Synthetically Tuned Pd-Based Intermetallic Compounds and their Structural Influence on the O2 Dissociation in Benzylamine Oxidation,ACS Applied Materials & Interfaces

当前位置： X-MOL 学术 › ACS Appl. Mater. Interfaces › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Synthetically Tuned Pd-Based Intermetallic Compounds and their Structural Influence on the O2 Dissociation in Benzylamine Oxidation
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2019-10-03 , DOI: 10.1021/acsami.9b11318
Vijaykumar S. Marakatti ₁ , Saurav Ch. Sarma , Shreya Sarkar , M. Krajčí ₂ , Eric M Gaigneaux ₁ , Sebastian C. Peter

Affiliation

Intermetallic compounds (IMCs) have diverse electronic and geometrical properties to offer. However, the synthesis of intermetallic nanoparticles is not always easy; developing new methodologies that are conventional for many systems can be challenging, especially when incorporating highly electropositive metals to reduce to IMCs using solution synthesis methodologies. In this study, we report a comprehensive approach to access nanocrystalline Pd_xM_y (M = Cu, Zn, Ga, Ge, Sn, Pb, Cd, In) intermetallic (IM) via the coreduction method employing sodium borohydride as the reductant. A combination of diffraction, spectroscopic, and microscopic techniques were performed to characterize the formed nanoparticles in terms of their phase composition, purity, particle size distribution, and surface oxidation properties of metals, respectively. IMCs of Pd with the elements such as Cu, Zn, Ga, and Ge exhibited higher catalytic activity that with elements such as In, Sn, Pb, and Cd. The DFT studies on these compounds revealed that the adsorption of benzylamine at the Pd site and the dissociative adsorption of O₂ on the IM surface play a significant effect on catalytic activity. Among them, PdCu IM exhibited an excellent conversion of benzylamine (94.0%), with 92.2% of dibenzylimine selectivity compared to other IMCs. Moreover, PdCu exhibited decent recyclability and activity for the oxidation of different substituted primary amines.

中文翻译：

合成调整的基于Pd的金属间化合物及其结构对苄胺氧化中O ₂分解的影响

金属间化合物（IMC）具有多种电子和几何特性。然而，金属间纳米颗粒的合成并不总是那么容易。开发许多系统常用的新方法可能是一项挑战，尤其是在使用溶液合成方法将高度电正性金属还原为IMC的情况下。在这项研究中，我们报告了一种访问纳米晶Pd _x M _y的综合方法（M = Cu，Zn，Ga，Ge，Sn，Pb，Cd，In）金属间化合物（IM）通过使用硼氢化钠作为还原剂的共芯法形成。进行了衍射，光谱和显微镜技术的组合，以分别根据其相组成，纯度，粒度分布和金属的表面氧化特性来表征所形成的纳米颗粒。Pd与Cu，Zn，Ga和Ge等元素的IMC表现出比In，Sn，Pb和Cd等元素更高的催化活性。对这些化合物的DFT研究表明，苄胺在Pd位点的吸附和O ₂的解离吸附在IM表面上的催化剂对催化活性起重要作用。其中，与其他IMC相比，PdCu IM表现出优异的苄胺转化率（94.0％），对二苄基亚胺的选择性为92.2％。此外，PdCu对不同取代的伯胺具有良好的循环利用性和氧化活性。

更新日期：2019-10-03

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南