Solid frustrated-Lewis-pair catalysts constructed by regulations on surface defects of porous nanorods of CeO(2).

Solid frustrated-Lewis-pair catalysts constructed by regulations on surface defects of porous nanorods of CeO(2).
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CeO2多孔纳米棒表面缺陷调控构建的固体受阻刘易斯对催化剂

DOI:
10.1038/ncomms15266
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发表时间:
2017-05-18
影响因子:
16.6
通讯作者:
Qu Y
Qu Y
中科院分区:
综合性期刊1区
文献类型:
--
作者:
Zhang S;Huang ZQ;Ma Y;Gao W;Li J;Cao F;Li L;Chang CR;Qu Y

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在原子水平上确定非均相催化剂的催化中心对于理解催化机理具有重要意义。通过对金属氧化物表面缺陷的表面工程改造,可以构建新的活性中心,调节催化剂的活性和选择性。在这里,我们概述了通过控制纳米氧化铈的表面缺陷来产生固体阻挫刘易斯对(FLP)金属氧化物的策略,用于烯烃和炔烃的有效氢化。具有高浓度表面缺陷的二氧化铈多孔纳米棒(PN-CeO 2)通过两个相邻的表面Ce 3+构建新的刘易斯酸位点。由于CeO 2的刚性晶格,相邻的表面晶格氧作为刘易斯碱和结构刘易斯酸形成固体FLP位,容易解离H-H键,活化能为0.17 eV。
Identification on catalytic sites of heterogeneous catalysts at atomic level is important to understand catalytic mechanism. Surface engineering on defects of metal oxides can construct new active sites and regulate catalytic activity and selectivity. Here we outline the strategy by controlling surface defects of nanoceria to create the solid frustrated Lewis pair (FLP) metal oxide for efficient hydrogenation of alkenes and alkynes. Porous nanorods of ceria (PN-CeO2) with a high concentration of surface defects construct new Lewis acidic sites by two adjacent surface Ce3+. The neighbouring surface lattice oxygen as Lewis base and constructed Lewis acid create solid FLP site due to the rigid lattice of ceria, which can easily dissociate H–H bond with low activation energy of 0.17 eV.