Journal
ADVANCED MATERIALS
Volume 31, Issue 19, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201900961
Keywords
conjugated polymers; Glaser polycondensation; gradient homojunctions; hydrogen evolution; photocathodes
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Funding
- EC under the Graphene Flagship [CNECTICT-604391]
- National Natural Science Foundation of China [21720102002]
- DFG [TRR234, INST 275/257-1 FUGG, FGR92]
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As appealing photoelectrode materials for photoeletrochemical hydrogen evolution reaction (PEC HER), conjugated polymers still show poor PEC HER performance as a result of their serious recombination of photogenerated electrons and holes. Herein, a novel design of gradient homojunction is demonstrated by controlled copolymerization of 1,4-diethynylbenzene (DEB) and 1,3,5-triethynylbenzene (TEB). The as-built gradient distribution of TEB monomer in poly(1,4-diethynylbenzene) (pDEB) leads to continuous band bending engineering, which constitutes a gradient homojunction. Under AM 1.5G irradiation and in 0.1 M Na2SO4 aqueous solution, the as-fabricated pDEB gradient homojunction exhibits a charge separation efficiency of 0.27% at 0.3 V versus reversible hydrogen electrode (RHE), which is 3.4 and 1.7 times higher than those for pure pDEB and the traditionally designed pDEB homojunction. As a result, the photocurrent of the pDEB gradient homojunction unprecedentedly reaches 55 mu A cm(-2) at 0.3 V versus RHE, which is much higher than 19 mu A cm(-2) for pure pDEB, 32 mu A cm(-2) for the pDEB homojunction, and state-of-the-art organic photocathodes, e.g., g-C3N4 (approximate to 1-32 mu A cm(-2)). This work opens up a new window for the design of gradient homojunctions and will advance the exploration of high-performance organic photoelectrodes.
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