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One-Pot Synthesis of Biomass-Based Hierarchical Porous Carbons with a Large Porosity Development
Chemistry of Materials ( IF 7.2 ) Pub Date : 2017-08-01 00:00:00 , DOI: 10.1021/acs.chemmater.7b02218
Marta Sevilla 1 , Guillermo A. Ferrero 1 , Antonio B. Fuertes 1
Affiliation  

A sustainable one-pot scheme for the synthesis of hierarchical porous carbons formed from biomass is developed herein. It is based on the carbonization of biomass-derived products (glucose, glucosamine, soya flour, and microalgae) in the presence of an activating agent (potassium oxalate) and calcium carbonate nanoparticles that form a hard template. During carbonization, double carbonates are formed in situ, which results in modifications in the morphology and size of the template nanoparticles, giving rise to a carbon material with an open macroporous foam-like structure rich in micro-/mesopores, the latter developing via a redox reaction between the carbon and potassium carbonate and also as a result of the reaction between the carbon and the evolved CO2. The porosity can be tailored by selecting an appropriate precursor. Thus, the carbon materials are basically micro-/macroporous in the case of glucose and glucosamine, and micro-/meso-/macroporous when soya flour and microalgae are used. A direct relationship is observed between the amount of nitrogen present in the precursor and mesopore development. Hence, the addition of urea to the mixture of glucose and potassium oxalate and CaCO3 nanoparticles also yields micro-/meso-/macroporous carbons. The materials synthesized at 800 °C have large surface areas in the ∼1800–3100 m2/g range. At 750 °C, the materials synthesized from N-rich biomass combine ultralarge surface areas of 2400–3050 m2/g and a remarkable N-doping (2–3 wt % N). This combination of textural and chemical properties is highly appealing for many energy-related applications and also for adsorption-based processes.

中文翻译:

一锅法合成具有大孔隙率的生物质基分层多孔碳

本文开发了一种可持续的一锅法,用于合成由生物质形成的分级多孔碳。它基于生物质衍生产品(葡萄糖,葡萄糖胺,大豆粉和微藻类)在形成硬模板的活化剂(草酸钾)和碳酸钙纳米颗粒存在下的碳化。在碳化过程中,会在原位形成双碳酸盐,这会导致模板纳米颗粒的形态和尺寸发生变化,从而形成碳纤维,其具有开放的大孔泡沫状结构,富含微孔/中孔,后者通过碳纳米管形成。碳与碳酸钾之间的氧化还原反应,也是碳与放出的CO 2之间反应的结果。可以通过选择合适的前体来调整孔隙率。因此,在葡萄糖和葡萄糖胺的情况下,碳材料基本上是微/大孔的,而当使用大豆粉和微藻类时,碳的材料是微/中/大孔的。观察到前体中存在的氮量与中孔形成之间存在直接关系。因此,向葡萄糖,草酸钾和CaCO 3纳米颗粒的混合物中添加尿素也会产生微/中/大分子碳。在800°C时合成的材料具有约1800–3100 m 2 / g的大表面积。在750°C时,由富氮生物质合成的材料结合了2400–3050 m 2的超大表面积/ g和显着的N掺杂(2-3 wt%N)。纹理和化学特性的这种结合对于许多与能源相关的应用以及基于吸附的工艺都具有极大的吸引力。
更新日期:2017-08-01
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