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Enhanced one-pot selective conversion of cellulose to ethylene glycol over NaZSM-5 supported metal catalysts
New Journal of Chemistry ( IF 3.3 ) Pub Date : 2021-09-08 , DOI: 10.1039/d1nj03257g
Sreejith Sreekantan 1 , Arun Arunima Kirali 1 , Banu Marimuthu 1, 2
Affiliation  

The mesopores interconnected with microporous NaZSM-5 was synthesised by sol–gel method. Reactions involving cellulose using different bimetallic and trimetallic combinations of nickel, aluminium, and tungsten metals supported on NaZSM-5 have been carried out. Different weight percentages (wt%) of Al, Ni, and W were loaded onto the NaZSM-5 support via a wet impregnation method. The prepared catalysts were characterized using PXRD, FE-SEM, HR-TEM, BET, and XPS studies to investigate the presence of mesopores, the textural properties, the metal loading, and the active oxidation states. The catalytic activities of the xAl–yNi–zW/NaZSM-5 (where x, y, and z are the wt% values of Al, Ni, and W, respectively) supported catalysts were studied during the one-pot conversion of cellulose into ethylene glycol at 220 °C and with a pressure of 70 bar H2 (at the reaction temperature) in water (as a solvent). The 5%Al–8%Ni–25%W/NaZSM-5 catalyst exhibited the highest cellulose conversion of 100%, with an ethylene glycol yield as high as 89% (C mol%) under moderate reaction conditions being reported for the first time. Al3+ in the catalyst hydrolyzed cellulose, and W5+ species acted as acid centres that facilitated the retro-aldol condensation reaction and eventually led to an increased EG yield in the presence of Ni. The catalyst was moderately stable after four consecutive runs for 6 h at 220 °C and at a H2 reaction pressure of 70 bar, though a 12 h reaction resulted in the highest EG yield. The high yields under moderate reaction conditions promise an energy-efficient and economically feasible process.

中文翻译:

在 NaZSM-5 负载的金属催化剂上增强纤维素一锅法选择性转化为乙二醇

通过溶胶-凝胶法合成了与微孔 NaZSM-5 互连的介孔。已经进行了涉及使用负载在 NaZSM-5 上的镍、铝和钨金属的不同双金属和三金属组合的纤维素的反应。通过湿浸渍法将不同重量百分比 (wt%) 的 Al、Ni 和 W 负载到 NaZSM-5 载体。使用 PXRD、FE-SEM、HR-TEM、BET 和 XPS 研究对制备的催化剂进行表征,以研究介孔的存在、结构特性、金属负载和活性氧化态。所述的催化活性X AL- ý Ni基ž W / NaZSM-5(其中,Xÿ,和ž分别是 Al、Ni 和 W 的 wt% 值)在 220 °C 和 70 bar H 2压力(在反应温度下)将纤维素一锅法转化为乙二醇的过程中研究了负载型催化剂水(作为溶剂)。5%Al–8%Ni–25%W/NaZSM-5 催化剂表现出最高的纤维素转化率 100%,在中等反应条件下乙二醇收率高达 89%(C mol%),这是首次报道时间。催化剂中的Al 3+水解纤维素,W 5+物质充当酸中心,促进逆醇醛缩合反应,并最终导致在 Ni 存在下增加 EG 产率。在 220 °C 和 H 2连续运行 6 小时后,催化剂中等稳定。70 巴的反应压力,尽管 12 小时的反应导致最高的 EG 收率。在温和的反应条件下的高产率保证了一种节能且经济可行的工艺。
更新日期:2021-09-08
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