Theoretical insights into interfacial and electronic structures of NiO_x/SrTiO_3 photocatalyst for overall water splitting
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摘要
SrTiO_3 is a promising candidate photocatalyst for overall water splitting.Loading suitable cocatalysts,such as NiO_x,the mixture of Ni and NiO,remarkably improve the photocatalytic activity.However,spatial locations and functions of components in NiO_x/SrTiO_3 are under debate.Here,using first-principles density functional theory(DFT)calculations,we investigate the initial growth of Ni_n(n=1–4)and(NiO)_n(n=1,2 and 4)clusters on stoichiometric(100)surfaces of SrTiO_3,and explore interfacial and electronic structures of composite photocatalysts.It is found that Ni_n clusters are easier to undergo aggregation on SrO-termination than on TiO_2-termination.The adsorption of Ni_ncluster on(100)surfaces elevates the Fermi level towards the conduction band,which may benefit the occurrence of hydrogen evolution reaction.The structural similarity between(NiO)_n cluster and surface has an essential effect on the most stable adsorption configuration.For(NiO)_n/SrTiO_3 systems,the occupied states of(NiO)_n cluster well overlap with those of(100)surfaces in the valence band maximum,which is in favor of the separation of photogenerated electrons and holes to SrTiO_3 support and(NiO)_n cluster,respectively.The detailed DFT analysis provides important insights into the growth of NiO_x on surfaces of SrTiO_3and presents an explanation on the different models of NiO_x/SrTiO_3 photocatalyst proposed by experimental groups.Our calculations build a basis for further investigations on the mechanism of photocatalytic water-splitting reaction in NiO_x/SrTiO_3composite system.
SrTiO_3 is a promising candidate photocatalyst for overall water splitting.Loading suitable cocatalysts,such as NiO_x,the mixture of Ni and NiO,remarkably improve the photocatalytic activity.However,spatial locations and functions of components in NiO_x/SrTiO_3 are under debate.Here,using first-principles density functional theory(DFT)calculations,we investigate the initial growth of Ni_n(n=1–4)and(NiO)_n(n=1,2 and 4)clusters on stoichiometric(100)surfaces of SrTiO_3,and explore interfacial and electronic structures of composite photocatalysts.It is found that Ni_n clusters are easier to undergo aggregation on SrO-termination than on TiO_2-termination.The adsorption of Ni_ncluster on(100)surfaces elevates the Fermi level towards the conduction band,which may benefit the occurrence of hydrogen evolution reaction.The structural similarity between(NiO)_n cluster and surface has an essential effect on the most stable adsorption configuration.For(NiO)_n/SrTiO_3 systems,the occupied states of(NiO)_n cluster well overlap with those of(100)surfaces in the valence band maximum,which is in favor of the separation of photogenerated electrons and holes to SrTiO_3 support and(NiO)_n cluster,respectively.The detailed DFT analysis provides important insights into the growth of NiO_x on surfaces of SrTiO_3and presents an explanation on the different models of NiO_x/SrTiO_3 photocatalyst proposed by experimental groups.Our calculations build a basis for further investigations on the mechanism of photocatalytic water-splitting reaction in NiO_x/SrTiO_3composite system.
SrTiO_3 is a promising candidate photocatalyst for overall water splitting.Loading suitable cocatalysts,such as NiO_x,the mixture of Ni and NiO,remarkably improve the photocatalytic activity.However,spatial locations and functions of components in NiO_x/SrTiO_3 are under debate.Here,using first-principles density functional theory(DFT)calculations,we investigate the initial growth of Ni_n(n=1–4)and(NiO)_n(n=1,2 and 4)clusters on stoichiometric(100)surfaces of SrTiO_3,and explore interfacial and electronic structures of composite photocatalysts.It is found that Ni_n clusters are easier to undergo aggregation on SrO-termination than on TiO_2-termination.The adsorption of Ni_ncluster on(100)surfaces elevates the Fermi level towards the conduction band,which may benefit the occurrence of hydrogen evolution reaction.The structural similarity between(NiO)_n cluster and surface has an essential effect on the most stable adsorption configuration.For(NiO)_n/SrTiO_3 systems,the occupied states of(NiO)_n cluster well overlap with those of(100)surfaces in the valence band maximum,which is in favor of the separation of photogenerated electrons and holes to SrTiO_3 support and(NiO)_n cluster,respectively.The detailed DFT analysis provides important insights into the growth of NiO_x on surfaces of SrTiO_3and presents an explanation on the different models of NiO_x/SrTiO_3 photocatalyst proposed by experimental groups.Our calculations build a basis for further investigations on the mechanism of photocatalytic water-splitting reaction in NiO_x/SrTiO_3composite system.
引文
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