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Self-Assembled Framework Enhances Electronic Communication of Ultrasmall-Sized Nanoparticles for Exceptional Solar Hydrogen Evolution
Open accessAbstract
Colloidal quantum dots (QDs) have demonstrated great promise in artificial photosynthesis. However, the ultrasmall size hinders its controllable and effective interaction with cocatalysts. To improve the poor interparticle electronic communication between free QD and cocatalyst, we design here a self-assembled architecture of nanoparticles, QDs and Pt nanoparticles, simply jointed together by molecular polyacrylate to greatly enhance the rate and efficiency of interfacial electron transfer (ET). The enhanced interparticle electronic communication is confirmed by femtosecond transient absorption spectroscopy and X-ray transient absorption. Taking advantage of the enhanced interparticle ET with a time scale of ∼65 ps, 5.0 mL of assembled CdSe/CdS QDs/cocatalysts solution produces 94 ± 1.5 mL (4183 ± 67 μmol) of molecular H 2 in 8 h, giving rise to an internal quantum yield of ∼65% in the first 30 min and a total turnover number of >1.64 × 10 7 per Pt nanoparticle. This study demonstrates that self-assembly is a promising way to improve the sluggish kinetics of the interparticle ET process, which is the key step for advanced H 2 photosynthesis.
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Cites
Xiang, Q., Yu, J., & Jaroniec, M. (2012) · Journal of the American Chemical Society · doi:10.1021/ja302846n · Cited by 2,360
Hohmann-Marriott, M. F., & Blankenship, R. E. (2011) · Annual Review of Plant Biology · doi:10.1146/annurev-arplant-042110-103811 · Cited by 744
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Wu, H., Li, X., Tung, C., & Wu, L. (2019) · Advanced Materials · doi:10.1002/adma.201900709 · Cited by 486
Self-citationZhao, Y., Waterhouse, G. I. N., Chen, G., Xiong, X., Wu, L.-Z., Tung, C.-H., & Zhang, T. (2019) · Chemical Society Reviews · doi:10.1039/c8cs00607e · Cited by 435
Self-citationSite-selective photoinduced cleavage and profiling of DNA by chiral semiconductor nanoparticles
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Metadata
- Authors
- Li, X.-B., Gao, Y.-J., Wang, Y., Zhan, F., Zhang, X.-Y., Kong, Q.-Y., Zhao, N.-J., Guo, Q., Wu, H.-L., Li, Z.-J., Tao, Y., Zhang, J.-P., Chen, B., Tung, C.-H., & Wu, L.-Z.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2017-03-24
- Volume
- 139
- Issue
- 13
- Pages
- 4789-4796
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2594439702
- Cited by
- 170
- References
- 2
- FWCI
- 6.90
- Type
- journal article
- Language
- en
- Open access
- green
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- The paper
- Li, X.-B., Gao, Y.-J., Wang, Y., Zhan, F., Zhang, X.-Y., Kong, Q.-Y., Zhao, N.-J., Guo, Q., Wu, H.-L., Li, Z.-J., Tao, Y., Zhang, J.-P., Chen, B., Tung, C.-H., & Wu, L.-Z. (2017). Self-Assembled Framework Enhances Electronic Communication of Ultrasmall-Sized Nanoparticles for Exceptional Solar Hydrogen Evolution. Journal of the American Chemical Society. https://doi.org/10.1021/jacs.6b12976
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