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Au促进Pt/WO_3催化甘油氢解制1,3-丙二醇(英文) 被引量:5
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作者 杨超军 张帆 +6 位作者 雷念 杨曼 刘菲 苗治理 孙永南 赵晓晨 王爱琴 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第8期1366-1372,共7页
近年来,以生物质为基础的生物柴油得到了迅速发展,导致了粗甘油过剩.通过甘油选择性氢解制1,3-丙二醇,进而被用于合成高价值的聚对苯二甲酸丙二醇酯被认为是最具工业应用潜力的反应之一,对于提高生物柴油的利用效率有着极其重要的意义.... 近年来,以生物质为基础的生物柴油得到了迅速发展,导致了粗甘油过剩.通过甘油选择性氢解制1,3-丙二醇,进而被用于合成高价值的聚对苯二甲酸丙二醇酯被认为是最具工业应用潜力的反应之一,对于提高生物柴油的利用效率有着极其重要的意义.但由于反应空间位阻和热力学上的限制给甘油氢解制1,3-丙二醇带来了很大的挑战,因此需要设计高活性的金属-酸双功能催化剂以降低甘油第二个C-O键断裂的活化能和减少其他副反应的发生.目前Pt-W和Ir-Re双功能催化剂可高选择性制得1,3-丙二醇,但仍需较严苛的反应条件实现对氢气的活化和解离.本课题组曾将准单原子/单原子Pt高度分散于具有大量氧空位和酸位点的WO_x载体上,十分有利于甘油选择性氢解制1,3-丙二醇反应;在Au-Pt/WO_x催化剂中添加Au可促进B酸产生,进而提高了甘油转化率和1,3-丙二醇的选择性.为了进一步研究Au对Pt/WO_x催化剂结构和催化性能的影响,本文利用CTAB辅助吸附法制备了Au/WO_3,再浸渍Pt制得Pt/Au/WO_3双金属催化剂.在甘油选择性氢解制1,3-丙二醇反应中,所制催化剂表现出比Au-Pt/WO_x更好的催化活性,1,3-丙二醇时空收率为0.078 g_(1,3-PDO)/(g_(cat)·h),是后者的1.95倍.值得一提的是,Au-Pt/WO_x催化剂在低压时活性较高,而Pt/Au/WO_3催化剂活性则在压力的升高而提高;另外反应温度的升高导致副产物正丙醇的选择性上升,1,3-丙二醇的选择性降低.因此,适宜的反应条件为155 ℃和5 MPa.与Pt/WO_3和Pt/WO_x相比,Pt/Au/WO_3表现出了更优异的催化性能,其1,3-丙二醇的时空收率是Pt/WO_3的2.36倍和Pt/WO_x的4倍.为了探究Au的掺入对Pt/WO_x催化剂性能的影响,通过XRD,TEM,H_2-TPR和XPS等技术对催化剂进行了深入表征.结果表明,与Pt/WO_3相比,Pt/Au/WO_3-600催化剂的XRD衍射峰向小角度偏移,其原因是Au3+离子半径(0.85?比W6+的(0.60?大,Au^(3+)以取代晶格W^(6+)形式进入WO_3晶格中;对H_2-TPR前300 ℃耗氢量的计算可知:Pt/WO_3可被还原至Pt/WO_2.96,而Pt/Au/WO_3可被还原至Pt/Au/WO_2.91.因此与Pt/WO_3相比,Pt/Au/WO_3表面氧空位更加丰富.TEM和XPS表征可知,添加0.1wt%Au后,促进了更低价态的Pt均匀分散在WO_3载体上,其平均粒径为2.36 nm.综上所述,Au的掺杂改变了Pt/Au/WO_3双金属催化剂的结构,不仅降低了Pt和W的还原温度,削弱了Pt和W之间的相互作用,也促进了更低价态的Pt均匀分散于WO_3载体上,使得Pt/Au/WO_3双金属催化剂在甘油氢解制1,3-丙二醇反应中具有更为优异的活性和产物选择性.该催化剂有望被广泛运用于其他生物质平台化合物加氢脱氧的反应中. 展开更多
关键词 双金属 Pt/Au/WO3 甘油 1 3-丙二醇 氢解作用
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Violation of Leggett–Garg Inequalities in Single Quantum Dots
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作者 孙永南 邹扬 +2 位作者 葛荣春 唐建顺 李传锋 《Chinese Physics Letters》 SCIE CAS CSCD 2012年第12期13-16,共4页
We investigate the violation of two types of Leggett-Garg(LG)inequalities in self-assembled quantum dots under the stationarity assumption.By comparing the two types of LG inequalities,we find the better one that is e... We investigate the violation of two types of Leggett-Garg(LG)inequalities in self-assembled quantum dots under the stationarity assumption.By comparing the two types of LG inequalities,we find the better one that is easier to be tested in an experiment.In addition,we show that the fine-structure splitting,background noise and temperature of quantum dots greatly affect the violation of LG inequalities. 展开更多
关键词 experiment. QUANTUM SPLITTING
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On Delay of the Delayed Choice Experiment
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作者 孙君 孙永南 +1 位作者 李传锋 郭光灿 《Chinese Physics Letters》 SCIE CAS CSCD 2015年第9期5-8,共4页
Following a suggestion by Wheeler, several delayed choice experiments have been performed. However, in those experiments one fact has always been ignored: that due to the fact that the single photon is nonlocal in ti... Following a suggestion by Wheeler, several delayed choice experiments have been performed. However, in those experiments one fact has always been ignored: that due to the fact that the single photon is nonlocal in time, the outcome will change if one changes the time to switch the experimental configuration within the photon's wavepaeket. This study obtains some insights into this aspect by proposing an experimental scheme based on the delayed choice experiment and giving some related analysis. The result shows a transitional behavior from a particle to a wave, leading to a conclusion that the measuring operator could be time dependent and be changed in a single measurement. 展开更多
关键词 On Delay of the Delayed Choice Experiment
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