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甲基硅烷化改性显著促进乙烯在Pt/SBA-15上的低温催化氧化
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作者 范雅轩 赵谦 郑寿荣 《环境化学》 CAS CSCD 北大核心 2024年第11期3798-3805,共8页
以介孔分子筛SBA-15为载体,采用浸渍法制备Pt基催化剂,通过三甲基氯硅烷(TMCS)对催化剂进行表面改性以提高其疏水性.表征结果表明甲基硅烷化显著促进了催化剂的表面疏水性.乙烯的低温催化氧化结果显示,随着TMCS接枝量的增加,催化剂的反... 以介孔分子筛SBA-15为载体,采用浸渍法制备Pt基催化剂,通过三甲基氯硅烷(TMCS)对催化剂进行表面改性以提高其疏水性.表征结果表明甲基硅烷化显著促进了催化剂的表面疏水性.乙烯的低温催化氧化结果显示,随着TMCS接枝量的增加,催化剂的反应活性呈现火山型变化规律.Pt/SBA-15-TMCS(1:6)的催化活性最高,能够保持约1 h对痕量乙烯100%的催化氧化效果,3 h后仍有29%的乙烯转化率,相比于Pt/SBA-15有显著提升.适量TMCS的改性带来的催化剂疏水性的改善能够有效抑制反应过程中水分子吸附对催化剂的不利影响,而过量TMCS的修饰则易团聚形成大颗粒堵塞介孔孔道,减少乙烯分子与活性位点的接触,降低催化效果. 展开更多
关键词 低温催化氧化 乙烯 pt/sba-15 表面改性
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添加Sm对Pt/SBA-15催化苯完全氧化反应活性和热稳定性的影响 被引量:1
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作者 毛建新 袁子卿 +1 位作者 严红绡 周仁贤 《化工学报》 EI CAS CSCD 北大核心 2020年第1期306-313,共8页
以Pt/SBA-15为催化剂,考察催化剂载体中添加Sm对于苯的完全氧化反应活性和热稳定性影响。采用了一种简便的记录起燃温度曲线和催化剂热稳定性评价方法,即向装载好催化剂的固定床反应器中持续通入恒定流量的反应气,逐步阶段性升高反应温... 以Pt/SBA-15为催化剂,考察催化剂载体中添加Sm对于苯的完全氧化反应活性和热稳定性影响。采用了一种简便的记录起燃温度曲线和催化剂热稳定性评价方法,即向装载好催化剂的固定床反应器中持续通入恒定流量的反应气,逐步阶段性升高反应温度,同时在线检测出口尾气的浓度变化,得到起燃温度曲线后,继续提高反应温度,然后恒定在某一设定的温度(如550℃)持续运行较长时间,期间定时在线取样分析,如果有必要还可以连续考察降温情况下催化剂的反应活性情况。研究结果表明,几种催化剂低温活性次序为:Pt/SBA-15≈Pt/4%Sm2O3/SBA-15>Pt/Sm2O3>4%Sm2O3/SBA-15,而对于高温稳定性则是Pt/4%Sm2O3/SBA-15>Pt/1.2%Sm2O3/SBA-15>Pt/SBA-15,Pt/Sm-SBA-15(SG)>Pt/SBA-15(SG)。总之,Sm的添加虽然未能提高Pt/SBA-15的低温催化活性,但是能明显提高催化剂在高温情况下活性的稳定性。1%Pt/4%Sm2O3/SBA-15同时具备较好的低温催化活性和高温稳定性,具有较好的应用前景。 展开更多
关键词 SM2O3 pt/sba-15 催化 完全氧化 热稳定性
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Characterization and performance of Pt/SBA-15 for low-temperature SCR of NO by C_3H_6 被引量:5
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作者 Xinyong Liu Zhi Jiang +3 位作者 Mingxia Chen Jianwei Shi Wenfeng Shangguan Yasutake Teraoka 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2013年第5期1023-1033,共11页
Pt supported on mesoporous silica SBA-15 was investigated as a catalyst for low temperature selective catalytic reduction(SCR) of NO by C 3 H 6 in the presence of excess oxygen.The prepared catalysts were characteri... Pt supported on mesoporous silica SBA-15 was investigated as a catalyst for low temperature selective catalytic reduction(SCR) of NO by C 3 H 6 in the presence of excess oxygen.The prepared catalysts were characterized by means of XRD,BET surface area,TEM,NO-TPD,NO/C 3 H 6-TPO,NH 3-TPD,XPS and 27 Al MAS NMR.The effects of Pt loading amount,O 2 /C 3 H 6 concentration,and incorporation of Al into SBA-15 have been studied.It was found that the removal efficiency increased significantly after Pt loading,but an optimal loading amount was observed.In particular,under an atmosphere of 150 ppm NO,150 ppm C 3 H 6,and 18 vol.