Sensitization of Pt/TiO2 Using Plasmonic Au Nanoparticles for Hydrogen Evolution under Visible-Light Irradiation
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Au nanoparticles with different sizes (10, 20, 30, and 50 nm) were synthesized using a seed-assisted approach and anchored onto Pt/TiO2 employing 3-mercaptopropionic acid as the organic linker. The sizes of the Au nanoparticles were controlled within a narrow range so that the size-dependent surface plasmonic resonance effect on sensitizing Pt/TiO2 can be thoroughly studied. We found that 20 nm Au nanoparticles (Au20) gave the best performance in sensitizing Pt/TiO2 to generate H2 under visiblelight illumination. Photoelectrochemical measurements indicated that Au20-Pt/TiO2 exhibited the most efficient “hot” electrons separation among the studied catalysts, correlating well with the photocatalytic activity. The superior performance of Au-supported Pt/TiO2 (Au20-Pt/TiO2) compared with Au anchored to TiO2 (Au20/TiO2) revealed the important role of Pt as a cocatalyst for proton reduction. To elucidate how the visible-light excited hot electrons in Au nanoparticles involved in the proton-reduction reaction process, Au20/TiO2 was irradiated by visible light (λ > 420 nm) with the presence of Pt precursor (H2PtCl6) in a methanol aqueous solution under deaerated condition. Energy-dispersive X-ray spectroscopy mapping analysis on the recovered sample showed that Pt ions could be reduced on the surfaces of both Au nanoparticles and TiO2 support. This observation indicated that the generated hot electrons on Au nanoparticles were injected into the TiO2 conduction band, which were then subsequently transferred to Pt nanoparticles where proton reduction proceeded. Besides, the excited hot electrons could also participate in the proton reduction on Au nanoparticles surface.
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Photonic crystals consisting of TiO2 nanotube arrays (PMTiNTs) with periodically modulated diameters were fabricated using a precise charge-controlled pulsed anodization technique. The PMTiNTs were decorated with gold nanoparticles (Au NPs) to form plasmonic photonic crystal photocatalysts (Au-PMTiNTs). A systematic study of CO2 photoreduction performance on as-prepared samples was conducted using different wavelengths and illumination sequences. A remarkable selectivity of the mechanism of CO2 photoreduction could be engineered by merely varying the spectral composition of the illumination sequence. Under AM1.5 G simulated sunlight (pathway#1), the Au-PMTiNTs produced methane (302 µmol h-1) from CO2 with high selectivity (89.3%). When also illuminated by a UV-poor white lamp (pathway#2), the Au-PMTiNTs produced formaldehyde (420 µmol h-1) and carbon monoxide (323 µmol h-1) with almost no methane evolved. We confirmed the photoreduction results by 13C isotope labeling experiments using GC-MS. These results point to optical control of the selectivity of high-rate CO2 photoreduction through selection of one of two different mechanistic pathways. Pathway#1 implicates electron-hole pairs generated through interband transitions in TiO2 and Au as the primary active species responsible for reducing CO2 to methane. Pathway#2 involves excitation of both TiO2 and surface plasmons in Au. Hot electrons produced by plasmon damping and photogenerated holes in TiO2 proceed to reduce CO2 to HCHO and CO through a plasmonic Z-scheme.
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Disclaimer: No one is perfect, so please mind that there might be mistakes and typos.
