Journal
NANOSCALE
Volume 9, Issue 12, Pages 4090-4096Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c7nr00534b
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Funding
- National Key Basic Research Program of China [2015CB351903]
- MOST [2016YFA0200602]
- National Natural Science Foundation of China [51402282, 21474095, 21573204, 21421063]
- CAS Key Research Program of Frontier Sciences [QYZDB-SSW-SLH018]
- Strategic Priority Research Program of CAS [XDB01020300]
- Fundamental Research Funds for the Central Universities
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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 O-2 evolution. Furthermore, first-principles calculations reveal that the photocatalytic O-2 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.
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