PtRu catalysts supported on heteropolyacid and chitosan functionalized carbon nanotubes for methanol oxidation reaction of fuel cells.

PtRu catalysts supported on heteropolyacid and chitosan functionalized carbon nanotubes for methanol oxidation reaction of fuel cells.
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DOI:
10.1039/c1cp21271k
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发表时间:
2011-08
期刊:
Physical chemistry chemical physics : PCCP
影响因子:
--
通讯作者:
Zhiming Cui;Chang Ming Li;S. Jiang
Zhiming Cui;Chang Ming Li;S. Jiang
中科院分区:
其他
文献类型:
--
作者:
Zhiming Cui;Chang Ming Li;S. Jiang

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开发了一种简单的自组装方法,用壳聚糖(CS)和磷钼酸(H(3)PMo(12)O(40),HPMo)和磷钨酸(H(3)PW(12)O(40),HPW)的杂多酸(HPA)功能化碳纳米管(CNT)。非共价官能化方法引入了均匀的表面官能团,对碳纳米管的石墨烯结构没有不利影响,可以在室温下进行,无需使用腐蚀性酸。与传统酸处理碳纳米管 (PtRu/AO-CNT) 上负载的 PtRu 纳米颗粒相比,HPA-CS-CNT 上负载的 PtRu 纳米颗粒分布均匀,尺寸小得多。 PtRu/HPA-CS-CNTs 催化剂上 CO(ad) 氧化的起始电位和峰值电位比 PtRu/AO-CNTs 上的更负,表明 HPA 促进 CO 的电氧化。PtRu/HPMo-CS-CNTs 催化剂比 PtRu/HPW-CS-CNTs 具有更高的甲醇氧化电催化活性和更高的对 CO 中毒的耐受性。 HPMo 在 PtRu/HPA-CS-CNTs 催化剂上更好的电催化增强很可能与以下事实有关:含钼的 HPAs(例如 HPMo)具有更不稳定的末端氧,可以提供额外的活性氧位点,同时以与 PtRu 二元合金体系中 Ru 类似的方式加速 CO 和甲醇的氧化。
A simple self-assembly approach has been developed to functionalize carbon nanotubes (CNTs) with chitosan (CS) and heteropolyacids (HPAs) of phosphomolybdic acid (H(3)PMo(12)O(40), HPMo) and phosphotungstic acid (H(3)PW(12)O(40), HPW). The non-covalent functionalization method, which introduces homogenous surface functional groups with no detrimental effect on graphene structures of CNTs, can be carried out at room temperature without the use of corrosive acids. The PtRu nanoparticles supported on HPAs-CS-CNTs have a uniform distribution and much smaller size as compared to those of the PtRu nanoparticles supported on conventional acid treated CNTs (PtRu/AO-CNTs). The onset and peak potentials for CO(ad) oxidation on PtRu/HPAs-CS-CNTs catalysts are more negative than those on PtRu/AO-CNTs, indicating that HPAs facilitate the electro-oxidation of CO. The PtRu/HPMo-CS-CNTs catalyst has a higher electrocatalytic activity for methanol oxidation and higher tolerance toward CO poisoning than PtRu/HPW-CS-CNTs. The better electrocatalytic enhancement of HPMo on the PtRu/HPAs-CS-CNTs catalyst is most likely related to the fact that molybdenum-containing HPAs such as HPMo have more labile terminal oxygen to provide additional active oxygen sites while accelerating the CO and methanol oxidation in a similar way to that of Ru in the PtRu binary alloy system.