Dataset Information

A Facile Design for Water-Oxidation Molecular Catalysts Precise Assembling on Photoanodes.

ABSTRACT: Regulating the interfacial charge transfer behavior between cocatalysts and semiconductors remains a critical challenge for attaining efficient photoelectrochemical water oxidation reactions. Herein, using bismuth vanadate (BiVO₄ ) photoanode as a model, it introduces an Au binding bridge as holes transfer channels onto the surfaces of BiVO₄ , and the cyano-functionalized cobalt cubane (Co₄ O₄ ) molecules are preferentially immobilized on the Au bridge due to the strong adsorption of cyano groups with Au nanoparticles. This orchestrated arrangement facilitates the seamless transfer of photogenerated holes from BiVO₄ to Co₄ O₄ molecules, forming an orderly charge transfer pathway connecting the light-absorbing layer to reactive sites. An exciting photocurrent density of 5.06 mA cm^-2 at 1.23 V versus the reversible hydrogen electrode (3.4 times that of BiVO₄ ) is obtained by the Co₄ O₄ @Au(A)/BiVO₄ photoanode, where the surface charge recombination is almost completely suppressed accompanied by a surface charge transfer efficiency over 95%. This work represents a promising strategy for accelerating interfacial charge transfer and achieving efficient photoelectrochemical water oxidation reaction.

SUBMITTER: Jiang W

PROVIDER: S-EPMC10787085 | biostudies-literature | 2024 Jan

REPOSITORIES: biostudies-literature

ACCESS DATA

Publications

A Facile Design for Water-Oxidation Molecular Catalysts Precise Assembling on Photoanodes.

Jiang Wenchao W Li Siyuan S Sui Qi Q Gao Yujie Y Li Fei F Xia Lixin L Jiang Yi Y

Advanced science (Weinheim, Baden-Wurttemberg, Germany) 20231120 2

Regulating the interfacial charge transfer behavior between cocatalysts and semiconductors remains a critical challenge for attaining efficient photoelectrochemical water oxidation reactions. Herein, using bismuth vanadate (BiVO4 ) photoanode as a model, it introduces an Au binding bridge as holes transfer channels onto the surfaces of BiVO4 , and the cyano-functionalized cobalt cubane (Co4 O4 ) molecules are preferentially immobilized on the Au bridge ...[more]

PMID: 37984864

Similar Datasets

Project description:Visible light driven water oxidation has been demonstrated at near-neutral pH using photoanodes based on nanoporous films of TiO2, polyoxometalate (POM) water oxidation catalyst [{Ru4O4(OH)2(H2O)4}(γ-SiW10O36)2]10- (1), and both known photosensitizer [Ru(bpy)2(H4dpbpy)]2+ (P2) and the novel crown ether functionalized dye [Ru(5-crownphen)2(H2dpbpy)](H22). Both triads, containing catalyst 1, and catalyst-free dyads, produce O2 with high faradaic efficiencies (80 to 94%), but presence of catalyst enhances quantum yield by up to 190% (maximum 0.39%). New sensitizer H22 absorbs light more strongly than P2, and increases O2 quantum yields by up to 270%. TiO2-2 based photoelectrodes are also more stable to desorption of active species than TiO2-P2: losses of catalyst 1 are halved when pH > TiO2 point-of-zero charge (pzc), and losses of sensitizer reduced below the pzc (no catalyst is lost when pH < pzc). For the triads, quantum yields of O2 are higher at pH 5.8 than at pH 7.2, opposing the trend observed for 1 under homogeneous conditions. This is ascribed to lower stability of the dye oxidized states at higher pH, and less efficient electron transfer to TiO2, and is also consistent with the 4th1-to-dye electron transfer limiting performance rather than catalyst TOFmax. Transient absorption reveals that TiO2-2-1 has similar 1st electron transfer dynamics to TiO2-P2-1, with rapid (ps timescale) formation of long-lived TiO2(e-)-2-1(h+) charge separated states, and demonstrates that metallation of the crown ether groups (Na+/Mg2+) has little or no effect on electron transfer from 1 to 2. The most widely relevant findings of this study are therefore: (i) increased dye extinction coefficients and binding stability significantly improve performance in dye-sensitized water splitting systems; (ii) binding of POMs to electrode surfaces can be stabilized through use of recognition groups; (iii) the optimal homogeneous and TiO2-bound operating pHs of a catalyst may not be the same; and (iv) dye-sensitized TiO2 can oxidize water without a catalyst.

Dataset Information

A Facile Design for Water-Oxidation Molecular Catalysts Precise Assembling on Photoanodes.

Publications

A Facile Design for Water-Oxidation Molecular Catalysts Precise Assembling on Photoanodes.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets