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纳米级介孔磷酸锡氧化物作为一种高效的固体酸催化剂。

Nano-sized mesoporous phosphated tin oxide as an efficient solid acid catalyst.

作者信息

Hassan S M, Mannaa M A, Ibrahim Amr Awad

机构信息

Chemistry Department, Faculty of Science, Mansoura University Mansoura Egypt

Chemistry Department, Faculty of Education and Science, Amran University Sa'dah Yemen.

出版信息

RSC Adv. 2019 Jan 8;9(2):810-818. doi: 10.1039/c8ra08962k. eCollection 2019 Jan 2.

Abstract

Herein, we prepared a mesoporous tin oxide catalyst (mSnO) activated with phosphate species by the adsorption of phosphate ions from a phosphoric acid solution onto tin oxyhydroxide (Sn(OH)) surface. The phosphate content ranged from 3 to 45 wt%. The nonaqueous titration of -butylamine in acetonitrile was used to determine the total surface acidity level. FTIR of chemically adsorbed pyridine was used to differentiate between the Lewis and Brönsted acid sites. Thermal and X-ray diffraction analysis indicated that the addition of phosphate groups stabilized the mesostructure of mSnO and enabled it to keep its crystalline size at the nanoscale. FTIR analysis indicated the polymerization of the HPO groups into PO , which in turn reacts with SnO to form a SnPO layer, which stabilizes the mesoporous structure of SnO. The acidity measurements showed that the phosphate species are distributed homogeneously over the mSnO surface until surface saturation coverage at 25 wt% PO , at which point the acid strength and surface acidity level are maximized. The catalytic activity was tested for the synthesis of hydroquinone diacetate, where it was found that the % yield of hydroquinone diacetate compound increased gradually with the increase in PO loading on mSnO until it reached a maximum value of 93.2% for the 25% PO /mSnO catalyst with 100% selectivity and excellent reusability for three consecutive runs with no loss in activity.

摘要

在此,我们通过将磷酸溶液中的磷酸根离子吸附到氢氧化锡(Sn(OH))表面,制备了一种用磷物种活化的介孔氧化锡催化剂(mSnO)。磷含量范围为3至45 wt%。采用乙腈中仲丁胺的非水滴定法来测定总表面酸度水平。用化学吸附吡啶的傅里叶变换红外光谱(FTIR)来区分路易斯酸位点和布朗斯特酸位点。热分析和X射线衍射分析表明,磷酸基团的加入稳定了mSnO的介孔结构,并使其晶体尺寸保持在纳米级。FTIR分析表明HPO基团聚合成PO,进而与SnO反应形成SnPO层,这稳定了SnO的介孔结构。酸度测量表明,磷物种在mSnO表面均匀分布,直至PO含量为25 wt%时达到表面饱和覆盖,此时酸强度和表面酸度水平达到最大值。测试了对苯二酚二乙酸酯合成的催化活性,结果发现,对苯二酚二乙酸酯化合物的产率百分比随着mSnO上PO负载量的增加而逐渐增加,对于25% PO/mSnO催化剂,产率最高达到93.2%,选择性为100%,并且具有优异的可重复使用性,连续运行三次活性无损失。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/80b8/9059524/9ecbda888e9c/c8ra08962k-f1.jpg

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