Wang Cheng, Xu Hui, Shang Hongyuan, Jin Liujun, Chen Chunyan, Wang Yuan, Yuan Mengyu, Du Yukou
College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, P. R. China.
Inorg Chem. 2020 Mar 2;59(5):3321-3329. doi: 10.1021/acs.inorgchem.0c00132. Epub 2020 Feb 21.
Although great progress in pursuing high-performance catalysts for advanced electrocatalysis has been made, the design of high-efficiency electrocatalysts continues to be a huge challenge for commercializing electrochemical energy technologies. Herein, a three-dimensional (3D) hierarchical assembly nanostructure consisting of ultrathin Ir-doped Pd nanosheets has been well designed, which could serve as a bifunctional electrocatalyst for advanced hydrogen evolution reaction (HER) and liquid fuel electrooxidation. In particular, the optimized PdIr nanocatalyst displays excellent electrocatalytic HER performance with an overpotential of only 73 mV at 10 mA cm along with excellent stability. More importantly, it can also show outstanding electrocatalytic performance for liquid fuel oxidation with a mass activity of 4326.1 mA mg for ethylene glycol oxidation reaction. Mechanistic study reveals that the highly porous 3D nanostructure, the modulation of electronic structure after the introduction of Ir, not only guarantees a high level of exposure of surface active sites and smooth charge transfer but also generates the new active centers for facilitating the adsorption of HO and recombination of H*, thereby dramatically increasing the intrinsic activity of electrocatalysis.
尽管在寻找用于先进电催化的高性能催化剂方面已经取得了很大进展，但高效电催化剂的设计仍然是电化学能源技术商业化面临的巨大挑战。在此，一种由超薄铱掺杂钯纳米片组成的三维（3D）分级组装纳米结构被精心设计出来，它可以作为一种用于先进析氢反应（HER）和液体燃料电氧化的双功能电催化剂。特别是，优化后的钯铱纳米催化剂表现出优异的电催化HER性能，在10 mA cm时过电位仅为73 mV，同时具有出色的稳定性。更重要的是，它对液体燃料氧化也能表现出出色的电催化性能，对乙二醇氧化反应的质量活性为4326.1 mA mg。机理研究表明，高度多孔的3D纳米结构以及引入铱后电子结构的调制，不仅保证了表面活性位点的高暴露水平和平滑的电荷转移，还产生了促进羟基吸附和氢原子重组的新活性中心，从而显著提高了电催化的本征活性。
