Synergic Catalysis of PdCu Alloy Nanoparticles within a Macroreticular Basic Resin for Hydrogen Production from Formic Acid
Synergic Catalysis of PdCu Alloy Nanoparticles within a Macroreticular Basic Resin for Hydrogen Production from Formic Acid
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DOI：
10.1002/chem.201501760
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发表时间：
2015-08-17
影响因子：
4.3
通讯作者：
Yamashita, Hiromi
中科院分区：
文献类型：
--
作者：
Mori, Kohsuke;Tanaka, Hiromasa;Yamashita, Hiromi
在含N（CH 3）（2）官能团的大孔树脂中成功地制备了高分散的PdCu合金纳米粒子。这种以前不受重视的合金组合首次被证明是负责从甲酸（HCOOH）脱氢用于化学储氢的高纯度H-2的有效生产。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，以及更好的耐受性对CO中毒相比，其monopoly Pd对应物。实验和DFT计算研究表明，树脂中的N（CH 3）（2）基团不仅具有协同合金化作用，而且还具有协同作用，在实现优异的催化性能方面起着至关重要的作用。该催化体系具有制备方法简单、不含添加剂、可循环使用而不浸出活性组分、抑制CO生成量小于3 ppm等优点，与传统的贵金属PdAg或PdAu催化剂相比，具有上级催化活性，因此具有成本效益。就燃料电池的潜在工业应用而言，本催化体系对于理想的氢载体是特别期望的。
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.