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摘要
利用NH4Y分子筛与铜源间的固相反应制备CuY催化剂,选用5种铜源调控CuY的织构特点及催化剂上铜物种的化学状态,并考察了CuY在甲醇氧化羰基化合成碳酸二甲酯过程中的催化性能。利用XRD、H2-TPR和NH3-TPD等表征手段对CuY进行分析。结果表明,以Cu(NO3)2为铜源制备得到的CuY-N上,碳酸二甲酯的时空收率(STYDMC)为137.4 mg/(g·h);以CuCl2为铜源制备的CuY-C上无CuOx物种,其催化活性比CuY-N差;以Cu(COOCH3)2为铜源制备得到的CuY-AC催化活性更差;以CuSO4为铜源制备的CuY-S几乎没有催化活性;而以Cu(acac)2为铜源制备的CuY-acac活性最佳,STYDMC达到267.3 mg/(g·h)。
Abstract
CuY catalysts are prepared by means of solid state reaction between NH4Y molecular sieve and copper resource.Five different copper resources are applied to adjust the textural properties and chemical states of copper species on CuY catalysts.The catalytic performance of CuY catalysts is investigated in synthesis of dimethyl carbonate through oxidative carbonylation of methanol.To obtain a deep understanding of their structure-performance relationship,XRD,H2-TPR and NH3-TPD are employed to characterize CuY catalysts.Experimental results indicate that space-time yield of dimethyl carbonate is 137.4 mg·g-1·h-1 over CuY-N catalyst from Cu(NO3)2.There are no CuOx aggregation on CuY-C catalyst from CuCl2,and CuY-C catalyst has a poorer activity than CuY-N catalyst.CuY-AC catalyst from Cu(COOCH3)2 shows a worse activity.CuY catalyst from CuSO4 has hardly any catalytic activity.CuY-acac catalyst from Cu(acac)2 shows the best catalytic activity,which can lead to a 267.3 mg·g-1·h-1 of space-time yield for dimethyl carbonate.
关键词
固相反应
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铜源
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甲醇氧化羰基化
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碳酸二甲酯
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CuY催化剂
Key words
solid state reaction
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copper resource
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oxidative carbonylation of methanol
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dimethyl carbonate
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CuY catalyst
铜源阴离子对CuY催化剂性能的影响[J].
现代化工, 2021, 41(5): 163-167 DOI:10.16606/j.cnki.issn0253-4320.2021.05.033