO2 solar photocathodes

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Nano Research 2019年第9期12卷 2390-2399页

作者： Elizabeth A. Fugate Somnath Biswas Mathew C. Clement Minkyu Kim Dongjoon Kim aravind asthagiri L. Robert Baker Department of Chemistry and Biochemistry The Ohio State UniversityColumbusOH 43210USA Department of Chemical and Biomolecular Engineering The Ohio State UniversityColumbusOH 43210USA

CuFeO2 is a promising photocathode for H2 evolution and CO2 reduction *** better understand the complex defect chemistry and role of impurity phases in this material and their effect on the photochemical performance,we employ visible light transient absorption spectroscopy and density functional theory(DFT)calculations to investigate the electron dynamics in electrochemically deposited Cu-Fe oxide thin *** analysis of carrier lifetime shows a fast,sub-ps contribution to relaxation followed by persistence of a Iong-lived state to time delays greater than 2 *** amplitude of the Iong-lived state is shown to correlate with the rate of fast initial relaxation,and this is explained in terms of a competition between charge carrier trapping and charge *** separation in CuFeO2 occurs via hole thermalizati on from O 2p to Cu 3d vale nee band states leadi ng to segregatio n of electr ons and holes across layers in the CuFeO2 *** between transient absorption measurements and DFT calculations suggest that Cu vacancies enhanee photochemical performance by facilitating charge separation *** contrast,O interstitials are predicted to switch the relative positions of O 2p and Cu 3d vale nee band states,which would in hibit charge separatio n by in ter-band hole thermal izatio *** ally,we find no evide nee for electron in jecti on from CuFeO2 to CuO suggest!ng that charge separati on at this heterostructure in terface does not play a role in the carrier lifetime or photochemical performance of the catalysts studied here.

关键词： delafossite CuFeO2 charge-carrier dynamics transient absorption spectroscopy Cu vacancy O interstitial

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