Supported core@shell electrocatalysts for fuel cells: close encounter with reality.

Supported core@shell electrocatalysts for fuel cells: close encounter with reality.
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DOI:
10.1038/srep01309
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发表时间:
2013
期刊:
影响因子:
4.6
通讯作者:
Kim, Soo-Kil
Kim, Soo-Kil
中科院分区:
综合性期刊3区
文献类型:
--
作者:
Hwang, Seung Jun;Yoo, Sung Jong;Shin, Jungho;Cho, Yong-Hun;Jang, Jong Hyun;Cho, Eunae;Sung, Yung-Eun;Nam, Suk Woo;Lim, Tae-Hoon;Lee, Seung-Cheol;Kim, Soo-Kil

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核壳型燃料电池电催化剂具有铂利用率高、电子结构可修饰以提高活性等优点。在这项研究中,我们提出了设计高活性和稳定的核@Shell/C的理论背景和一种新的简便的合成策略。在氧吸附能和空位形成能的指导下,采用密度泛函理论计算了Pd3Cu1@Pt/C催化剂的氧还原活性和稳定性。这些预测得到了Pd3Cu1/C核的无表面活性剂合成和以Hantzsch酯为还原剂的选择性铂壳形成的实验验证。以同样的方式设计合成了用于氢氧化反应的Pd@Pd4Ir6/C催化剂。所开发的催化剂表现出高活性、高选择性和在单电池水平上的4,000 h的长期寿命。
Core@shell electrocatalysts for fuel cells have the advantages of a high utilization of Pt and the modification of its electronic structures toward enhancement of the activities. In this study, we suggest both a theoretical background for the design of highly active and stable core@shell/C and a novel facile synthetic strategy for their preparation. Using density functional theory calculations guided by the oxygen adsorption energy and vacancy formation energy, Pd3Cu1@Pt/C was selected as the most suitable candidate for the oxygen reduction reaction in terms of its activity and stability. These predictions were experimentally verified by the surfactant-free synthesis of Pd3Cu1/C cores and the selective Pt shell formation using a Hantzsch ester as a reducing agent. In a similar fashion, Pd@Pd4Ir6/C catalyst was also designed and synthesized for the hydrogen oxidation reaction. The developed catalysts exhibited high activity, high selectivity, and 4,000 h of long-term durability at the single-cell level.
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