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首页> 外文期刊>Catalysis science & technology >A novel bifunctional Pd-ZIF-8/rGO catalyst with spatially separated active sites for the tandem Knoevenagel condensation-reduction reaction
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A novel bifunctional Pd-ZIF-8/rGO catalyst with spatially separated active sites for the tandem Knoevenagel condensation-reduction reaction

机译:一种新颖的双官能Pd-ZIF-8 / rGO催化剂空间上分开活动网站的串联诺文葛耳condensation-reduction反应

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摘要

A novel bifunctional catalyst with spatially separated active sites was prepared by the immobilization of Pd nanoparticles (NPs) via covalent interaction and coordination of a zeolitic imidazolate framework (ZIF-8) on the surface of graphene oxide (GO), respectively, which was used as an efficient catalyst for the Knoevenagel condensation-reduction tandem reaction. The results of Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), Raman spectroscopy, UV-vis spectroscopy, X-ray photoelectron spectroscopy (XPS) and thermogravimetric analysis (TGA) demonstrated that Pd and ZIF-8 were successfully immobilized on the surface of GO, and the GO was reduced to reduced graphene oxide (rGO) using NaBH4 as the reductant in the preparation of Pd-ZIF-8/rGO. The textural properties and morphology of Pd-ZIF-8/rGO were characterized by N-2 adsorption-desorption, scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Pd-ZIF-8/rGO shows excellent catalytic performance in the tandem reaction with 100% benzaldehyde conversion and 98.3% selectivity to benzylmalononitrile. The excellent catalytic performance of Pd-ZIF-8/rGO in the tandem reaction is due to the high catalytic activities of spatially separated Pd NPs and ZIF-8 active sites and concentrated reactants on the surface of Pd-ZIF-8/ rGO due to the pi-pi interaction between rGO and the reactants. The anchoring and stabilization effects of oxygenated groups of GO inhibit the aggregation and leakage of active sites, leading to good catalytic recyclability with almost unchanged catalytic activity for more than eight cycles in the tandem reaction.
机译:一种新颖的双功能催化剂与空间网站是由分离的活跃固定的钯纳米颗粒(NPs)通过共价相互作用和协调的沸石的imidazolate框架(ZIF-8)氧化石墨烯表面(去),分别这是作为一个高效的催化剂诺文葛耳condensation-reduction串联的反应。红外光谱(ir)、x射线衍射(XRD)、拉曼光谱、紫外可见光谱,x射线光电子能谱(XPS)和热重分析(TGA)Pd和ZIF-8成功固定化表面上的去,去减少减少氧化石墨烯(rGO)使用NaBH4作为还原剂制备的Pd-ZIF-8 / rGO。结构和形态的属性Pd-ZIF-8 / rGO n的特征adsorption-desorption,扫描电子显微镜(SEM)和透射电子显微镜(TEM)。串联反应的催化性能苯甲醛转化率100%和98.3%benzylmalononitrile选择性。Pd-ZIF-8 / rGO的催化性能是由于高催化串联反应空间上分开Pd NPs和活动反应物ZIF-8活跃网站和集中表面Pd-ZIF-8 / rGO由于介子rGO和反应物之间的互动。锚定氧合和稳定的影响组去抑制聚合和泄漏活跃的网站,导致良好的催化催化再循环能力几乎不变串联活动超过8个周期的反应。

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