dtubbenhauer@gmail.com
Corrected slides: dtubbenhauer.com/talks.html
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原版纸张【微信：741003700 】【(uvic毕业证书)维多利亚大学毕业证】【微信：741003700 】学位证，留信认证（真实可查，永久存档）offer、雅思、外壳等材料/诚信可靠,可直接看成品样本，帮您解决无法毕业带来的各种难题！外壳，原版制作，诚信可靠，可直接看成品样本。行业标杆！精益求精，诚心合作，真诚制作！多年品质 ,按需精细制作，24小时接单,全套进口原装设备。十五年致力于帮助留学生解决难题，包您满意。
本公司拥有海外各大学样板无数，能完美还原海外各大学 Bachelor Diploma degree, Master Degree Diploma
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留信网认证的作用:
1:该专业认证可证明留学生真实身份
2:同时对留学生所学专业登记给予评定
3:国家专业人才认证中心颁发入库证书
4:这个认证书并且可以归档倒地方
5:凡事获得留信网入网的信息将会逐步更新到个人身份内，将在公安局网内查询个人身份证信息后，同步读取人才网入库信息
6:个人职称评审加20分
7:个人信誉贷款加10分
8:在国家人才网主办的国家网络招聘大会中纳入资料，供国家高端企业选择人才
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Sensitization of Pt/TiO2 Using Plasmonic Au Nanoparticles for Hydrogen Evolution under Visible-Light Irradiation
- 1. ACS Applied Materials & Interfaces Article ASAP, 22 August 2017, DOI: 10.1021/acsami.7b06265 Key Contact Fenglong Wang (flwangsdu@gmail.com) Yijiao Jiang (yijiao.jiang@mq.edu.au) Rose Amal (r.amal@unsw.edu.au)
- 2. Figure 1. Strategy for synthesis of Au nanoparticles supported on Pt/TiO2 composite catalysts. ACS Applied Materials & Interfaces Article ASAP, 22 August 2017, DOI: 10.1021/acsami.7b06265
- 3. Figure 2. TEM images of the synthesized gold nanoparticles with size of approximately 50 nm (a), 30 nm (b), 20 nm (c), and 10 nm (d); TEM images of Pt/TiO2 showing 3 nm Pt nanoparticles distributed on the surface of TiO2 (e) and Au20-Pt/TiO2 nanocomposites displaying Au20 and Pt nanoparticles supported on the TiO2 surface (f). ACS Applied Materials & Interfaces Article ASAP, 22 August 2017, DOI: 10.1021/acsami.7b06265
- 4. Figure 3. (a) XPS Pt 4f spectrum and (b) XPS Au 4f spectrum of the Au20-Pt/TiO2 sample. Figure 4. Hydrogen-production activity of different catalysts under visible-light irradiation (λ > 420 nm) from water/methanol mixture. ACS Applied Materials & Interfaces Article ASAP, 22 August 2017, DOI: 10.1021/acsami.7b06265
- 5. Figure 6. Photocurrent responses of Au20Pt/TiO2 under full visible light spectrum (>420 nm), blue light (400 nm), green light (550 nm), and red light (675 nm). All measurements were performed with a 420 nm cutoff filter to prevent the excitation of TiO2 support under UV light. Bandpass filters (50 nm fwhm bandwidth) were used to obtain the 400, 550, and 675 nm light sources. Figure 5. Photocurrent response of Au nanoparticles with different sizes supported on Pt/TiO2 nanocomposites under visible-light irradiation (λ > 420 nm). Every 40 s cycle comprises 20 s of irradiation, followed by 20 s of dark current measurement. ACS Applied Materials & Interfaces Article ASAP, 22 August 2017, DOI: 10.1021/acsami.7b06265
- 6. Figure 7. TEM image of the products obtained through photodeposition of Pt on Au20/TiO2 nanocomposites (a−d) and the proposed photocatalytic hydrogen-production process on the Au-sensitized Pt/TiO2 under visible-light irradiation (e). ACS Applied Materials & Interfaces Article ASAP, 22 August 2017, DOI: 10.1021/acsami.7b06265
- 7. Figure 8. Photocurrent response of Au20Pt/TiO2 in the presence of (a) methanol and (b) ethanol as hole scavenger. PEC measurement is performed with a 420 nm cutoff filter to prevent the excitation of TiO2. The photocurrent response is baseline-corrected to show the SPR enhancement under visible light. ACS Applied Materials & Interfaces Article ASAP, 22 August 2017, DOI: 10.1021/acsami.7b06265