Phase engineering can overcome the weaknesses of catalysts by tuning the electronic structures and catalytic functions.In this study,we investigate the role of phase-engineered NiSx,specifically hexagonal,trigonal and...Phase engineering can overcome the weaknesses of catalysts by tuning the electronic structures and catalytic functions.In this study,we investigate the role of phase-engineered NiSx,specifically hexagonal,trigonal and cubic phases,as a cocatalyst decorated onto the semiconductor surface.We demonstrate that NiSx with different phases(i.e.h-NiS,t-NiS and c-NiS_(2))can greatly improve the photocatalytic hydrogen evolution rate of various classical semiconductors including TiO_(2),CdS and carbon nitride(CN).In particular,it is observed that c-NiS_(2) can promote the H2 evolution performance with the highest improvement factor compared with h-NiS and t-NiS regardless of the type of hosting semiconductor.The highly efficient sacrificial hydrogen evolution performance rates are achieved on c-NiS_(2)/CN(4078μmol h^(−1) g^(−1)),c-NiS_(2)/TiO_(2)(345μmol h^(−1) g^(−1))and c-NiS_(2)/CdS(14604μmol h^(−1) g^(−1))under light irradiation(λ>320 nm).As revealed by detailed characterizations and theoretical computations,the significant higher performance of c-NiS_(2) is because c-NiS_(2) possesses more appropriate hydrogen adsorption Gibbs free energy and better ability in facilitating charge migration compared to h-NiS and t-NiS.Our findings highlight the great potential of phase engineering as a general strategy for improving the catalytic performance of different catalysts.展开更多
基金support from Natural Science Foundation of Jiangsu Province(BK20210827)China Postdoctoral Science Foundation(2021M700117)National Natural Science Foundation of China(22178152,U1904215).
文摘Phase engineering can overcome the weaknesses of catalysts by tuning the electronic structures and catalytic functions.In this study,we investigate the role of phase-engineered NiSx,specifically hexagonal,trigonal and cubic phases,as a cocatalyst decorated onto the semiconductor surface.We demonstrate that NiSx with different phases(i.e.h-NiS,t-NiS and c-NiS_(2))can greatly improve the photocatalytic hydrogen evolution rate of various classical semiconductors including TiO_(2),CdS and carbon nitride(CN).In particular,it is observed that c-NiS_(2) can promote the H2 evolution performance with the highest improvement factor compared with h-NiS and t-NiS regardless of the type of hosting semiconductor.The highly efficient sacrificial hydrogen evolution performance rates are achieved on c-NiS_(2)/CN(4078μmol h^(−1) g^(−1)),c-NiS_(2)/TiO_(2)(345μmol h^(−1) g^(−1))and c-NiS_(2)/CdS(14604μmol h^(−1) g^(−1))under light irradiation(λ>320 nm).As revealed by detailed characterizations and theoretical computations,the significant higher performance of c-NiS_(2) is because c-NiS_(2) possesses more appropriate hydrogen adsorption Gibbs free energy and better ability in facilitating charge migration compared to h-NiS and t-NiS.Our findings highlight the great potential of phase engineering as a general strategy for improving the catalytic performance of different catalysts.
