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Vertically aligned Ni/Nio nanocomposites with abundant oxygen deficient hetero-interfaces for enhanced overall water splitting

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Science China Chemistry 2022年第10期65卷 1885-1894页

作者： Hongxia Wang Meiyan Cui Gaoliang Fu Jiaye Zhang Xingyu Ding Irene Azaceta Matthew Bugnet Demie M.Kepaptsoglou Vlado K.lazarov victor ade la peña 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 State Key laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Henan Provincial Key laboratory of Nanocomposites and Applications Institute of Nanostructured Functional MaterialsHuanghe Science and Technology CollegeZhengzhou 450006China Department of Physics University of YorkHeslingtonYorkYO105DDUK SuperSTEM laboratory SciTech Daresbury CampusDaresbury WA44ADUK School of Chemical and Process Engineering Univeristy of LeedsLeeds LS29JTUK Univ Lyon CNRSINSA LyonUCBLMATEISUMR 551069621 VilleurbanneFrance Photoactivated Processes Unit IMDEA Energy InstituteParque Tecnológico de MóstolesAvda.Ramón de la Sagra 328935 MóstolesMadridSpain

The design of heterostructured transition metal-based electrocatalysts with controlled composition and interfaces is key to increasing the efficiency of the water electrolysis and the elucidation of reaction *** this work,we report the synthesis of well-controlled vertically aligned Ni/Nio nanocomposites consisting of Ni nanoclusters embedded in Nio,which result in highly efficient electrocatalysts for overall water *** show that such a high catalytic efficiency toward both the hydrogen evolution reaction(HER)and the oxygen evolution reaction(oER)originates from a synergetic effect at Ni/Nio interfaces that significantly reduces the energy barrier for water dissociation,and favours the formation of reactive H*intermediates on the Ni side of the interface,and oH_(ads) on the Nio side of the interface.A study of water chemisorption based on near-ambient pressure photoelectron spectroscopy indicates that the abundant hetero-interfaces in Ni/Nio nanocomposite promote the dissociation of water with a three-fold increase in the surface concentration of oH_(ads) compared with pure *** functional theory calculations indicate that Ni/Nio interface leads to the reduction of the water dissociation energy barrier due to a high concentration of oxygen vacancies at Nio side of the interface,whereas the formation of highly active metallic Ni sites with an optimal value of Gibbs free energy of H*(ΔG_(H*)=−0.16 eV)owes to a favourable adjustment of the electron energetics at the interface,thus accelerating the overall electrochemical water splitting.

关键词： water splitting hydrogen evolution reaction electronic structure heterostructure vertically aligned nanocomposites

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

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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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Highly efficient multi-metal catalysts for carbon dioxide reduction prepared from atomically sequenced metal organic frameworks

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Nano Research 2021年第2期14卷 493-500页

作者： Celia Castillo-Blas Consuelo Alvarez-Galvan Ines Puente-orench Alba Garcia-Sanchez Freddy E.oropeza Enrique Gutirrez-Puebla Angeles Monge victor A.de la pena-o'hea Felipe Gandara Materials Science Institute of Madrid(CSIC) C/Sor Juana Ines de la Cruz 3Madrid 28049Spain Instituto de Catalisis y petroleoquimica(CSIC) dM arie Curie 2Madrid 28049Spain Instituto de Ciencia de Materiales de Aragon Pedro Cerbuna 12Zaragoza 50009Spain Institut laue langevin 71 Avenue des Martyrs38042 GrenobleFrance Photoactivated Processes Unit IMDEA Energy Institute Mostoles Technology ParkAvenida Ramdn de la Sagra 3MostolesMadrid 28935Spain Department of Inorganic Chemistry University Autonomous of MadridC/Frandsco Tomdsy Valiente 7Madrid 28049Spain

The precise control on the combination of multiple metal atoms in the structure of metal-organic frameworks(MoFs)endowed by reticular chemistry,allows the obtaining of materials with compositions that are programmed for achieving enhanced *** present work illustrates how through the transformation of MoFs with desired arrangements of metal cations,multi-metal spinel oxides with precise compositions can be obtained,and used as catalyst precursor for the reverse water-gas shift *** differences in the spinel initial composition and structure,determined by neutron powder diffraction,influence the overall catalytic activity with changes in the process of in s itu formation of active,metal-oxide supported metal nanoparticles,which have been monitored and characterized with in situ X-ray diffraction and photoelectron spectroscopy studies.

关键词： reticular chemistry multi-metal metal-organic frameworks(MoFs) carbon dioxide reduction heterogeneous catalysis reverse water-gas shift in-situ X-ray photoelectron spectroscopy(XPS)

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