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Synthesis and photochemical study of N-doped mixed oxide solid solution photocatalyst for hydrogen production under visible light irradiation.

机译：可见光照射下制氢用氮掺杂混合氧化物固溶光催化剂的合成及光化学研究。

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摘要

Sol-gel method was used to synthesize N-doped solid solution mixed oxide photocatalysts. N-doped GaZn mixed oxide photocatalyst, N-doped Zn0.75 Cd0.25O2 photocatalyst, and N-doped CdIn 2O4 photocatalysts were synthesized and characterized. Preliminary work was conducted for the screening of the photocatalysts to determine which photocatalyst material is capable of absorbing visible light while producing hydrogen through water splitting. Photocatalytic activities were conducted in a pure water reaction solution and in the presence of sacrificial electron donors. Sacrificial electron donors are used to donate electrons, thus prevent the photocatalyst from being photo-degraded. A plexiglass gas-tight batch reactor was used for the photocatalytic water to produce hydrogen. Two 15-W LED lamps were used as the light source.;XRD patterns showed that the photocatalyst materials consist of well crystalline structure. The diffraction peaks of the materials shifted to higher angels indicating that the crystal structure obtained were not a physical mixture of In2O3 and CdO phases but a CdIn2O 4 solid solution. The photocatalytic activity of the photocatalyst increase when small amounts of In2O3 and CdO coexist in the structure of the N-doped CdIn2O4 photocatalyst.;Sol aging time had an effect on the photocatalytic activity of the photocatalysts. As the sol aging time increases, the photocatalytic activity of the photocatalyst increased. N-doped CdIn2O4 photocatalyst aged for 2 hours showed no hydrogen production as compared to photocatalyst aged for 12 hours. The photocatalyst aged for 24 hours showed high hydrogen production as compared to photocatalyst aged for 12 hours.;Preliminary results showed that N-doped CdIn2O4 photocatalyst produced more hydrogen and worked well without the sacrificial electron donors. The effect of urea was examined to determine if urea impacts the crystal structure of the photocatalysts. The results showed that the concentration of urea had an effect on the crystal structure of the photocatalyst and the photocatalytic activity. The photocatalyst particles consist of high crystallite structure as the concentration of urea increases. However, an increase in urea concentration affects the size of the particles. The particle size increases as the urea concentration increases. N-doped CdIn2O4 photocatalysts were synthesized at different sintering temperatures to determine the effects on the photocatalytic water splitting. The particle size of the photocatalyst is increased with increasing sintering temperature. A larger particles size, 900 °C catalysts, has a low photocatalytic hydrogen production. The photocatalyst sintered at 800 °C yielded more hydrogen compared to other photocatalysts sintered at 600 °C, 700 °C, and 900 °C. The hydrogen production rate of 800 °C was 154.27 micromol/h and the apparent quantum yield was 8.3 %, at approximately 450 nm. Nitrogen doping modified the band gap of CdIn2O4 and enhanced absorption of visible light.;The photocatalyst was loaded with Pt to enhance the photocatalytic hydrogen production; however the production rate of Pt/N-doped CdIn2O 4 photocatalyst was lower than that of 800 °C photocatalyst. The hydrogen production rate of Pt (2 wt.%)-loaded was 117.24 micromol/h with an apparent quantum yield of 6.1%.;The stability of the photocatalyst was examined with 800 °C photocatalyst without sacrificial electron donors. The physicochemical stability of the photocatalyst was assessed during three reaction cycles. The results showed that the photocatalyst is stable and does not photo-degrade. The hydrogen production rate of reaction cycle 2 was 195.24 micromol/h and the apparent quantum yield was 10% (~465 nm).;The photocatalytic hydrogen production was enhanced by loading CuO nano-size clusters on N-doped CdIn2O4 photocatalyst. The hydrogen production rate was 234.87 micromol/h and the apparent quantum yield was 12.2%.
机译：采用溶胶-凝胶法合成了掺氮固溶体混合氧化物光催化剂。合成并表征了N掺杂的GaZn复合氧化物光催化剂，N掺杂的Zn0.75 Cd0.25O2光催化剂和N掺杂的CdIn 2O4光催化剂。进行了筛选光催化剂的初步工作，以确定哪种光催化剂材料能够吸收可见光，同时通过水分解产生氢。在纯水反应溶液中和牺牲电子给体的存在下进行光催化活性。牺牲电子给体用于提供电子，从而防止光催化剂被光降解。将有机玻璃气密间歇反应器用于光催化水以产生氢。用两个15W LED灯作为光源。X射线衍射图表明光催化剂材料具有良好的晶体结构。材料的衍射峰移向更高的角度，表明获得的晶体结构不是In2O3和CdO相的物理混合物，而是CdIn2O 4固溶体。当N掺杂的CdIn2O4光催化剂的结构中共存有少量In2O3和CdO时，光催化剂的光催化活性增加。溶胶老化时间对光催化剂的光催化活性有影响。随着溶胶老化时间的增加，光催化剂的光催化活性增加。与老化12小时的光催化剂相比，老化2小时的N掺杂的CdIn 2 O 4光催化剂没有产生氢。与老化12小时的光催化剂相比，老化24小时的光催化剂显示较高的氢产生。初步结果表明，N掺杂的CdIn2O4光催化剂产生更多的氢，并且在没有牺牲电子给体的情况下也能很好地工作。检查尿素的作用以确定尿素是否影响光催化剂的晶体结构。结果表明，尿素的浓度对光催化剂的晶体结构和光催化活性有影响。随着尿素浓度的增加，光催化剂颗粒由高结晶结构组成。但是，尿素浓度的增加会影响颗粒的尺寸。粒径随着尿素浓度的增加而增加。在不同的烧结温度下合成了N掺杂的CdIn2O4光催化剂，以确定对光催化水分解的影响。光催化剂的粒径随着烧结温度的升高而增加。较大粒径的催化剂（900℃）具有较低的光催化产氢量。与在600°C，700°C和900°C下烧结的其他光催化剂相比，在800°C下烧结的光催化剂产生更多的氢。在约450nm下，800℃的氢气产生速率为154.27μmol/ h，表观量子产率为8.3％。氮掺杂改变了CdIn2O4的能带隙并增强了可见光的吸收。然而，Pt / N掺杂的CdIn2O 4光催化剂的生产率低于800℃的光催化剂。负载Pt（2 wt。％）的氢气产生率为117.24 micromol / h，表观量子产率为6.1％。;在没有牺牲电子给体的情况下，用800°C的光催化剂测试了光催化剂的稳定性。在三个反应周期中评估了光催化剂的物理化学稳定性。结果表明，光催化剂是稳定的，并且不会光降解。反应周期2的产氢速率为195.24 micromol / h，表观量子产率为10％（〜465 nm）。通过在N掺杂的CdIn2O4光催化剂上负载CuO纳米尺寸的团簇可以提高光催化产氢量。氢气产生率为234.87微摩尔/小时，表观量子产率为12.2％。

著录项

  • 作者

    Leswifi, Taile Y.;

  • 作者单位

    Michigan Technological University.;

  • 授予单位 Michigan Technological University.;
  • 学科 Engineering Environmental.;Alternative Energy.
  • 学位 Ph.D.
  • 年度 2014
  • 页码 140 p.
  • 总页数 140
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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