Co embedded within biomass-derived mesoporous N-doped carbon as an acid-resistant and chemoselective catalyst for transfer hydrodeoxygenation of biomass with formic acid,Green Chemistry

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Co embedded within biomass-derived mesoporous N-doped carbon as an acid-resistant and chemoselective catalyst for transfer hydrodeoxygenation of biomass with formic acid
Green Chemistry ( IF 9.3 ) Pub Date : 2017-10-26 00:00:00 , DOI: 10.1039/c7gc02648j
Huanhuan Yang _{1,

2,

3,

4,

5} , Renfeng Nie _{1,

2,

3,

4,

5} , Wang Xia _{1,

2,

3,

4,

5} , Xiaolong Yu _{1,

2,

3,

4,

5} , Dingfeng Jin _{6,

7,

8,

9} , Xinhuan Lu _{1,

2,

3,

4,

5} , Dan Zhou _{1,

2,

3,

4,

5} , Qinghua Xia _{1,

2,

3,

4,

5}

Affiliation

An N-doped Co@C catalyst (Co@NC) is synthesized by a one-pot carbonization of biomass-derived glucose and harmless melamine with CoCl₂ as the catalyst, where C and N resources could be transformed into highly graphitic N-doped carbon, while the coordinated Co²⁺ ions are reduced to uniform Co nanoparticles (NPs), which are embedded in N-doped graphitic structures. Under base-free conditions with formic acid (FA) as a hydrogen donor, the optimized Co@NC-700 (pyrolyzed at 700 °C) shows a highly efficient H₂ generation from FA and the best activity for vanillin hydrodeoxygenation (HDO) with FA. For example, Co@NC-700 exhibits 15.4 times higher activity in comparison with uncovered Co on AC (Co/AC), and affords >95% vanillin conversion with 2-methoxy-4-methylphenol (MMP) as the sole product at 180 °C for 4 h. Compared with molecular hydrogen, Co@NC-700 gives a much higher activity and MMP selectivity for vanillin HDO with FA. The Co@NC-700 demonstrates enhanced acid resistance in acidic medium and adsorption of vanillin, and is recyclable and versatile for hydrogenating various unsaturated compounds. The superior performance of Co@NC-700 could be ascribed to N-derived defective sites on Co@NC, which could play multiple roles as base additives in FA dehydrogenation and as a metal-like active center in vanillin HDO.

中文翻译：

嵌入生物质衍生的中孔氮掺杂碳中的钴作为耐酸和化学选择性催化剂，用于甲酸对生物质的转移加氢脱氧

通过生物质衍生的葡萄糖和无害三聚氰胺的一锅式碳化，以CoCl ₂为催化剂，合成了N掺杂的Co @ C催化剂（Co @ NC），其中C和N资源可以转化为高度石墨化的N掺杂碳，同时将配位的Co ²⁺离子还原为均匀的Co纳米颗粒（NPs），将其嵌入N掺杂的石墨结构中。在以甲酸（FA）为氢供体的无碱条件下，优化的Co @ NC-700（在700°C下热解）显示出高效的H ₂由FA生成，并且具有FA的香草醛加氢脱氧（HDO）的最佳活性。例如，Co @ NC-700的活性比未发现的Co上的Co（Co / AC）高出15.4倍，并且在180°C时以2-甲氧基-4-甲基苯酚（MMP）作为唯一产品提供了> 95％的香兰素转化率保持4小时。与分子氢相比，Co @ NC-700对带有FA的香兰素HDO具有更高的活性和MMP选择性。Co @ NC-700在酸性介质中显示出增强的耐酸性，并吸附了香兰素，并且可回收利用，具有多种氢化各种不饱和化合物的用途。Co @ NC-700的优异性能可归因于Co @ NC上N衍生的缺陷位点，这些位点在FA脱氢中作为基础添加剂以及在香兰素HDO中作为金属样活性中心发挥着多种作用。

更新日期：2017-11-10

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