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A Nanojunction Polymer Photoelectrode for Efficient Charge Transport and Separation.

ABSTRACT: A metal-free photoanode nanojunction architecture, composed of B-doped carbon nitride nanolayer and bulk carbon nitride, was fabricated by a one-step approach. This type of nanojunction (s-BCN) overcomes a few intrinsic drawbacks of carbon nitride film (severe bulk charge recombination and slow charge transfer). The top layer of the nanojunction has a depth of ca. 100 nm and the bottom layer is ca. 900 nm. The nanojunction photoanode results into a 10-fold higher photocurrent than bulk graphitic carbon nitride (G-CN) photoanode, with a record photocurrent density of 103.2 μA cm^-2 at 1.23 V vs. RHE under one sun irradiation and an extremely high incident photon-to-current efficiency (IPCE) of ca. 10 % at 400 nm. Electrochemical impedance spectroscopy, Mott-Schottky plots, and intensity-modulated photocurrent spectroscopy show that such enhancement is mainly due to the mitigated deep trap states, a more than 10 times faster charge transfer rate and nearly three times higher conductivity due to the nanojunction architecture.

SUBMITTER: Ruan Q

PROVIDER: S-EPMC5519949 | biostudies-literature | 2017 Jul

REPOSITORIES: biostudies-literature

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A Nanojunction Polymer Photoelectrode for Efficient Charge Transport and Separation.

Ruan Qiushi Q Luo Wenjun W Xie Jijia J Wang Yiou Y Liu Xu X Bai Zhiming Z Carmalt Claire J CJ Tang Junwang J

Angewandte Chemie (International ed. in English) 20170612 28

A metal-free photoanode nanojunction architecture, composed of B-doped carbon nitride nanolayer and bulk carbon nitride, was fabricated by a one-step approach. This type of nanojunction (s-BCN) overcomes a few intrinsic drawbacks of carbon nitride film (severe bulk charge recombination and slow charge transfer). The top layer of the nanojunction has a depth of ca. 100 nm and the bottom layer is ca. 900 nm. The nanojunction photoanode results into a 10-fold higher photocurrent than bulk graphitic ...[more]

PMID: 28520233

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Project description:The ongoing depletion of fossil fuels has led to an intensive search for additional renewable energy sources. Solar-based technologies could provide sufficient energy to satisfy the global economic demands in the near future. Photovoltaic (PV) cells are the most promising man-made devices for direct solar energy utilization. Understanding the charge separation and charge transport in PV materials at a molecular level is crucial for improving the efficiency of the solar cells. Here, we use light-induced EPR spectroscopy combined with DFT calculations to study the electronic structure of charge separated states in blends of polymers (P3HT, PCDTBT, and PTB7) and fullerene derivatives (C60-PCBM and C70-PCBM). Solar cells made with the same composites as active layers show power conversion efficiencies of 3.3% (P3HT), 6.1% (PCDTBT), and 7.3% (PTB7), respectively. Upon illumination of these composites, two paramagnetic species are formed due to photo-induced electron transfer between the conjugated polymer and the fullerene. They are the positive, P(+), and negative, P(-), polarons on the polymer backbone and fullerene cage, respectively, and correspond to radical cations and radical anions. Using the high spectral resolution of high-frequency EPR (130 GHz), the EPR spectra of these species were resolved and principal components of the g-tensors were assigned. Light-induced pulsed ENDOR spectroscopy allowed the determination of (1)H hyperfine coupling constants of photogenerated positive and negative polarons. The experimental results obtained for the different polymer-fullerene composites have been compared with DFT calculations, revealing that in all three systems the positive polaron is distributed over distances of 40-60 Å on the polymer chain. This corresponds to about 15 thiophene units for P3HT, approximately three units for PCDTBT, and about three to four units for PTB7. No spin density delocalization between neighboring fullerene molecules was detected by EPR. Strong delocalization of the positive polaron on the polymer donor is an important reason for the efficient charge separation in bulk heterojunction systems as it minimizes the wasteful process of charge recombination. The combination of advanced EPR spectroscopy and DFT is a powerful approach for investigation of light-induced charge dynamics in organic photovoltaic materials.

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A Nanojunction Polymer Photoelectrode for Efficient Charge Transport and Separation.

Publications

A Nanojunction Polymer Photoelectrode for Efficient Charge Transport and Separation.

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