论文标题

用Pt掺杂的镁含量,用​​于光催化氢的进化

Magneli phases doped with Pt for photocatalytic hydrogen evolution

论文作者

Wierzbicka, Ewa, Domaschke, Maximilian, Denisov, Nikita, Fehn, Dominik, Hwang, Imgon, Kaufmann, Marlena, Kunstmann, Babette, Schmidt, Jochen, Meyer, Karsten, Peukert, Wolfgang, Schmuki, Patrik

论文摘要

已定义的定位化钛氧化物(Ti $ _x $ o $ $ _ {2x-1} $,$ 3 <x <10 $)称为Magneli阶段,主要是因为其异常的高电导率和类似金属的行为而进行了研究。在光催化中,据报道,含有钛颗粒的镁相可提供有利的电荷分离,从而提高了反应效率。在当前的工作中,我们描述了含镁的混合相纳米颗粒的一步合成,该纳米颗粒含有直接集成的少量PT。对于H $ _2 $ Evolution的相位优化的纳米颗粒(仅包含几百ppm pt)是非常有效的光催化剂(它们提供的h $ _2 $进化比普通疗法酶高出50-100倍,而普通的解剖酶载有相似量的PT)。这些光催化剂是在结合热壁反应器的设置中合成的,该反应器用于Tiox合成与产生PT纳米颗粒的火花发电机。不同的反应器温度导致解剖酶和木质相之间的各种相比。使用XRD,HRTEM,XPS和EPR光谱以及ICP -OES分析来表征钛纳米颗粒(约24-53 nm)。以900 $^\ CIRC $ C制备的最佳光催化剂(由32%剖析酶,11%金红石和57%的Magneli相结合的混合相颗粒组成,加载了290 ppm的PPM)可以提供光催化H $ _2 $ _2 $的演化率。 5432 Micromol H $^{ - 1} g $^{ - 1} $用于UV和CA。 1670 Micromol H $^{ - 1} g $^{ - 1} $用于AM1.5照明。对于转换为更高量的木尼相(1000 $^\ circ $ c和1100 $^\ circ $ c)的粉末,观察到光催化H $ _2 $发电活动的急剧损失。因此,在最佳条件下,高光催化效率归因于与常规的PT/Aratase连接相比,Magneli Titania和PT的多障碍之间的有效协同作用。

Defined substoichiometric titanium oxides (Ti$_x$O$_{2x-1}$ with $3 < x < 10$) called Magneli phases have been investigated mostly for their unusual high conductivity and metal-like behavior. In photocatalysis, Magneli phase containing titania particles have been reported to provide favorable charge separation resulting in enhanced reaction efficiency. In the current work we describe a one-step synthesis of Magneli-containing mixed phase nanoparticles that carry directly integrated minute amounts of Pt. Phase optimized nanoparticles that contain only a few hundred ppm Pt are very effective photocatalysts for H$_2$ evolution (they provide a 50-100 times higher H$_2$ evolution than plain anatase loaded with a similar amount of Pt). These photocatalysts are synthesized in a setup combining a hot-wall reactor that is used for TiOx synthesis with a spark generator producing Pt nanoparticles. Different reactor temperatures result in various phase ratios between anatase and Magneli phases. The titania nanoparticles (ca. 24 - 53 nm) were characterized using XRD, HRTEM, XPS and EPR spectra as well as ICP-OES analysis. The best photocatalyst prepared at 900$^\circ$C (which consists of mixed phase particles of 32% anatase, 11% rutile and 57% Magneli phases loaded with 290 ppm of Pt) can provide a photocatalytic H$_2$ evolution rate of ca. 5432 micromol h$^{-1} g$^{-1}$ for UV and ca. 1670 micromol h$^{-1} g$^{-1}$ for AM1.5 illumination. For powders converted to higher amounts of Magneli phases (1000$^\circ$C and 1100$^\circ$C), a drastic loss of the photocatalytic H$_2$ generation activity is observed. Thus, the high photocatalytic efficiency under best conditions is ascribed to an effective synergy between multi-junctions of Magneli titania and Pt that enable a much more effective charge separation and reaction than conventional Pt/anatase junctions.

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