笼型孔镍基催化剂的制备及其对苯酚加氢提质的应用
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- 英文论文题名：Synthesis of cage like Ni-based catalyst for hydrotreatment of phenol
- 论文作者：刘璐娟 ; 朱培红 ; 刘永刚 ; 翟贇璞
- 英文论文作者：Lujuan Liu ; Peihong Zhu ; Yonggang Liu ; Yunpu Zhai ; College of Chemistry and Molecular Engineering ; Zhengzhou University
- 年：2016
- 作者机构：郑州大学化学与分子工程学院;
- 论文关键词：生物油 ; 催化加氢 ; 镍基催化剂 ; 笼型材料 ; 抗烧结
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第三十七分会：纳米催化
- 语种：中文
- 分类号：TE624;O643.36
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第三十七分会 ; 纳米催化
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：285k
- 原文格式：D
- 会议级别：全国
摘要
目前在生物油催化加氢提质过程中存在着催化剂高温易烧结的问题,故本文以PS小球和F127为双模板,同resols、TEOS、AlCl_3·6H_2O共同组装,制备了笼形载体,负载Ni后,得到催化剂Ni/C-SiO_2-Al_2O_3(Ni/CL-CSA)。表征结果显示,Ni/CL-CSA具有100nm左右的大孔笼、3.8 nm的介孔窗口和6 nm的镍颗粒,镍粒子分散在大孔笼中(Fig 1A)。用作对比的介孔催化剂Ni/C-SiO_2-Al_2O_3(Ni/MP-CSA)具有有序的二维六方直型孔道,镍粒径为6.5 nm(Fig 1B)。将催化剂用于苯酚的加氢反应,200℃、5 MPa冷氢压下,尽管反应5小时,两种催化剂对苯酚的转化率都将近100%,但是在反应3 h时,Ni/CL-CSA对苯酚转化率已达到88.3%,远高于Ni/MP-CSA对苯酚的转化率62.2%(Fig 2),说明大孔结构可减小反应物和产物的传输阻力,提高反应速率。经过600℃、N2下焙烧5 h后,Ni/MP-CSA对苯酚转化率降低了18.6%,而笼型催化剂Ni/CL-CSA只降低了5.4%,进一步表征显示Ni/CL-CSA和Ni/MP-CSA中的镍粒径分别增加3.7 nm和7.5 nm,说明笼形催化剂可以有效地避免镍的聚集和长大,使催化剂具有良好的稳定性性。
A Ni-based cage like C-SiO_2-Al_2O_3(Ni/CL-CSA) catalyst was synthesized via a dual-templating method.The Ni/CL-CSA has three-dimensional connected cage-like macropores of about 100 nm and mesoporous windows of about 3.8 nm.Ni particles of 6 nm was incorporated into the macropores(Fig 1A).As comparison,mesoporous Ni/C-SiO_2-Al_2O_3(Ni/MP-CSA) with Ni particles of 6.5 nm dispersed in the mesopores(Fig 1B) were prepared.When used in the hydrotreatment of phenol,the phenol can be completely converted after 5 hours' reaction over both catalysts.But it is worth noting that 88.3% of phenol has been converted within 3h over Ni/CL-CSA,while only 62.2% of phenol can be converted over Ni/MP-CSA(Fig 2).It implies that the cage-like macropores and mesoporous windows can improve the mass transfer rate.After 600 ℃ heat treatment for 5 h,the nickel particle size of fresh Ni/CL-CSA and Ni/MP-CSA increased by 3.7 nm and 7.5 nm,revealing that the cage-like structure can avoid the particles from growing up,thus improving the catalytic stability.
A Ni-based cage like C-SiO_2-Al_2O_3(Ni/CL-CSA) catalyst was synthesized via a dual-templating method.The Ni/CL-CSA has three-dimensional connected cage-like macropores of about 100 nm and mesoporous windows of about 3.8 nm.Ni particles of 6 nm was incorporated into the macropores(Fig 1A).As comparison,mesoporous Ni/C-SiO_2-Al_2O_3(Ni/MP-CSA) with Ni particles of 6.5 nm dispersed in the mesopores(Fig 1B) were prepared.When used in the hydrotreatment of phenol,the phenol can be completely converted after 5 hours' reaction over both catalysts.But it is worth noting that 88.3% of phenol has been converted within 3h over Ni/CL-CSA,while only 62.2% of phenol can be converted over Ni/MP-CSA(Fig 2).It implies that the cage-like macropores and mesoporous windows can improve the mass transfer rate.After 600 ℃ heat treatment for 5 h,the nickel particle size of fresh Ni/CL-CSA and Ni/MP-CSA increased by 3.7 nm and 7.5 nm,revealing that the cage-like structure can avoid the particles from growing up,thus improving the catalytic stability.
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