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用于多相催化还原人为污染物的纳米受限空间内的高分散钯纳米颗粒。

Highly dispersive palladium nanoparticle in nanoconfined spaces for heterogeneous catalytic reduction of anthropogenic pollutants.

作者信息

Subhan Fazle, Aslam Sobia, Yan Zifeng, Yaseen Muhammad

机构信息

Department of Chemistry, Abdul Wali Khan University Mardan, K.P. Pakistan; State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Qingdao 266580, China.

Department of Chemistry, Abdul Wali Khan University Mardan, K.P. Pakistan; State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Qingdao 266580, China.

出版信息

J Colloid Interface Sci. 2021 Jul 15;594:304-315. doi: 10.1016/j.jcis.2021.03.030. Epub 2021 Mar 15.

Abstract

Pd-containing catalysts are highly promising in catalytic reactions, and their activity severely dependent on the dispersion extent of Pd nanoparticles (Pd NPs) . However, the regulation of Pd NPs size and dispersion degree are now pretty much the agendas. Here we report a facile solid-state fabrication strategy (SSFS) to promote Pd NPs dispersion in the nano environment of as made mesoporous silica KIT-6 (AK) by taking advantage of three critical factors, namely (i) the confined spaces where Pd precursor locate during fabrication, (ii) the interaction between Pd and supports, and (iii) the 3-dimentional (3D) structure of AK. First, AK presents 3D confined spaces between silica walls and template P123. Second, both silica walls and template P123 in AK offer interaction with Pd precursor. Third, the 3D structure provides more easy access for Pd insertion than linear channels structure without any pore blockage. The characterization results revealed that AK give better dispersion with smaller size of (3.9 nm) Pd than its counterpart (16 nm) prepared from template-free KIT-6 (CK). Moreover, the synthesized catalysts exhibit excellent activity and stability in catalytic conversion of p-nitrophenol (p-NP) and Methylene blue (MB). For a typical PdAK-1.0 catalyst, the complete conversion of P-NP and MB was achieved in less than 10 min with a reaction rate constant (k) of 0.3106 and 0.345 min, respectively. It is superior to that on PdCK-1.0 prepared from template free KIT-6 and several reported catalysts. Furthermore, the PdAK-1.0 catalyst presents pretty good stability in catalytic reduction and is apparently better than PdCK-1.0.

摘要

含钯催化剂在催化反应中极具前景,其活性严重依赖于钯纳米颗粒(Pd NPs)的分散程度。然而,目前对Pd NPs尺寸和分散度的调控仍是亟待解决的问题。在此,我们报道了一种简便的固态制备策略(SSFS),通过利用三个关键因素,即(i)制备过程中钯前驱体所处的受限空间,(ii)钯与载体之间的相互作用,以及(iii)介孔二氧化硅KIT-6(AK)的三维(3D)结构,来促进Pd NPs在制备的介孔二氧化硅AK的纳米环境中的分散。首先,AK在二氧化硅壁和模板P123之间呈现出3D受限空间。其次,AK中的二氧化硅壁和模板P123都能与钯前驱体发生相互作用。第三,与没有任何孔堵塞的线性通道结构相比,3D结构为钯的插入提供了更便捷的通道。表征结果表明,与由无模板KIT-6(CK)制备的对应物(16 nm)相比,AK能使钯具有更好的分散性且尺寸更小(3.9 nm)。此外,合成的催化剂在对硝基苯酚(p-NP)和亚甲基蓝(MB)的催化转化中表现出优异的活性和稳定性。对于典型的PdAK-1.0催化剂,P-NP和MB在不到10分钟内即可完全转化,反应速率常数(k)分别为0.3106和0.345 min⁻¹。它优于由无模板KIT-6制备的PdCK-1.0以及几种已报道的催化剂。此外,PdAK-1.0催化剂在催化还原中表现出相当好的稳定性,明显优于PdCK-1.0。

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