% O 2,0.5% Pt/SBA-15 showed remarkably high catalytic performance giving 80.1% NOx reduction and 87.04% C 3 H 6 conversion simultaneously at 140°C.The enhanced SCR activity of Pt/SBA-15 is associated with its outstanding oxidation activities of NO to NO 2 and C 3 H 6 to CO 2 in low temperature range.The research results also suggested that higher concentration of O 2 and higher concentration of C 3 H 6 favored NO removal.The incorporation of Al into SBA-15 improved catalytic performance,which could be ascribed to the enhancement of catalyst surface acidity caused by tetrahedrally coordinated AlO 4.Moreover,the catalysts could be easily reused and possessed good stability. 展开更多
关键词 LOW-TEMPERATURE selective catalytic reduction C 3 H 6 pt/sba-15
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Pt/CeO_2/SBA-15催化剂上Pt-CeO_2接触界面的相互作用
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作者 毕亚东 张微 +1 位作者 徐恒泳 李文钊 《高等学校化学学报》 SCIE EI CAS CSCD 北大核心 2009年第10期2032-2035,共4页
通过沉积沉淀法(Deposition precipitation,DP)将CeO2纳米粒子高度分散在SBA-15分子筛上,进一步采用浸渍法负载Pt后制备了Pt/CeO2/SBA-DP催化剂.紫外-可见漫反射光谱分析表明,在Pt/CeO2/SBA-DP催化剂上可以形成更多的Pt-CeO2接触界面,... 通过沉积沉淀法(Deposition precipitation,DP)将CeO2纳米粒子高度分散在SBA-15分子筛上,进一步采用浸渍法负载Pt后制备了Pt/CeO2/SBA-DP催化剂.紫外-可见漫反射光谱分析表明,在Pt/CeO2/SBA-DP催化剂上可以形成更多的Pt-CeO2接触界面,有利于从CeO2到Pt的电子转移过程.CO程序升温还原(CO-TPR)测试证实,Pt/CeO/SBA-DP催化剂上CeO表面氧物种具有较高的还原能力. 展开更多
关键词 氧化铈 sba-15分子筛 紫外-可见漫反射光谱 CO程序升温还原
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短孔道Pt/W-s-SBA-15催化剂的合成及甘油催化氢解制1,3-丙二醇性能的研究 被引量:10
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作者 成诗婕 曾杨 +3 位作者 裴燕 范康年 乔明华 宗保宁 《化学学报》 SCIE CAS CSCD 北大核心 2019年第10期1054-1062,共9页
合成了孔道平行于短轴方向的W原位掺杂的介孔SBA-15分子筛(W-s-SBA-15),以其为载体制备了Pt/W-s-SBA-15催化剂,考察了催化剂中Pt、W负载量变化对甘油氢解制1,3-丙二醇(1,3-PDO)性能的影响.采用多种手段对催化剂的形貌、活性组分Pt和W的... 合成了孔道平行于短轴方向的W原位掺杂的介孔SBA-15分子筛(W-s-SBA-15),以其为载体制备了Pt/W-s-SBA-15催化剂,考察了催化剂中Pt、W负载量变化对甘油氢解制1,3-丙二醇(1,3-PDO)性能的影响.采用多种手段对催化剂的形貌、活性组分Pt和W的存在状态、催化剂的酸性等性质进行了系统的表征.催化剂评价结果表明,随着Pt、W负载量的增加,甘油的总转化率和液相转化率(CTL)提高,而1,3-PDO选择性呈先升高后降低的火山型变化趋势.在Pt负载量为4.0 wt%、W/Si物质的量比为1/480的4Pt/W-s-SBA-15(1/480)催化剂上,在433 K、H2压力4.0 MPa、反应时间24h的条件下,甘油氢解制1,3-PDO的得率可达49.0%.根据表征结果,我们发现在Pt/W-s-SBA-15催化剂上的甘油转化率与Pt活性比表面积直接相关,而小的Pt粒径、Pt与单分散WO4之间密切的协同作用,则有助于提高1,3-PDO的选择性. 展开更多
关键词 短孔道W-sba-15 甘油氢解 1 3-丙二醇
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Effect of aluminum modification on catalytic properties of PtSn-based catalysts supported on SBA-15 for propane dehydrogenation 被引量:6
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作者 Yongzheng Duan Yuming Zhou +3 位作者 Yiwei Zhang Xiaoli Sheng Shijian Zhou Zewu Zhang 《Journal of Natural Gas Chemistry》 EI CAS CSCD 2012年第2期207-214,共8页
