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化学工业与工程
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��ѧ��ҵ�빤�� 2009, Vol. 26 Issue (1) :44-49    DOI:
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In-situ Infrared Study on Direct Synthesis of Diethyl Carbonate from Ethanol and CO_2
CAO Xin-yuan,WANG Wei,MA Xin-bin(Key Laboratory for Green Chemical Technology,School of Chemical Engineering and Technology,Tianjin University,Tianjin 300072,China)
(Key Laboratory for Green Chemical Technology,School of Chemical Engineering and Technology,Tianjin University,Tianjin 300072,China

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ժҪ ����ԭλ������Ҵ��Ͷ�����̼������ﯴ߻������ºϳ�̼�������(DEC)�ķ�Ӧ����������о����Ҵ��ǻ��ϵ���ԭ��������ﯱ����Zr4+�໥����,������ﯱ����������ǻ���Ӧ�γ�����������(����λ��Ͷ���λ��������)��ˮ,������̼��Ҫ�뵥��λ���������������뷴Ӧ�γ��һ�̼���;������̼������ﯱ��浥������ʱ�γ�̼�����κ�̼����,�Ҵ������������̼�����κ�̼���ξ��ɷ�Ӧ�γ��м������һ�̼���,��������̬�Ķ�����̼��ȷ�Ӧ����,�Ҵ��������̼��Ӧ��Ҫ������̬��CO2���뷴Ӧ��ʽ���С�����һ�̼������Ҵ�������ﯱ��淴Ӧ�γ��ǻ���̼���������
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Abstract�� In-situ infrared spectroscopy has been used to investigate the mechanism of diethyl carbonate(DEC) synthesis from ethanol and carbon dioxide.The atom O of ethanol coordinates with unsaturated Zr~(4+) cations presenting at the catalyst surface to form two kinds of ethoxide(monodentate and bidentate) and simultaneously proton is released,which reacts with hydroxyl group on the ZrO_2 surface to produce water.Dissociative carbon dioxide inserts into the(Zr��O) to form ethyl carbonate group((Zr��OC(O))CH_2CH_3)) as a mediate species,carbon dioxide adsorbs on the ZrO_2 catalyst as carbonate and bicarbonate species,both of which can react with ethanol to form(Zr��OC(O))CH_2CH_3).Compared with reaction of dissociative carbon dioxide,this process is slower.DEC is formed by reaction of the ethyl carbonate species with ethanol on the surface of ZrO_2.
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Received 2009-01-15; published 2009-01-15
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����ԭ;����;���±�;.�Ҵ���CO_2ֱ�Ӻϳ�̼���������ԭλ�����о�[J].  ��ѧ��ҵ�빤��, 2009,26(1): 44-49
CAO Xin-yuan,WANG Wei,MA Xin-bin.In-situ Infrared Study on Direct Synthesis of Diethyl Carbonate from Ethanol and CO_2[J].  Chemcial Industry and Engineering, 2009,26(1): 44-49
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