A solvent-free, one-step synthesis of sulfonic acid group-functionalized mesoporous organosilica with ultra-high acid concentrations and excellent catalytic activities,Green Chemistry

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A solvent-free, one-step synthesis of sulfonic acid group-functionalized mesoporous organosilica with ultra-high acid concentrations and excellent catalytic activities
Green Chemistry ( IF 9.3 ) Pub Date : 2018-01-23 00:00:00 , DOI: 10.1039/c8gc00002f
Qin Wu _{1,

2,

3,

4,

5} , Fujian Liu _{1,

2,

3,

4,

5} , Xianfeng Yi _{6,

7,

8,

9,

10} , Yongcun Zou _{11,

12,

13,

14,

15} , Lilong Jiang _{1,

2,

3,

4,

5}

Affiliation

National Engineering Research Center of Chemical Fertilizer Catalyst (NERC-CFC)
School of Chemical Engineering
Fuzhou University
Fuzhou 350002
PR China
State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics
National Center for Magnetic Resonance in Wuhan
Key Laboratory of Magnetic Resonance in Biological Systems
Wuhan Institute of Physics and Mathematics
Chinese Academy of Sciences
State Key Laboratory of Inorganic Synthesis & Preparative Chemistry
Department of Chemistry
Jilin University
Changchun 130012
China

We demonstrate herein a novel solvent-free technique for the synthesis of sulfonic acid group-functionalized mesoporous organosilica, which was achieved from the self-assembly of a block copolymer template using mercaptopropyltrimethoxysilane (MPTS) and tetramethoxysilane (TMOS) under melting conditions without using additional solvents and subsequent condensation at high temperature (up to 140 °C). The resultant samples were designated as SMS-xs, where x stands for molar ratio of MPTS/(MPTS + TMOS). SMS-xs have relatively large BET surface areas, highly cross-linked frameworks, and abundant and uniform mesopores with wormhole-like characteristics. Interestingly, MPTS could be used as the solo precursor to prepare mesoporous organosilica (SMS-1.0), which had controllable acidity and an ultra-high concentration of sulfur (5.51 mmol g⁻¹, the highest acid density to date), which was even higher than those of commercial Amberlyst 15 (4.7 mmol g⁻¹), HS-JLU-20-0.8 (4.61 mmol g⁻¹) and sulfonated carbon (CH_0.30O_0.33S_0.16, 4.90 mmol g⁻¹). These structural characteristics give SMS-xs excellent activities and good reusability in biomass conversions and fine chemicals synthesis, which are much better than various solid acids, such as Amberlyst 15, H-form USY zeolite, and sulfonic acid group-functionalized ordered mesoporous silica.

中文翻译：

一种无溶剂的一步法合成磺酸基官能化的介孔有机二氧化硅，具有超高的酸浓度和出色的催化活性

我们在本文中演示了用于合成磺酸基团官能化介孔有机二氧化硅的新型无溶剂技术，该技术是通过在熔融条件下使用巯基丙基三甲氧基硅烷（MPTS）和四甲氧基硅烷（TMOS）自组装嵌段共聚物模板而实现的，而无需使用其他方法溶剂，然后在高温（最高140°C）下凝结。所得样品命名为SMS- x s，其中x代表MPTS /（MPTS + TMOS）的摩尔比。SMS- X具有较大的BET表面积，高度交联的骨架，并具有蠕虫样特征的丰富且均匀的中孔。有趣的是，MPTS可以用作制备有机介孔有机硅（SMS-1.0）的单独前体，该介孔有机酸具有可控的酸度和超高浓度的硫（5.51 mmol g ^-1，迄今为止最高的酸密度），甚至是比市售的Amberlyst 15（4.7毫摩尔克更高^-1），HS-JLU-20-0.8（4.61毫摩尔克^-1）和磺化碳（CH _0.30 ö _0.33 š _0.16，4.90毫摩尔克^-1）。这些结构特征使SMS- x在生物质转化和精细化学品合成中具有出色的活性和良好的可重用性，这比各种固体酸（例如Amberlyst 15，H型USY沸石和磺酸基官能化的有序介孔二氧化硅）要好得多。

更新日期：2018-03-06

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