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首页> 外文期刊>Catalysis science & technology >Nearly atomic precise gold nanoclusters on nickel-based layered double hydroxides for extraordinarily efficient aerobic oxidation of alcohols
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Nearly atomic precise gold nanoclusters on nickel-based layered double hydroxides for extraordinarily efficient aerobic oxidation of alcohols

机译：近原子精确的黄金纳米束镍基水滑石非常有效的有氧氧化醇

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摘要

A series of nickel-based layered double hydroxides supported nearly atomic precise Au-25 nanoclusters catalysts, and especially Au-25/NixAl-LDH systems (x = Ni/Al, 2, 3, 4) were fabricated via modified electrostatic adsorption of captopril-capped clusters Au(25)Capt(18) onto the predispersed positively-charged NixAl-LDH supports followed by proper calcination. Detailed characterizations show that the ultrafine gold clusters of similar to 0.9 nm were well dispersed on the edge sites of hexagonal plate-like particles of NixAl-LDH (x = 2, 3) originated from their ordered LDH layers with more Ni-OH sites and strong Au-LDH synergy, while slightly aggregated to similar to 1.1 nm on the irregular Ni4Al-LDH due to its poor layer structure along with doped nickel oxide. The catalysts exhibit excellent activity for selective oxidation of 1-phenylethanol to acetophenone with molecular oxygen under base-free, and the activity follows an increased order of Au-25/Ni4Al-LDH < Au-25/Ni2Al-LDH < Au-25/Ni3Al-LDH. The Au-25/Ni3Al-LDH shows the highest activity with TOF of 6780 h(-1) in toluene and 118 500 h(-1) in solvent-free and can be applied for a wide range of alcohols, mainly ascribed to ultrafine gold clusters and strongest gold-LDH interaction associated with the highly ordered Ni3Al-LDH layers. Similar regularity is found in the Au-25/NixMn-LDH and Au-25/Ni3-xMnxFe-LDH systems. The Au-25/Ni3Al-LDH can be reused 5 times without loss of activity. The least-squares fit analysis yields the rate constant (k) and apparent activation energy (E-a) of Au-25/NixAl-LDH catalysts for 1-phenylethanol oxidation, and the order of k and E-a values act in accordance with their reactivities.
机译：一系列的镍基水滑石支持近原子精确Au-25制备催化剂,尤其是Au-25 / NixAl-LDH系统(x =镍/铝,2、3、4)通过修改后的静电吸附捏造captopril-capped集群的非盟(25)上校(18)上predispersed带正电荷的NixAl-LDH支持适当的煅烧紧随其后。特征表明,超细金集群的类似于0.9纳米分散在网站的六角状粒子NixAl-LDH起源于(x = 2、3)他们命令LDH层Ni-OH网站和强大的Au-LDH协同作用,而略聚合类似1.1 nm不规则Ni4Al-LDH由于其可怜的层状结构掺杂氧化镍。选择性氧化的优秀活动1-phenylethanol与分子苯乙酮氧气在base-free,活动增加的顺序Au-25 / Ni4Al-LDH

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