Catalytic activity of metal‐free amine‐modified dextran microgels in hydrogen release through methanolysis of NaBH4,International Journal of Energy Research

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Catalytic activity of metal‐free amine‐modified dextran microgels in hydrogen release through methanolysis of NaBH4
International Journal of Energy Research ( IF 4.3 ) Pub Date : 2020-03-27 , DOI: 10.1002/er.5395
Erk Inger ₁ , Aydin K. Sunol ₂ , Nurettin Sahiner _{2,

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Affiliation

Polymeric microgels were prepared from dextran (Dex) by crosslinking linear natural polymer dextran with divinyl sulfone (DVS) with a surfactant‐free emulsion technique resulting in high gravimetric yield of 78.5 ± 5.3% with wide size distribution. Dex microgels were chemically modified, and then used as catalyst in the methanolysis of NaBH₄ to produce H₂. The chemical modification of Dex microgel was done on epichlorohydrin (ECH)‐reacted Dex microgels with ethylenediamine (EDA), diethylenetriamine (DETA), and triethylenetetraamine (TETA) in dimethylformamide (DMF) at 90°C for 12 hours. The modified dextran‐TETA microgels were protonated using treatment with hydrochloric acid (HCl) and m‐Dex microgels‐TETA‐HCl was found to be a very efficient catalyst for methanolysis of NaBH₄ to produce H₂. The effects of reaction temperature and NaBH₄ concentration on H₂ generation rates were investigated and m‐Dex microgels‐TETA‐HCl catalyst possessed excellent catalytic performances with 100% conversion and 80% activity at end of 10 consecutive uses and was highly re‐generatable with simple HCl treatment. Interestingly, m‐Dex microgels‐TETA‐HCl catalyst can catalyze NaBH₄ methanolysis reaction in a mild temperature range 0 to 35°C with E_a value of 30.72 kJ/mol and in subzero temperature range, −20 to 0°C with E_a value of 32.87 kJ/mol, which is comparable with many catalysts reported in the literature.

中文翻译：

无金属胺修饰的右旋糖酐微凝胶通过NaBH4甲醇解氢释放氢的催化活性

聚合物微凝胶是由葡聚糖（Dex）通过将线性天然聚合物葡聚糖与二乙烯基砜（DVS）交联并采用无表面活性剂的乳液技术制备的，从而获得了78.5±5.3％的高重量产率，且粒径分布宽。将葡聚糖微凝胶进行化学修饰，然后将其用作NaBH ₄甲醇解生成H _2的催化剂。在表氯醇（ECH）反应的Dex微凝胶上，用乙二胺（EDA），二亚乙基三胺（DETA）和三亚乙基四胺（TETA）在二甲基甲酰胺（DMF）中于90°C进行12小时的化学修饰。使用盐酸（HCl）处理改性的葡聚糖-TETA微凝胶，发现m-Dex微凝胶-TETA-HCl是NaBH甲醇分解的非常有效的催化剂₄产生H ₂。研究了反应温度和NaBH ₄浓度对H ₂生成速率的影响，并且m-Dex微凝胶-TETA-HCl催化剂具有出色的催化性能，在连续10次使用结束时转化率为100％，活性为80％，并且可高度再生用简单的HCl处理。有趣的是，M-塞米松微凝胶-TETA盐酸催化剂可以催化的NaBH _4个在温和的温度范围为0〜35℃用甲醇分解反应Ë_一个具有30.72千焦/摩尔和在零度以下的温度范围内，-20℃至0℃下的值ê_该值是32.87kJ / mol，与文献中报道的许多催化剂相当。

更新日期：2020-03-27

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