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Issue 12, 2017
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Photocatalytic oxygen evolution from low-bandgap conjugated microporous polymer nanosheets: a combined first-principles calculation and experimental study

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Abstract

Nanostructured semiconducting polymers have emerged as a very promising class of metal-free photocatalytic materials for solar water splitting. However, they generally exhibit low efficiency and lack the ability to utilize long-wavelength photons in a photocatalytic oxygen evolution reaction (OER). Here, based on first-principles calculations, we reveal that the two-dimensional (2D) aza-fused conjugated microporous polymer (aza-CMP) with a honeycomb network is a semiconductor with novel layer-dependent electronic properties. The bandgap of the as-synthesized aza-CMP nanosheets is measured to be 1.22 eV, suggesting that they can effectively boost light absorption in the visible and near infrared (NIR) region. More importantly, aza-CMP also possesses a valence band margin suitable for a photocatalytic OER. Taking advantage of the 2D layered nanostructure, we further show that the exfoliated ultrathin aza-CMP nanosheets can exhibit a three-fold enhancement in the photocatalytic OER. After deposition of a Co(OH)2 cocatalyst, the hybrid Co(OH)2/aza-CMP photocatalyst exhibits a markedly improved performance for photocatalytic O2 evolution. Furthermore, first-principles calculations reveal that the photocatalytic O2 evolution reaction is energetically feasible for aza-CMP nanosheets under visible light irradiation. Our findings reveal that nanostructured polymers hold great potential for photocatalytic applications with efficient solar energy utilization.

Graphical abstract: Photocatalytic oxygen evolution from low-bandgap conjugated microporous polymer nanosheets: a combined first-principles calculation and experimental study

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Publication details

The article was received on 22 Jan 2017, accepted on 27 Feb 2017, published on 02 Mar 2017 and first published online on 02 Mar 2017


Article type: Paper
DOI: 10.1039/C7NR00534B
Citation: Nanoscale, 2017,9, 4090-4096
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    Photocatalytic oxygen evolution from low-bandgap conjugated microporous polymer nanosheets: a combined first-principles calculation and experimental study

    L. Wang, Y. Wan, Y. Ding, Y. Niu, Y. Xiong, X. Wu and H. Xu, Nanoscale, 2017, 9, 4090
    DOI: 10.1039/C7NR00534B

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