Institute for Clean Energy & Advanced Materials, Southwest University, Chongqing, PR China.
Chemistry. 2012 Dec 3;18(49):15693-8. doi: 10.1002/chem.201201571. Epub 2012 Oct 11.
Unique DNA-promoted Pd nanocrystals on carbon nanotubes (Pd/DNA-CNTs) are synthesized for the first time, in which through its regularly arranged PO(4)(3-) groups on the sugar-phosphate backbone, DNA directs the growth of ultrasmall Pd nanocrytals with an average size of 3.4 nm uniformly distributed on CNTs. The Pd/DNA-CNT catalyst shows much more efficient electrocatalytic activity towards oxygen reduction reaction (ORR) with a much more positive onset potential, higher catalytic current density and better stability than other Pd-based catalysts including Pd nanocrystals on carbon nanotubes (Pd/CNTs) without the use of DNA and commercial Pd/C catalyst. In addition, the Pd/DNA-CNTs catalyst provides high methanol tolerance. The high electrocatalytic performance is mainly contributed by the ultrasmall Pd nanocrystal particles grown directed by DNA to enhance the mass transport rate and to improve the utilization of the Pd catalyst. This work may demonstrate a universal approach to fabricate other superior metal nanocrystal catalysts with DNA promotion for broad applications in energy systems and sensing devices.
首次合成了独特的 DNA 促进的碳纳米管上的 Pd 纳米晶(Pd/DNA-CNTs),其中通过 DNA 在糖-磷酸主链上规则排列的 PO(4)(3-)基团,指导超小 Pd 纳米晶的生长,Pd 纳米晶均匀分布在 CNTs 上,平均尺寸为 3.4nm。与其他 Pd 基催化剂(包括未使用 DNA 的碳纳米管上的 Pd 纳米晶(Pd/CNTs)和商业 Pd/C 催化剂)相比,Pd/DNA-CNT 催化剂对氧还原反应(ORR)具有更高的电催化活性,起始电位更正,催化电流密度更高,稳定性更好。此外,Pd/DNA-CNTs 催化剂对甲醇具有高耐受性。高电催化性能主要归因于 DNA 促进生长的超小 Pd 纳米晶颗粒,这提高了质量传输速率并提高了 Pd 催化剂的利用率。这项工作可能展示了一种通用的方法来制备其他具有 DNA 促进作用的优异金属纳米晶催化剂,以在能源系统和传感设备中广泛应用。