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Influence of Brønsted and Lewis acidity of the modified Al-MCM-41 solid acid on cellulose conversion and 5-hydroxylmethylfurfuran selectivity
Chemosphere ( IF 8.8 ) Pub Date : 2020-11-23 , DOI: 10.1016/j.chemosphere.2020.129062
Son Tung Pham , Manh B. Nguyen , Giang H. Le , Trinh Duy Nguyen , Chinh D. Pham , Thanh Son Le , Tuan A. Vu

The modified Al-MCM-41 solid acids with turning Si/Al molar ratio were successfully fabricated through a hydrothermal route and utilized as a suitable catalyst in the cellulose conversion into 5-hydroxylmethylfurfural (5-HMF). The crystal structure, composition, morphologies and porosity of as-synthesized acids were characterized by XRD, FT-IR, N2 adsorption-desorption, TEM and EDS. The 27Al MAS NMR and 29Si-MAS NMR results revealed the existence of both Al framework and Al extra framework. Besides, the existence of medium-weak and strong acid sites, according to Brønsted and Lewis acidity, in Al-MCM-41 acids was confirmed by NH3-TPD and FTIR-pyridine adsorption. The 30Al-MCM-41 solid acid (Si/Al molar ratio = 30) exhibited excellent activity with the highest 5-HMF yield of 40.56% compared to other samples. We also discovered that 5-HMF production, as well as cellulose conversion, strongly depended on the total acid, strong/medium-weak acid ratio, as well as Brønsted/Lewis acid ratio. Therefore, these parameters have been considered as essential factors for the design of solid acid for 5-HMF production.



中文翻译:

改性Al-MCM-41固体酸的布朗斯台德和路易斯酸度对纤维素转化率和5-羟甲基呋喃选择性的影响

通过水热法成功制备了具有Si / Al摩尔比变化的Al-MCM-41固体酸,并将其用作纤维素转化为5-羟甲基糠醛(5-HMF)的合适催化剂。用XRD,FT-IR,N 2吸附-脱附,TEM和EDS对合成后的酸的晶体结构,组成,形貌和孔隙率进行了表征。在27的Al MAS NMR和29的Si-MAS NMR结果显示两者Al骨架和Al骨架外的存在。此外,根据NH 3证实,根据Brønsted和Lewis酸度,在Al-MCM-41酸中存在中弱和强酸位点-TPD和FTIR-吡啶吸附。与其他样品相比,30Al-MCM-41固体酸(Si / Al摩尔比= 30)表现出出色的活性,最高5-HMF收率为40.56%。我们还发现5-HMF的产生以及纤维素的转化率在很大程度上取决于总酸,强酸/中弱酸比率以及布朗斯台德/路易斯酸比率。因此,这些参数已被认为是设计5-HMF生产固体酸的必要因素。

更新日期:2020-11-23
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