The catalytic properties of PtSn-based catalysts supported on siliceous SBA-15 and Al-modified SBA-15, such as Al-incorporated SBA-15 (AlSBA-15) and alumina-modified SBA-15 (Al2O3/SBA-15), for propane dehydrogenat... The catalytic properties of PtSn-based catalysts supported on siliceous SBA-15 and Al-modified SBA-15, such as Al-incorporated SBA-15 (AlSBA-15) and alumina-modified SBA-15 (Al2O3/SBA-15), for propane dehydrogenation were investigated. Al2O3/SBA-15 was prepared either by an impregnation method using aluminum nitrate aqueous solution, or by the treatment of SBA-15 with a Al(OC3H7)3 solution in anhydrous toluene. N2-physisorption, FT-IR spectroscopy, solid-state 27Al MAS NMR spectroscopy, hydrogen chemisorption, XRF, NH3 temperature-programmed desorption, X-ray photoelectron spectroscopy and TPO were used to characterize these samples. Among these catalysts, the PtSn-based catalyst supported on Al2O3/SBA-15, which was grafted with Al(OC3H7)3, exhibited the best catalytic performance in terms of activity and stability The possible reason was due to the high Pt metal dispersion and/or the strong interactions among Pt, Sn, and the support. 展开更多
关键词 PROPANE DEHYDROGENATION pt sba-15 aluminum modification
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Dehydrogenation of Propane on Pt or Pt Sn Catalysts with Al_2O_3 or SBA-15 Support 被引量:4
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作者 冯静 张明森 杨元一 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2014年第Z1期1232-1236,共5页
Dehydrogenation of propane on Pt or Pt Sn catalyst over Al2O3 or SBA-15 support was investigated. The catalysts were characterized by CO-pulse chemisorption, thermogravimetry, temperature-programmed-reduction of H2,an... Dehydrogenation of propane on Pt or Pt Sn catalyst over Al2O3 or SBA-15 support was investigated. The catalysts were characterized by CO-pulse chemisorption, thermogravimetry, temperature-programmed-reduction of H2,and diffuse reflectance infrared Fourier transform spectroscopy of absorbed CO. The results show that the platinum species is in oxidation state in the catalyst on Al2O3 support, so the catalyst must be reduced in H2 before dehydrogenation reaction. Addition of Sn improves the Pt dispersion, but the catalyst deactivates rapidly because of the coke formation. The interaction of Pt and Al2O3 is strong. On SBA-15 support, the platinum species is completely reduced to Pt0 in the calcination process, so the reduction is not needed. Addition of Sn improves the activity and selectivity of the catalyst. The interaction of Pt and SBA-15 is weak, so it is easy for Pt particles to sinter. 展开更多
关键词 PROPANE DEHYDROGENATION pt SN AL2O3 sba-15
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Preparation and Characterization of Pt-Sn/SBA-15 Catalysts and Their Catalytic Performances for Long Chain Alkane Dehydrogenation 被引量:8
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作者 卢泽湘 季生福 +1 位作者 刘辉 李成岳 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2008年第5期740-745,共6页
