单原子催化
详细信息    查看官网全文
摘要
负载型金属催化剂是多相催化剂中最重要的一类催化剂,广泛应用于能源转化、环境催化以及精细化工领域。为了提高金属催化剂的原子利用率,一般将金属活性组分高分散于载体上。金属活性组分分散的极限是单原子分散,即,所有的金属活性组分都以单原子的形式分散于载体表面,我们定义该类催化剂为"单原子催化剂"。自从2011年我们课题组首次提出"单原子催化剂"概念以来,单原子催化在最近5年得到了快速发展,已经成为多相催化领域的研究热点。在本报告中,作者将介绍3类典型的单原子催化剂,包括负载型Pt族金属单原子催化剂(Pt/Fe Ox,Ir/Fe Ox,Au/CeO_2等)、合金化单原子催化剂(Au-Pd,Ag-Pd,Zn-Pd),以及M-N-C(M指过渡金属Fe、Co等)催化剂。结合本课题组的实验结果讨论影响单原子分散的主要因素;阐述单原子催化剂在一氧化碳氧化、芳香硝基化合物的选择加氢、乙炔选择加氢等反应中的优异催化性能;揭示单原子催化剂的构效关系。
Heterogeneous catalysts are critical to energy production,pollution control,and fine chemical synthesis.Supported metal catalysts are among the most important heterogeneous catalysts.The efficiency of such catalysts as used in industry is,however,extremely low on a per metal atom basis,because only the surface active-site atoms are used.Catalysts with single-atom dispersion,which we define as the single-atom catalysts(SAC),are thus highly desirable to maximize the atom efficiency.In this presentation,we will show three types of SACs,including reducible oxide supported noble metal SACs,single-atom alloys,and M-N-C(M refers to Co and Fe).The key factors governing the atomic dispersion of active metals are discussed,the catalytic performances of the single-atom catalysts in CO oxidation and chemoselective reduction of nitroarenes and acetylene are presented and compared with nanoparticle counterparts,and the structure-performance relationship is understood based on a series of characterizations and DFT calculations.
引文
[1]Qiao,B.;et al.,Nat.Chem.2011,3:634.
    [2]Yang,X.;et al.,Acc.Chem.Res.2013,46:1740.
    [3]Lin,J.;et al.,J.Am.Chem.Soc.2013,135:15314.
    [4]Wei,H.;et al.,Nat.Commun.2014,5:5634.
    [5]Pei,G.;et al.,ACS.Catal.2015,5:3717.
    [6]Zhou,H.;et al.,ACS Catal.2016,6:1054.

© 2004-2018 中国地质图书馆版权所有 京ICP备05064691号 京公网安备11010802017129号

地址:北京市海淀区学院路29号 邮编:100083

电话:办公室:(+86 10)66554848;文献借阅、咨询服务、科技查新:66554700