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Synergic Catalysis of PdCu Alloy Nanoparticles within a Macroreticular Basic Resin for Hydrogen Production from Formic Acid

机译:大孔碱性树脂中PdCu合金纳米粒子的协同催化从甲酸制氢

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摘要

Highly dispersed PdCu alloy nanoparticles have been successfully prepared within a macroreticular basic resin bearing N(CH3)(2) functional groups. This previously unappreciated combination of alloy is first proven to be responsible for the efficient production of high-purity H-2 from formic acid (HCOOH) dehydrogenation for chemical hydrogen storage. By the addition of Cu, the electronically promoted Pd sites show significantly higher catalytic activity as well as a better tolerance towards CO poisoning as compared to their monometallic Pd counterparts. Experimental and DFT calculation studies revealed not only the synergic alloying effect but also cooperative action by the N(CH3)(2) groups within the resin play crucial roles in achieving exceptional catalytic performances. In addition to the advantages such as, facile preparation method, free of additives, recyclable without leaching of active component, and suppression of unfavorable CO formation less than 3ppm, the present catalytic system is cost-effective because of the superior catalytic activity compared with that of well-established precious PdAg or PdAu catalysts. The present catalytic system is particularly desirable for an ideal hydrogen vector in terms of potential industrial application for fuel cells.
机译:已经在带有N(CH3)(2)官能团的大网状碱性树脂中成功制备了高度分散的PdCu合金纳米颗粒。这种先前未被欣赏的合金组合首先被证明是负责从甲酸(HCOOH)脱氢有效生产高纯度H-2的方法,以用于化学储氢。与单金属Pd对应物相比,通过添加Cu,电子促进的Pd位点显示出显着更高的催化活性以及对CO中毒的更好耐受性。实验和DFT计算研究表明,树脂中的N(CH3)(2)基团不仅具有协同合金作用,而且还起到了协同作用,在获得优异的催化性能方面起着至关重要的作用。除了制备方法简便,无添加剂,可回收利用而不会浸出活性成分以及抑制低于3ppm的不利CO生成等优点外,本催化体系具有成本效益,因为与之相比,该体系具有优越的催化活性。成熟的贵重PdAg或PdAu催化剂。就燃料电池的潜在工业应用而言,本发明的催化系统对于理想的氢载体是特别理想的。

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