PtSn/Al_2O_3微纳结构调控与丙烷脱氢性能研究
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- 英文论文题名：Designed PtSn/Al_2O_3 catalysts for propane dehydrogenation
- 论文作者：石磊 ; 王阳 ; 宋威 ; 王庆楠 ; 陆安慧
- 英文论文作者：Lei Shi ; Yang Wang ; Wei Song ; Qing-Nan Wang ; An-Hui Lu ; State Key Laboratory of Fine Chemicals ; School of Chemical Engineering ; Dalian University of Technology
- 年：2016
- 作者机构：大连理工大学化工学院精细化工国家重点实验室;
- 论文关键词：Al_2O_3 ; 纳米片 ; PtSn纳米簇 ; 丙烷 ; 脱氢
- 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：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：283k
- 原文格式：D
- 会议级别：全国
摘要
催化脱氢制烯烃是丙烷资源高效、清洁利用的重要途径,其中高比表面积Al_2O_3负载的Pt系催化剂应用最为广泛。然而,在苛刻的丙烷脱氢条件下,由积碳和烧结引发的Pt系催化剂的失活仍然是该反应亟待解决的难题。本文通过设计合成表面富含不饱和配位Al离子(27%,Fig.1A-B)的γ-Al_2O_3纳米片,实现了PtSn纳米簇的二维分散和稳定(Fig.1C-G)。CO-DRIFT和H_2-TPR结果证实Pt和Sn之间存在电子转移,Sn组分增强了Pt物种的电子密度。丙烷催化脱氢反应测试(Fig.2)显示,该催化剂具有高的反应活性和产物选择性、优越的抗积碳和抗烧结稳定性,各项指标远超现有商业γ_Al_2O_3纳米颗粒负载的PtSn催化剂。本研究通过载体结构的创新有效改善了Pt系丙烷脱氢催化剂的反应稳定性,实现了物理限制、化学锚定和动力学控制全方位的高稳定催化剂设计理念,为高效贵金属催化剂的研制提供了新的思路。
Herein,we have demonstrated that a γ-Al_2O_3 nanosheet that contains 27% pentacoordinated Al sites,can nicely disperse and stabilize the raft-like Pt-Sn clusters as a result of strong interaction between metal and support.Consequently,it allows a strong electronic interaction between Pt and Sn atoms,resulting in an increase of the electron density of the Pt sites.When used in the propane dehydrogenation reaction,such a catalyst displays excellent specific activity of propylene formation with >99% selectivity,and superior anti-coking and anti-sintering ability.Its exceptional ability to maintain the high activity and stability at ultrahigh space velocities further shows that the sheet construction of the catalyst facilitates the kinetic transfer process.
Herein,we have demonstrated that a γ-Al_2O_3 nanosheet that contains 27% pentacoordinated Al sites,can nicely disperse and stabilize the raft-like Pt-Sn clusters as a result of strong interaction between metal and support.Consequently,it allows a strong electronic interaction between Pt and Sn atoms,resulting in an increase of the electron density of the Pt sites.When used in the propane dehydrogenation reaction,such a catalyst displays excellent specific activity of propylene formation with >99% selectivity,and superior anti-coking and anti-sintering ability.Its exceptional ability to maintain the high activity and stability at ultrahigh space velocities further shows that the sheet construction of the catalyst facilitates the kinetic transfer process.
引文
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[4]Shi,L.;Deng,G.M.;Li,W.C.;Miao,S.;Zhang,W.P.;Lu A.-H.Angew Chem Int Ed 2015,54:13994.
[2]Wang,J.;Lu,A.-H;Li,M.R.;Zhang,W.P.;Cheng,Y.S.;Tian,D.X.;Li,W.C.;ACS Nano 2013,7:4902.
[3]Kwak,J.H.;Hu,J.Z.;Mei,D.;Yi,C.W.;Kim,D.H.;Peden,C.H.F.;Szanyi,J.Science 2009,325:1670.
[4]Shi,L.;Deng,G.M.;Li,W.C.;Miao,S.;Zhang,W.P.;Lu A.-H.Angew Chem Int Ed 2015,54:13994.