State Key Laboratory of Heavy Oil Processing, China University of Petroleum , Changping, Beijing 102249, China.
Sichuan Tianyi Science & Technology Co. Ltd. , Chengdu 610225, China.
ACS Appl Mater Interfaces. 2016 Mar;8(10):6439-48. doi: 10.1021/acsami.5b11717. Epub 2016 Mar 4.
Despite being technically possible, the hydrogen production by means of electrocatalytic water splitting is still practically unreachable mainly because of the lack of inexpensive and high active catalysts. Herein, a novel and facile approach by melamine polymerization, exfoliation and Co(2+)-assisted thermal annealing is developed to fabricate Co nanoparticles embedded in bamboo-like and nitrogen-rich carbonitride nanotubes (Co@NCN). The electronic interaction between the embedded Co nanoparticles and N-rich carbonitride nanotubes could strongly promote the HER performance. The optimized Co@NCN-800 exhibits outstanding HER activity with an onset potential of -89 mV (vs RHE), a large exchange current density of 62.2 μA cm(-2), and small Tafel slope of 82 mV dec(-1), as well as excellent stability (5000 cycles) in acid media, demonstrating the potential for the replacement of Pt-based catalysts. Control experiments reveal that the superior performance should be ascribed to the synergistic effects between embedded Co nanoparticles and N-rich carbonitride nanotubes, which originate from the high pyridinic N content, fast charge transfer rate from Co particles to electrodes via electronic coupling, and porous and bamboo-like carbonitride nanotubes for more active sites in HER.
尽管通过电催化水分解来生产氢气在技术上是可行的,但由于缺乏廉价且高活性的催化剂,实际上仍无法实现。在此,开发了一种通过三聚氰胺聚合、剥离和 Co(2+)-辅助热退火来制备嵌入竹状和富氮碳氮化物纳米管中的 Co 纳米粒子的新颖且简便的方法(Co@NCN)。嵌入的 Co 纳米粒子与富氮碳氮化物纳米管之间的电子相互作用可以强烈促进 HER 性能。优化后的 Co@NCN-800 在酸性介质中具有出色的 HER 活性,起始电位为-89 mV(相对于 RHE),大交换电流密度为 62.2 μA cm(-2),Tafel 斜率小至 82 mV dec(-1),以及出色的稳定性(5000 个循环),证明了替代 Pt 基催化剂的潜力。对照实验表明,优异的性能应归因于嵌入的 Co 纳米粒子和富氮碳氮化物纳米管之间的协同效应,这源于高吡啶 N 含量、通过电子偶联从 Co 颗粒到电极的快速电荷转移率以及多孔和竹状碳氮化物纳米管提供更多的 HER 活性位点。