期刊
FARADAY DISCUSSIONS
卷 222, 期 -, 页码 176-189出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9fd00098d
关键词
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资金
- Natural Sciences and Engineering Research Council of Canada [RGPIN 2017-05143]
- Canada Foundation for Innovation
- Dalhousie University
- Nova Scotia Graduate Scholarship
- NSERC
H(2)has been identified as one of the potential energy vectors that can provide a sustainable energy supply when produced through solar-driven water-splitting reaction. Si is the second most abundant element in the Earth's crust and can absorb a significant fraction of the solar spectrum while presenting little toxicity risk, making it an attractive material for photocatalytic H(2)production. Hydrogen-terminated mesoporous Si (mp-Si) nanoparticles can be utilized to effectively drive the hydrogen evolution reaction using UV-to-visible light. In this work, the response of the photocatalytic activity of mp-Si nanoparticles to a series of HF acid treatments was investigated. A two-step magnesiothermic reduction method was used to prepare crystalline mp-Si nanoparticles with a specific surface area of 573 m(2)g(-1). The HF etching process was optimized as a function of the amount of acid added and the reaction time. The reaction time did not influence the H(2)evolution rate substantially. However, the amount of HF used did have a significant effect on the photocatalytic activity. In the presence of >= 1.0 mL HF acid per 0.010 g of Si, morphological damage was observed using electron microscopy. N(2)adsorption measurements indicated that the pore size and surface area were also altered. Solution-phase(19)F{H-1} NMR studies indicated the formation of SiF(5)(-)and SiF(6)(2-)when larger volumes of HF were used. Both factors, morphological damage and the presence of byproducts in the pores, likely result in a lowering of the photocatalytic H(2)evolution rate. Under the optimized HF treatment conditions (0.5 mL of HF per 0.010 g of Si), a H(2)evolution rate of 1398 +/- 30 mu mol g(-1)h(-1)was observed.
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