Splitting water into hydrogen and oxygen by dye-sensitized photoelectrochemical cell(DSPEC)is a promising approach to solar fuels production.In this study,a series of pyridine derivatives as surface additives were mod...Splitting water into hydrogen and oxygen by dye-sensitized photoelectrochemical cell(DSPEC)is a promising approach to solar fuels production.In this study,a series of pyridine derivatives as surface additives were modified on a molecular chromophore and water oxidation catalyst co-loaded TiO_(2)photoanode,TiO_(2)|RuP,1(RuP=Ru(4,4′-(PO3H2)2-2,2′-bipyridine)(2,2′-bipyridine)2,1=Ru(bda)(L)2,(bda=2,2′-bipyridine-6,6′-dicarboxylate,L=10-(pyridin-4-yloxy)decyl)phosphonic acid).The addition of pyridine additives was found to result in up to 42%increase in photocurrent.Under simulated sun-light irradiation,TiO_(2)|RuP,1,P1(P1=4-Hydroxypyridine)produced a photocurrent density of 1 mA/cm2 at a bias of 0.4 V vs.NHE in acetate buffer.Moreover,the observed photocurrents are correlated with the electron-donating ability of the substituent groups on pyridine ring.Transient absorption measurements and electrochemical impedance spectroscopy revealed that surface-bound pyridine can effectively retard the back-electron transfer from the TiO_(2)conduction band to the oxidized dye,which is a major process responsible for energy loss in DSPECs.展开更多
Two-dimensional(2D)metal oxides and chalcogenides(MOs&MCs)have been regarded as a new class of promising electro-and photocatalysts for many important chemical reactions such as hydrogen evolution reaction,CO_(2) ...Two-dimensional(2D)metal oxides and chalcogenides(MOs&MCs)have been regarded as a new class of promising electro-and photocatalysts for many important chemical reactions such as hydrogen evolution reaction,CO_(2) reduction reaction and N2 reduction reaction in virtue of their outstanding physicochemical properties.However,pristine 2D MOs&MCs generally show the relatively poor catalytic performances due to the low electrical conductivity,few active sites and fast charge recombination.Therefore,considerable efforts have been devoted to engineering 2D MOs&MCs by rational structural design and chemical modification to further improve the catalytic activities.Herein,we comprehensively review the recent advances for engineering technologies of 2D MOs&MCs,which are mainly focused on the intercalation,doping,defects creation,facet design and compositing with functional materials.Meanwhile,the relationship between morphological,physicochemical,electronic,and optical properties of 2D MOs&MCs and their electro-and photocatalytic performances is also systematically discussed.Finally,we further give the prospect and challenge of the field and possible future research directions,aiming to inspire more research for achieving high-performance 2D MOs&MCs catalysts in energy storage and conversion fields.展开更多
文摘Splitting water into hydrogen and oxygen by dye-sensitized photoelectrochemical cell(DSPEC)is a promising approach to solar fuels production.In this study,a series of pyridine derivatives as surface additives were modified on a molecular chromophore and water oxidation catalyst co-loaded TiO_(2)photoanode,TiO_(2)|RuP,1(RuP=Ru(4,4′-(PO3H2)2-2,2′-bipyridine)(2,2′-bipyridine)2,1=Ru(bda)(L)2,(bda=2,2′-bipyridine-6,6′-dicarboxylate,L=10-(pyridin-4-yloxy)decyl)phosphonic acid).The addition of pyridine additives was found to result in up to 42%increase in photocurrent.Under simulated sun-light irradiation,TiO_(2)|RuP,1,P1(P1=4-Hydroxypyridine)produced a photocurrent density of 1 mA/cm2 at a bias of 0.4 V vs.NHE in acetate buffer.Moreover,the observed photocurrents are correlated with the electron-donating ability of the substituent groups on pyridine ring.Transient absorption measurements and electrochemical impedance spectroscopy revealed that surface-bound pyridine can effectively retard the back-electron transfer from the TiO_(2)conduction band to the oxidized dye,which is a major process responsible for energy loss in DSPECs.
基金Australian Research Council(ARC)for funding received under the ARC Discovery Project scheme(DP180102752)the financial support via the ARC DECRA scheme(DE160100715)+1 种基金the support from the Shuguang Program supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission(18SG035)State Key Laboratory for Modification of Chemical Fibers and Polymer Materials,Donghua University(KF2015)。
文摘Two-dimensional(2D)metal oxides and chalcogenides(MOs&MCs)have been regarded as a new class of promising electro-and photocatalysts for many important chemical reactions such as hydrogen evolution reaction,CO_(2) reduction reaction and N2 reduction reaction in virtue of their outstanding physicochemical properties.However,pristine 2D MOs&MCs generally show the relatively poor catalytic performances due to the low electrical conductivity,few active sites and fast charge recombination.Therefore,considerable efforts have been devoted to engineering 2D MOs&MCs by rational structural design and chemical modification to further improve the catalytic activities.Herein,we comprehensively review the recent advances for engineering technologies of 2D MOs&MCs,which are mainly focused on the intercalation,doping,defects creation,facet design and compositing with functional materials.Meanwhile,the relationship between morphological,physicochemical,electronic,and optical properties of 2D MOs&MCs and their electro-and photocatalytic performances is also systematically discussed.Finally,we further give the prospect and challenge of the field and possible future research directions,aiming to inspire more research for achieving high-performance 2D MOs&MCs catalysts in energy storage and conversion fields.
