Preparation of carbide-derived carbon supported platinum catalysts

Preparation of carbide-derived carbon supported platinum catalysts
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DOI:
10.1016/j.cattod.2014.10.049
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发表时间:
2015-07-01
期刊:
影响因子:
5.3
通讯作者:
Etzold, B. J. M.
Etzold, B. J. M.
中科院分区:
化学2区
文献类型:
--
作者:
Hasse, B.;Glaesel, J.;Etzold, B. J. M.

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明确的碳负载催化剂对于推断结构活性关系和催化剂优化很有意义。碳化物衍生碳(CDC)是具有可调孔结构的高纯度多孔碳。研究了铂在硅和碳化钛基CDC上的沉积,采用酸处理、铂前驱体离子吸附和气相还原三步工艺。确定了这些步骤对碳载体性质的影响以及控制铂负载量和所得簇尺寸的可能性。最关键的是酸处理步骤,其中引入了氧基团。如果功能化程度太高(非碳含量高于 30 wt%),硝酸处理可能会导致孔结构受到严重破坏。对于硫酸处理,非碳含量低于 15 wt%,并且仅观察到孔隙结构的微小变化。离子吸附技术可以成功地转移到CDC支持物上。对于中等到高度的功能化(非碳含量高于 20 wt%),实现了 2.5 wt% 铂的完全沉积。通过选择铂前驱体、浸渍 pH 值和还原温度,铂簇尺寸可在 2.5 至 5.3 nm 之间变化。因此,可以推断出如何制备基于 CDC 和离子吸附技术的调谐 Pt/C 催化剂的重要知识。 (C) 2014 Elsevier B.V. 保留所有权利。
Well defined carbon supported catalysts are of interest to deduce structure activity relationships and for catalyst optimization. Carbide-derived carbons (CDC) are high purity porous carbons with tunable pore structure. The deposition of platinum on silicon and titanium carbide based CDC was studied, using a three step process of acid treatment, ion-adsorption of platinum precursor and gas phase reduction. The influence of the steps on the carbon support properties and possibility to control the platinum loading and resulting cluster size was determined. Most crucial is the acid treatment step, where oxygen groups are introduced. At a too high degree of functionalization (non-carbon content above 30 wt%), which can result for nitric acid treatment, the pore structure is heavily attacked. For sulfuric acid treatments non-carbon contents below 15 wt% and only minor changes in the pore structure were observed. The ion-adsorption technique could be successfully transferred to the CDC supports. For medium to high degrees of functionalization (non-carbon contents above 20 wt%) the full deposition of 2.5 wt% of platinum was achieved. By the choice of platinum precursor, the pH of impregnation and the temperature of reduction the platinum cluster size could be varied from 2.5 to 5.3 nm. Thus, important knowledge how to prepare tuned Pt/C catalysts based on CDC and the ion-adsorption technique could be deduced. (C) 2014 Elsevier B.V. All rights reserved.