Enhanced photocatalytic activity for H2 evolution under irradiation of UV-vis light by Au-modified nitrogen-doped TiO2.

Enhanced photocatalytic activity for H2 evolution under irradiation of UV-vis light by Au-modified nitrogen-doped TiO2.
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DOI:
10.1371/journal.pone.0103671
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发表时间:
2014
期刊:
影响因子:
3.7
通讯作者:
Zhang M
Zhang M
中科院分区:
综合性期刊3区
文献类型:
--
作者:
Zhao W;Ai Z;Dai J;Zhang M

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光催化水分解制氢是解决许多能源和环境问题的潜在方法。开发可见光活性光催化剂以有效利用太阳光并寻找适当的方法来提高光催化产氢活性一直是研究的热点。本研究试图通过N掺杂和Au负载来扩大太阳光的利用并增强TiO2的光催化活性。合成了 Au/N 掺杂 TiO2 光催化剂,并成功用于分别在紫外光和紫外可见光照射下光催化水分解产氢。使用 X 射线衍射 (XRD)、透射电子显微镜 (TEM)、X 射线光电子能谱 (XPS)、紫外可见漫反射光谱 (DRS)、光致发光光谱 (PL) 和光电化学表征对样品进行了表征。 DRS 分别通过掺杂 N 和沉积 Au 将光吸收扩展到可见光区域。 PL 分析表明,由于 N 掺杂而导致电子-空穴复合,并且由于负载的金颗粒而有效抑制了电子-空穴复合。在紫外光照射下,合成样品的光催化产氢速率遵循Au/TiO2>Au/N掺杂TiO2>TiO2>N掺杂TiO2的顺序。在紫外可见光照射下,N-TiO2 和 Au/N-TiO2 样品比相应的无氮样品(TiO2 和 Au/TiO2)表现出更高的 H2 释放量。这种不一致的结果可能归因于 N 的掺杂和 Au 颗粒的表面等离子体共振 (SPR) 效应延长了可见光吸收。光电化学表征进一步表明Au/N掺杂TiO2的可见光响应增强。对比研究表明,氮掺杂和金负载的结合增强了TiO2的可见光响应,提高了太阳能的利用率,大大提高了紫外可见光下光催化产氢的活性。
Photocatalytic water splitting for hydrogen evolution is a potential way to solve many energy and environmental issues. Developing visible-light-active photocatalysts to efficiently utilize sunlight and finding proper ways to improve photocatalytic activity for H2 evolution have always been hot topics for research. This study attempts to expand the use of sunlight and to enhance the photocatalytic activity of TiO2 by N doping and Au loading. Au/N-doped TiO2 photocatalysts were synthesized and successfully used for photocatalytic water splitting for H2 evolution under irradiation of UV and UV–vis light, respectively. The samples were characterized using X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), UV–vis diffuse reflectance spectroscopy (DRS), photoluminescence spectroscopy (PL), and photoelectrochemical characterizations. DRS displayed an extension of light absorption into the visible region by doping of N and depositing with Au, respectively. PL analysis indicated electron-hole recombination due to N doping and an efficient inhibition of electron-hole recombination due to the loaded Au particles. Under the irradiation of UV light, the photocatalytic hydrogen production rate of the as-synthesized samples followed the order Au/TiO2 > Au/N-doped TiO2 > TiO2 > N-doped TiO2. While under irradiation of UV–vis light, the N-TiO2 and Au/N-TiO2 samples show higher H2 evolution than their corresponding nitrogen-free samples (TiO2 and Au/TiO2). This inconsistent result could be attributed to the doping of N and the surface plasmonic resonance (SPR) effect of Au particles extending the visible light absorption. The photoelectrochemical characterizations further indicated the enhancement of the visible light response of Au/N-doped TiO2. Comparative studies have shown that a combination of nitrogen doping and Au loading enhanced the visible light response of TiO2 and increased the utilization of solar energy, greatly boosting the photocatalytic activity for hydrogen production under UV–vis light.
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