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Pd-SnO2/Al2O3 heteroaggregate nanocatalysts for selective hydrogenations of p-nitroacetophenone and p-nitrobenzaldehyde
Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2017-10-10 , DOI: 10.1016/j.apcata.2017.10.004
Miaomiao Liu , Weiqiang Tang , Yisheng Xu , Hongbo Yu , Hongfeng Yin , Shuangliang Zhao , Shenghu Zhou

Pd-SnO2 heteroaggregate nanocatalysts were synthesized by in-situ transformation of PdSn bimetallic nanoparticles on alumina. The PdSn bimetallic nanoparticles were prepared by co-reduction of Pd and Sn precursors. The obtained PdSn nanoparticles possibly have a core-shell like structure with Pd cores and Sn-rich shells due to the fast reduction of Pd precursors. The Pd-SnO2/Al2O3 heteroaggreagte nanocatalysts were synthesized by calcination of PdSn/Al2O3 in air followed by H2 reduction. Various characterization techniques, such as HRTEM, XRD and XPS, were used to characterize the PdSn and Pd-SnO2. The Pd3-(SnO2)1/Al2O3 heteroaggreagte nanocatalysts with a ratio of Pd/Sn of 3/1 illustrated enhanced catalytic performances for p-nitroacetophenone and p-nitrobenzaldehyde hydrogenations relative to monometallic Pd nanocatalysts. Theoretical calculations using density functional theory suggested that Pd-SnO2 facilitates the adsorption of reactants in a higher degree than that of products, thus enhancing the catalytic activity even with partial coverage of Pd surfaces with SnO2. The blockage effect of SnO2 on Pd surfaces is speculated to enhance the catalytic selectivity for p-nitroacetophenone and p-nitrobenzaldehyde hydrogenations over Pd-SnO2 heteroaggregate nanocatalysts.



中文翻译:

钯的SnO 2 / Al的2个ö 3 heteroaggregate纳米催化剂用于选择性加氢p硝基乙酰苯和p -nitrobenzaldehyde

通过氧化铝上原位转化PdSn双金属纳米粒子,合成了Pd-SnO 2杂聚集体纳米催化剂。通过共还原Pd和Sn前体制备PdSn双金属纳米颗粒。由于Pd前体的快速还原,获得的PdSn纳米颗粒可能具有带有Pd核和富Sn壳的核-壳状结构。通过在空气中煅烧PdSn / Al 2 O 3,然后还原H 2,合成了Pd-SnO 2 / Al 2 O 3杂聚合纳米催化剂。各种表征技术(例如HRTEM,XRD和XPS)用于表征PdSn和Pd-SnO 2。钯3 - (SNO 21 / Al的2 ö 3 heteroaggreagte纳米催化剂用的3/1斑竹增强的催化性能的Pd / Sn构成的比p硝基乙酰苯和p相对于单金属的Pd纳米催化剂-nitrobenzaldehyde氢化。使用密度泛函理论的理论计算表明,Pd-SnO 2的吸附程度高于产物,从而促进了反应物的吸附,因此即使SnO 2部分覆盖了Pd表面,也提高了催化活性。推测SnO 2对Pd表面的阻滞作用可增强对p的催化选择性。Pd-SnO 2杂聚集体纳米催化剂上的硝基苯乙酮和硝基苯甲醛加氢反应。

更新日期:2017-10-10
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