In this work, two new dyes YK-1 and YK-2 with carboxylic acid and hydroxamic acid as anchoring groups,respectively, in combination with diphenylamine as donor and perylenemonoimide as acceptor were synthesized and app...In this work, two new dyes YK-1 and YK-2 with carboxylic acid and hydroxamic acid as anchoring groups,respectively, in combination with diphenylamine as donor and perylenemonoimide as acceptor were synthesized and applied in p-type dye-sensitized solar cells（p-DSCs） and dye-sensitized photoelectrochemical cells（PEC）. The results showed that the sensitizer（YK-1） based on carboxylic acid displayed a higher conversion efficiency of 0.064% under AM 1.5 solar conditions in p-DSCs. However, it was interesting that the hydroxamic acid based sensitizer（YK-2） on Ni O photocathode displayed better performance in a hydrophilic environment over a broad p H range under visible-light irradiation because of a versatile covalent attachment to Ni O surfaces. This may be ascribed to hydroxamic acid anchors, which have more sites interacting with the surface of Ni O in aqueous solution. This study demonstrates that YK-2 containing hydroxamic acid anchoring group is a promising candidate to achieve highly efficient and stable activity for dye-sensitized PEC system.展开更多
Dye-sensitized photoelectrochemical tandem cells have shown the promise for light driven hydrogen production from water owing to the low cost,wide absorption spectra in the visible region and ease to process of their ...Dye-sensitized photoelectrochemical tandem cells have shown the promise for light driven hydrogen production from water owing to the low cost,wide absorption spectra in the visible region and ease to process of their constitutive photoelectrode materials.However,most photo-driven water splitting photoelectrochemical cells driven by organic dye sensitized solar cells exhibit unsatisfactory hydrogen evolution rate,primarily attributed to their poor light capturing ability and low photocurrent performance.Here we present the construction of a tandem system consisting of an organic blue-colored S5 sensitizer-based dyesensitized photoelectrochemical cell(DSPEC) wired in series with three spectral-complemental dyes BTA-2,APP-3 and APP-1 sensitizers-based dye-sensitized solar cell(DSC),respectively.The two spectral-complemental chromophores were used in DSC and DSPEC to ensure that the full solar spectrum could be absorbed as much as possible.The results showed that the photocurrent of tandem device was closely related to the open-circuit voltage(Voc) of sensitized DSC,in which the tandem configuration consisting of S5 based DSPEC and BTA-2 based DSC gave the best photocurrent.On this basis,tandem device with the only light energy and no external applied electrical bias was further constructed of BTA-2 based 2-junction DSC and S5 based DSPEC and obtained a photocurrent of 500 μA cm-2 for hydrogen generation.Furthermore,I-/I3-was used as a redox couple between dye regeneration and O2 production on the surface of Pt-IrO2/WO3.The strategy opens up the application of pure organic dyes in DSC/DSPEC tandem device.展开更多
It is a challenge to develop single polymer-based photocatalyst for overall water splitting without adding sacrificial agents due to the insufficient driving force for charge separation and the lack of active sites of...It is a challenge to develop single polymer-based photocatalyst for overall water splitting without adding sacrificial agents due to the insufficient driving force for charge separation and the lack of active sites of organic polymer.Metal oxyhyroxides are widely acted as co-catalyst for photoelectrocatalysis oxygen evolution reaction.Here,we firstly report the peryleno[1,12-bcd]thiophene sulfone-based linear co-polymer PS-5 for photocatalytic overall water splitting by photo-depositing simple and low-cost cocatalyst FeOOH under the visible-light illumination.The density functional theory(DFT)calculations and experimental results indicated clearly that the oxygen vacancies-richβ-FeOOH can effectively promote the separation of photo-generated excitons and provide active sites for photocatalytic oxygen evolution reaction.As a result,the average H_(2)and O_(2)production rates of optimized PS-5/β-FeOOH-0.2M reach at~170 and~76.6μmol h^(-1)g^(-1),respectively,with a stoichiometric ratio at about 2:1.This work provides a simple and low-cost method for the preparation of overall water splitting system based on polymer photocatalyst.展开更多
基金supported by the National Natural Science Foundation of China (21372082, 21421004, 21772040 and 21572062)the Fundamental Research Funds for the Central Universities (222201717003)the Programme of Introducing Talents of Discipline to Universities (B16017)
文摘In this work, two new dyes YK-1 and YK-2 with carboxylic acid and hydroxamic acid as anchoring groups,respectively, in combination with diphenylamine as donor and perylenemonoimide as acceptor were synthesized and applied in p-type dye-sensitized solar cells（p-DSCs） and dye-sensitized photoelectrochemical cells（PEC）. The results showed that the sensitizer（YK-1） based on carboxylic acid displayed a higher conversion efficiency of 0.064% under AM 1.5 solar conditions in p-DSCs. However, it was interesting that the hydroxamic acid based sensitizer（YK-2） on Ni O photocathode displayed better performance in a hydrophilic environment over a broad p H range under visible-light irradiation because of a versatile covalent attachment to Ni O surfaces. This may be ascribed to hydroxamic acid anchors, which have more sites interacting with the surface of Ni O in aqueous solution. This study demonstrates that YK-2 containing hydroxamic acid anchoring group is a promising candidate to achieve highly efficient and stable activity for dye-sensitized PEC system.
