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Inductive effect of Ti-doping in Fe_(2)o_(3)enhances the photoelectrochemical water oxidation

Science China Chemistry 2023年第7期66卷 2091-2097页

作者： Yumei Lin Yan Wang Hongxia Wang Jingjing Wang Xiaofeng Wu jan.P.Hofmann Giulio Gorni Victor A.de la Pena o'shea Freddy E.oropeza Kelvin H.L.Zhang State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Surface Science Laboratory Department of Materials and Earth SciencesTechnical University of DarmstadtDarmstadt 64287Germany CELLS-ALBA Synchrotron Barcelona 08290Spain Institute of optics(Io-CSIC) c/Serrano 121Madrid 28006Spain Photoactivated Processes Unit IMDEA Energy InstituteMadrid 28935Spain

Hematite(α-Fe_(2)o_(3))is an ideal oxide semiconductor candidate for photoelectrochemical(PEC)water *** of Fe_(2)o_(3)is known to benefit the PEC water oxidation efficiency,but despite extensive research efforts,the underlying mechanism still remains *** this work,we report a comprehensive study on the relationship between the electronic structure,interfacial reaction kinetics and PEC activity of Ti-doped Fe_(2)o_(3)*** results show that the interfacial charge transfer efficiency at the Fe_(2)o_(3)/electrolyte interface is the main factor in the significant increase of the PEC activity of doped Fe_(2)o_(3).Electrochemical impedance spectroscopy reveals that the interfacial charge transfer efficiency is determined by energy overlap between the water oxidation potential and energy distribution of an intermediate surface state that has been identified as Fe^(IV)=o groups on Fe_(2)o_(3)surface generated during PEC ***,the potential energy distribution of this intermediate surface state can be modulated by Ti doping,and a shift towards a more positive potential of the intermediate surface state increases the overlap with the water oxidation potential and thus enhances the kinetics of charge transfer for PEC water *** origin of such potential energy modulation is traced to the inductive effect from Ti-doping on the Fe^(3+)/Fe^(4+)redox transition and the Fe-o bond *** results provide new insight into the mechanism for the doping effect on the PEC water splitting,introducing new strategies to optimize the PEC activity by tuning the redox properties of active metal oxides.

关键词： hematite surface states doping photoelectrochemical water splitting electronic structure

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Correlating the electronic structure of perovskite La_(1-x)SrxCoo_(3) with activity for the oxygen evolution reaction:The critical role of Co 3d hole state

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Journal of Energy Chemistry 2022年第2期31卷 637-645页

作者： Zechao Shen Mei Qu Jueli Shi Freddy E.oropeza Victor A.de la Peña o’shea Giulio Gorni C.M.Tian jan.P.Hofmann Jun Cheng Jun Li Kelvin H.L.Zhang State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina Photoactivated Processes Unit IMDEA Energy InstituteParque Tecnológico de MóstolesAvda.Ramón de la Sagra 328935 MóstolesMadridSpain CELLS-ALBA Synchrotron Carrer de la Llum 2-2608290 Cerdanyola del VallèsSpain Surface Science Laboratory Department of Materials and Earth SciencesTechnical University of Darmstadt Otto-Berndt-Strasse 364287 DarmstadtGermany

Perovskite LaCoo_(3) is being increasingly explored as an effective low-cost electrocatalyst for the oxygen evolution reaction(oER).Sr doping in LaCoo_(3)(La1-xSrxCoo_(3))has been found to substantially increase its catalytic *** this work,we report a detailed study on the evolution of the electronic structure of La1-xSrxCoo_(3) with 0≤x≤1 and its correlation with electrocatalytic activity for the oER.A combination of X-ray photoemission spectroscopy(XPS)and X-ray absorption spectroscopy(XAS)was used to unravel the electronic density of states(DoS)near the Fermi level(EF),which provide insights into the key electronic structure features for the enhanced oER catalytic *** analysis on the Co L-edge XAS suggest that LaCoo_(3) has a low spin state with t_(2g)^(6) e_(g)^(0) configuration at room *** implies that the high oER catalytic activity of LaCoo_(3) should not be rationalized by the occupancy of eg=1 *** Sr^(2+) for La^(3+) in LaCoo_(3) induces Co4+oxidation states and effectively dopes hole states into the top of valence band.A semiconductor-to-metal transition is observed for x>0.2,due to the holeinduced electronic DoS at the EF and increased hybridization between Co 3 d and o 2 *** an electronic modulation enhances the surface adsorption of the*oH intermediate and reduces the energy barrier for interfacial charge transfer,thus improving the oER catalytic activity in La_(1-x)Sr_(x)Coo_(3).In addition,we found that the La_(1-x)Sr_(x)Coo_(3) surface undergoes amorphization after certain period of oER measurement,leading to a partial deactivation of the *** Sr doping levels accelerated the amorphization process.

关键词： Perovskite oxide oxygen evolution Cobalt Electronic structure

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