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DOI10.1039/d1ee00152c
A hybrid bulk-heterojunction photoanode for direct solar-to-chemical conversion
Yao L.; Liu Y.; Cho H.-H.; Xia M.; Sekar A.; Primera Darwich B.; Wells R.A.; Yum J.-H.; Ren D.; Grätzel M.; Guijarro N.; Sivula K.
发表日期2021
ISSN17545692
起始页码3141
结束页码3151
卷号14期号:5
英文摘要Organic semiconductors (OSs) are emerging candidates as light-harvesting materials in photoelectrochemical (PEC) cells for direct solar-to-chemical conversion. Despite significant recent progress with OS-based photocathodes, the development of efficient and stable OS-based photoanodes remains a challenge. Here, we demonstrate the concept of an in situ formed covalent polymer network (CPN) in a hybrid CPN:SnO2 bulk-heterojunction (BHJ) to increase the photocurrent density (Jph) and stability of OS-based photoanodes for PEC splitting of hydroiodic acid (HI). Our results indicate that the CPN:SnO2 BHJ overcomes the limited exciton diffusion length in OSs and provides a Jph improvement of more than three orders of magnitude compared to equivalent bilayer heterojunctions. Furthermore, insight into the operation of the hybrid BHJ in direct contact with aqueous electrolyte is gained with electrochemical impedance spectroscopy and PEC measurements under varying pH. With 1 M HI (pH 0) as the electrolyte, an optimized CPN:SnO2 photoanode without catalyst or protection layer delivers a Jph of 3.3 mA cm-2 at the thermodynamic potential of iodide oxidation (+0.54 V vs. the normal hydrogen electrode) and a continuous operation for 27 h (Jph loss of 12%), representing a new benchmark for OS photoanodes for solar-to-chemical conversion. Complete HI splitting is further demonstrated in an all-OS photocathode/photoanode PEC cell to produce H2 and I3- from simulated sunlight without applied bias. © 2021 The Royal Society of Chemistry.
英文关键词Electrochemical impedance spectroscopy; Electrolytes; Field emission cathodes; Heterojunctions; Organic semiconductor materials; Photocathodes; Photocurrents; Bulk heterojunction (BHJ); Exciton diffusion length; Hybrid bulk heterojunctions; Normal hydrogen electrodes; Photocurrent density; Photoelectrochemicals; Thermodynamic potentials; Three orders of magnitude; Photoelectrochemical cells; chemical compound; detection method; electrode; electrolyte; fuel cell; oxidation; thermodynamics
语种英语
来源期刊Energy & Environmental Science
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/190675
作者单位Institute of Chemical Sciences and Engineering (ISIC), École Polytechnique Fédérale de Lausanne (EPFL), Station 6, Lausanne, 1015, Switzerland
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GB/T 7714
Yao L.,Liu Y.,Cho H.-H.,et al. A hybrid bulk-heterojunction photoanode for direct solar-to-chemical conversion[J],2021,14(5).
APA Yao L..,Liu Y..,Cho H.-H..,Xia M..,Sekar A..,...&Sivula K..(2021).A hybrid bulk-heterojunction photoanode for direct solar-to-chemical conversion.Energy & Environmental Science,14(5).
MLA Yao L.,et al."A hybrid bulk-heterojunction photoanode for direct solar-to-chemical conversion".Energy & Environmental Science 14.5(2021).
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