A series of the Pt-Sn/SBA-15 catalysts were prepared and their properties characterized by using X-ray powder diffraction (XRD), N2 adsorption-desorption, high resolution transmission electron microscope, X-ray phot... A series of the Pt-Sn/SBA-15 catalysts were prepared and their properties characterized by using X-ray powder diffraction (XRD), N2 adsorption-desorption, high resolution transmission electron microscope, X-ray photoelectron spectroscopy (XPS) and H2-temperature programmed reduction. Their performances in long chain alkane dehydrogenation were evaluated in a fixed-bed microreactor with dodecane as a model alkane. The results indicated that SBA-15 maintained the well-order mesoporous structure during the reaction. The performance of the catalyst was found not dominated by its textural properties, but by the molar ratio of Sn to Pt which governed the degree of Sn reduction. Owing to the highest degree of Sn reduction, 1% (by mass) Pt-1.8% (by mass) Sn/SBA-15 showed the best catalytic activity. At 0.1 MPa and 470℃, the molar ratio of hydrogen to alkane at 4, and liquid hourly space velocity (LHSV) 20 h^-1, the dodecane conversion is 10%, and the dodecene selectivity is about 70%. 展开更多
关键词 sba-15 catalyst ptSn alloy DODECANE DEHYDROGENATION
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可溶性酚醛树脂为碳源合成有序介孔炭及其电催化性能 被引量:10
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作者 陈秀 何建平 +4 位作者 党王娟 周建华 王涛 张传香 赵桂网 《新型炭材料》 SCIE EI CAS CSCD 北大核心 2008年第3期281-288,共8页
利用介孔硅SBA-15与苯酚、甲醛混合,原位合成可溶性酚醛树脂,高温炭化得有序介孔炭(C1);同时将预聚的酚醛树脂与SBA-15共混后再聚合,高温炭化得有序介孔炭(C2)。微波多元醇还原法合成Pt/C1、Pt/C2、Pt/CMK-5(糠醇为碳源)电催化剂。使用... 利用介孔硅SBA-15与苯酚、甲醛混合,原位合成可溶性酚醛树脂,高温炭化得有序介孔炭(C1);同时将预聚的酚醛树脂与SBA-15共混后再聚合,高温炭化得有序介孔炭(C2)。微波多元醇还原法合成Pt/C1、Pt/C2、Pt/CMK-5(糠醇为碳源)电催化剂。使用X射线衍射仪(XRD),N2物理吸附,透射电镜(TEM)和循环伏安技术(CV)对介孔炭的结构和催化剂的性能进行了表征。结果表明:C1主要由规则的六方介孔孔道构成,比表面积为947m2/g,孔径分布集中在4.5nm,Pt微粒在C1上具有良好的分散性,平均粒径约为3nm。C2的孔道较为模糊,负载的Pt微粒有一定程度的团聚。CV曲线显示,Pt/C1催化剂的电化学活性面积(EAS)为54.2m2/g,其催化甲醇氧化的性能优于Pt/C2及Pt/CMK5-而略差于商用催化剂Pt/C(E-TEK)。 展开更多
关键词 sba-15 介孔炭 可溶性酚醛树脂 微波法 炭载铂催化剂
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介孔碳负载铂催化剂的分散性和电催化活性 被引量:12
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作者 党王娟 何建平 +4 位作者 周建华 计亚军 刘晓磊 梅天庆 力虎林 《物理化学学报》 SCIE CAS CSCD 北大核心 2007年第7期1085-1089,共5页
以介孔硅SBA-15为模板,糠醇为碳源制备了高度有序的介孔碳(CMK-5),并用微波法合成碳负载的铂纳米粒子的催化剂.为改善铂微粒的分散性能,在微波碳载过程中添加了适量的阳离子表面活性剂(CTAB).XRD和TEM测试结果表明,CTAB的加入改善了铂... 以介孔硅SBA-15为模板,糠醇为碳源制备了高度有序的介孔碳(CMK-5),并用微波法合成碳负载的铂纳米粒子的催化剂.为改善铂微粒的分散性能,在微波碳载过程中添加了适量的阳离子表面活性剂(CTAB).XRD和TEM测试结果表明,CTAB的加入改善了铂催化剂的分散性,且使铂微粒的平均粒径降至2.9nm左右.循环伏安测试结果显示,加入CTAB后所得Pt/CMK-5催化剂的电化学活性面积大于未加CTAB的以及商业JohnsonMatthey公司的Pt/C催化剂的活性面积. 展开更多
关键词 sba-15 介孔碳CMK-5 微波 阳离子表面活性剂 pt/CMK-5催化剂 CTAB
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