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黑荆树单宁稳定钯纳米胶体催化水有机两相苯甲醇氧化反应

Aqueous-Organic Biphasic Oxidation of Benzyl Alcohol Catalyzed by Palladium Nano-colloid Stabilized by Black Wattle Tannin
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摘要 催化氧化苯甲醇是制备苯甲醛的一种简便高效的方法.以天然高分子黑荆树单宁(BWT)为两亲性稳定剂,制备水溶性钯纳米胶体催化剂,用于苯甲醇的氧化反应.采用透射电镜(TEM)、傅里叶变换红外光谱(FT-IR)等表征手段表征所制备催化剂的形貌,探讨制备条件对催化剂形貌的影响.TEM测试表明,单宁的用量对胶体中钯纳米粒子的粒径具有显著的影响,随着BWT用量从2 mg增加到60 mg,Pd粒子的粒径呈现减小趋势.FT-IR测试表明,BWT通过其结构中大量的酚羟基对Pd纳米粒子进行稳定和分散.系统考察单宁用量、反应温度、反应时间等因素对Pd纳米胶体在苯甲醇氧化反应中活性的影响,结果表明:当BWT用量为15 mg时制备的BWT15 mg-Pd胶体催化剂在50℃,空气气氛下8 h催化苯甲醇的转化率高达98.58%; BWT用量对催化剂重复使用性能也有显著的影响,BWT15 mg-Pd可以重复使用5次转化率仍然在90%以上,明显优于BWT5 mg-Pd和BWT60 mg-Pd. Catalytic oxidation of benzyl alcohol is an efficient synthesis method of benzaldehyde.In this paper,black wattle tannin(BWT)was used as amphiphilic stabilizer to prepare water soluble palladium nanocolloid catalyst for oxidation of benzyl alcohol.The morphology of the catalyst was characterized by Transmission Electron Microscopy(TEM)and Fourier Transform infrared spectrometer(FTIR).The influence of preparation conditions on the morphology of the catalyst was discussed.TEM images showed that the particle size decreased with the increase of the amount of BWT from 2 mg to 60 mg.BWT amount had a significant effect on the size of palladium nanoparticles in the colloid.FTIR results indicated that the Pd nanoparticles were stabilized and dispersed through a large number of phenolic hydroxyl groups in BWT structure.The effects of BWT amount,reaction temperature and time on the activity of asprepared Pd nanoparticles in benzyl alcohol oxidation were investigated.When the BWT amount was 15 mg,the conversion rate was up to 98.58%when the BWT-Pd colloid catalyst was used as catalyst at 50℃in air for 8 hours.The amount of BWT also had a significant effect on the reusability of the catalyst.The conversion rate of BWT15 mgPd was above 90%after 5 cycles,which was obviously superior to that of BWT5 mgPd and BWT60 mgPd.
作者 邱云飞 王毓嘉 肖萌 郝柏村 马骏 廖洋 尚鸿燕 毛卉 QIU Yunfei;WANG Yujia;XIAO Meng;HAO Baicun;MA Jun;LIAO Yang;SHANG Hongyan;MAO Hui(College of Chemistry and Materials Science,Sichuan Normal University,Chengdu 610066,Sichuan;Key Laboratory of Land Resources Evaluation and Monitoring in Southwest,Sichuan Normal University,Chengdu 610066,Sichuan)
出处 《四川师范大学学报(自然科学版)》 CAS 北大核心 2018年第6期807-812,共6页 Journal of Sichuan Normal University(Natural Science)
基金 国家自然科学基金(21506134和21776188) 四川省科技支撑项目(2016NZ0053)
关键词 黑荆树单宁 Pd纳米胶体 醇氧化 重复使用性 black wattle tannin Pd palladium nanocolloid alcohol oxidation reusability
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