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Plasmonic gold deposited on mesoporous TixSi1−xO2 with isolated silica in lattice: An excellent photocatalyst for photocatalytic conversion of CO2 into methanol under visible light irradiation
Journal of CO2 Utilization ( IF 7.2 ) Pub Date : 2018-07-07 , DOI: 10.1016/j.jcou.2018.06.016
Rajkumar Yadav , Vipin Amoli , Jitendra Singh , Manish Kumar Tripathi , Piyali Bhanja , Asim Bhaumik , Anil Kumar Sinha

Solar-driven chemical production of methanol from CO2 has become a hot topic of research due to high-value addition, with methanol as a product, as well as reduction of CO2 which is a greenhouse gas. Here we report gold nanoparticles deposited on mesoporous titania with isolated Si sites, which converted CO2 into methanol under visible light irradiation using LED light source. Si amount in titania lattice was optimized to obtain the best methanol yield. DFT calculation showed that Si sites incorporation was responsible for higher adsorption of CO2 onto the surface, which was further proved experimentally with CO2 uptake results. We achieved highest methanol production of 1835 μmolgcat−1 using Au/TixSi1−xO2 material with 28 mol% Si in titania lattice and 1.0 wt% Au nanoparticles deposition. The Au/TixSi1−xO2 photocatalysts were thoroughly characterized by inductively coupled plasma atomic emission (ICP-AES) spectrometry, powder X-ray diffraction (PXRD), field emission scanning electron microscopy (FE-SEM), high angle annular dark field-scanning transmission electron microscopic (HAADF-STEM), transmission electron microscopy (TEM), energy dispersive X-ray spectrometry (EDX), 29Si MAS NMR, UV-vis diffuse reflection spectroscopy (DRS), N2 sorption studies, CO2 uptake experiments, cyclic voltammetry (CV) and DFT calculations. The products were analyzed by GC-FID, GC–MS, and HPLC. The photocatalytic reaction was monitored using in situ FT-IR which established the formation of formaldehyde as an intermediate product which further converted into methanol.



中文翻译:

用晶格中的分离二氧化硅在等孔Ti x Si 1− x O 2上沉积等离子金:一种出色的光催化剂,用于在可见光照射下将CO 2光催化转化为甲醇

由于以甲醇为产物的高附加值添加以及温室气体CO 2的还原,太阳能从CO 2中化学驱动生产甲醇已成为研究的热点。在这里,我们报道了金纳米颗粒沉积在介孔二氧化钛上并具有孤立的Si位点,该颗粒在可见光照射下使用LED光源将CO 2转化为甲醇。优化二氧化钛晶格中的Si量以获得最佳的甲醇收率。DFT计算表明,Si位点的引入是导致CO 2在表面上的更高吸附的原因,实验结果进一步证明了CO 2的吸收。我们实现了1835μmolg猫的最高甲醇产量-1使用Au / Ti x Si 1- x O 2材料,在二氧化钛晶格中具有28 mol%的Si和1.0 wt%的Au纳米颗粒沉积。通过电感耦合等离子体原子发射光谱(ICP-AES),粉末X射线衍射(PXRD),场发射扫描电子显微镜(FE-SEM),高角度对Au / Ti x Si 1- x O 2光催化剂进行了全面表征环形暗场扫描透射电子显微镜(HAADF-STEM),透射电子显微镜(TEM),能量色散X射线光谱法(EDX),29 Si MAS NMR,紫外-可见漫反射光谱法(DRS),N 2吸附研究,CO 2吸收实验,循环伏安法(CV)和DFT计算。用GC-FID,GC-MS和HPLC分析产物。使用原位FT-IR监测光催化反应,该FT-IR建立了甲醛的形成,该甲醛为中间产物,其进一步转化为甲醇。

更新日期:2018-07-07
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