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Functional Pd/reduced graphene oxide nanocomposites: effect of reduction degree and doping in hydrodechlorination catalytic activity
Journal of Nanoparticle Research ( IF 2.5 ) Pub Date : 2019-12-18 , DOI: 10.1007/s11051-019-4696-x
Cristina Ruiz-Garcia , Yu Lei , Francisco Heras , Ana Laura Elías , Mauricio Terrones , Miguel A. Gilarranz

Pd catalysts supported on carbon have interesting features for chlorophenols-bearing water treatment by hydrodechlorination, including high stability, activity, and tunable support. In this work, a set of materials based on reduced graphene oxide (rGO) with different degrees of reduction, surface oxygen groups, nitrogen doping, and specific surface area were decorated with Pd nanoparticles, with diameter average size between 5 and 50 nm. Ethanol, hydrazine monohydrate, and sodium borohydride were used as reducing agents, and Pd(AcO)2 was used as a Pd precursor to obtain Pd/rGO nanocomposites in our developed one-pot synthesis approach. A thorough characterization revealed that a similar degree of reduction was obtained for sodium borohydride at 25 °C and hydrazine at 60 °C, although hydrazine also led to nitrogen doping. Pd nanoparticles were homogenously nucleated on the surface of the GO and the obtained nanocomposites were tested as catalysts for hydrodechlorination of 4-chlorophenol in the aqueous phase. The materials with a higher degree of reduction showed the best specific catalytic activity at 70 °C. However, the turnover frequency (TOF) only increased with the reduction degree for the N-doped Pd/rGO, indicating the important role of the nitrogenous functionalities in the catalytic activity. Therefore, the N doping of Pd/rGO catalysts is a feasible strategy to synthesize catalysts highly active for hydrodechlorination.

Graphical abstract



中文翻译:

功能性钯/还原氧化石墨烯纳米复合材料:还原度和掺杂对加氢脱氯催化活性的影响

负载在碳上的Pd催化剂具有通过加氢脱氯处理含氯酚水的有趣功能,包括高稳定性,活性和可调载体。在这项工作中,一组基于具有不同还原度,表面氧基团,氮掺杂和比表面积的还原氧化石墨烯(rGO)的材料用Pd纳米粒子装饰,其直径平均大小在5到50 nm之间。乙醇,一水合肼和硼氢化钠用作还原剂,Pd(AcO)2在我们开发的一锅法合成方法中,将其用作Pd前驱体以获得Pd / rGO纳米复合材料。彻底的表征表明,尽管肼也会导致氮掺杂,但在25°C的硼氢化钠和60°C的肼的还原度相似。Pd纳米颗粒在GO表面均匀地成核,并测试了所得的纳米复合材料作为在水相中对4-氯苯酚进行加氢脱氯的催化剂。还原度较高的材料在70°C时表现出最佳的比催化活性。然而,周转频率(TOF)仅随着N掺杂的Pd / rGO的还原程度而增加,表明含氮官能团在催化活性中的重要作用。所以,

图形概要

更新日期:2019-12-18
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