基金supported by the National Natural Science Foundation of China(21971064,21421004,21772040,21572062)Shanghai Municipal Science and Technology Major Project(2018SHZDZX03)+1 种基金the Fundamental Research Funds for the Central Universities(50321101918001,222201717003)the Programme of Introducing Talents of Discipline to Universities(B16017)
文摘Dye-sensitized photoelectrochemical tandem cells have shown the promise for light driven hydrogen production from water owing to the low cost,wide absorption spectra in the visible region and ease to process of their constitutive photoelectrode materials.However,most photo-driven water splitting photoelectrochemical cells driven by organic dye sensitized solar cells exhibit unsatisfactory hydrogen evolution rate,primarily attributed to their poor light capturing ability and low photocurrent performance.Here we present the construction of a tandem system consisting of an organic blue-colored S5 sensitizer-based dyesensitized photoelectrochemical cell(DSPEC) wired in series with three spectral-complemental dyes BTA-2,APP-3 and APP-1 sensitizers-based dye-sensitized solar cell(DSC),respectively.The two spectral-complemental chromophores were used in DSC and DSPEC to ensure that the full solar spectrum could be absorbed as much as possible.The results showed that the photocurrent of tandem device was closely related to the open-circuit voltage(Voc) of sensitized DSC,in which the tandem configuration consisting of S5 based DSPEC and BTA-2 based DSC gave the best photocurrent.On this basis,tandem device with the only light energy and no external applied electrical bias was further constructed of BTA-2 based 2-junction DSC and S5 based DSPEC and obtained a photocurrent of 500 μA cm-2 for hydrogen generation.Furthermore,I-/I3-was used as a redox couple between dye regeneration and O2 production on the surface of Pt-IrO2/WO3.The strategy opens up the application of pure organic dyes in DSC/DSPEC tandem device.
基金supported by the National Natural Science Foundation of China(21788102,21971064,21772040)Shanghai Municipal Science and Technology Major Project(2018SHZDZX03)+1 种基金the Fundamental Research Funds for the Central Universities(222201717003,50321101918001)the Programme of Introducing Talents of Discipline to Universities(B16017)。
文摘It is a challenge to develop single polymer-based photocatalyst for overall water splitting without adding sacrificial agents due to the insufficient driving force for charge separation and the lack of active sites of organic polymer.Metal oxyhyroxides are widely acted as co-catalyst for photoelectrocatalysis oxygen evolution reaction.Here,we firstly report the peryleno[1,12-bcd]thiophene sulfone-based linear co-polymer PS-5 for photocatalytic overall water splitting by photo-depositing simple and low-cost cocatalyst FeOOH under the visible-light illumination.The density functional theory(DFT)calculations and experimental results indicated clearly that the oxygen vacancies-richβ-FeOOH can effectively promote the separation of photo-generated excitons and provide active sites for photocatalytic oxygen evolution reaction.As a result,the average H_(2)and O_(2)production rates of optimized PS-5/β-FeOOH-0.2M reach at~170 and~76.6μmol h^(-1)g^(-1),respectively,with a stoichiometric ratio at about 2:1.This work provides a simple and low-cost method for the preparation of overall water splitting system based on polymer photocatalyst.
