Hydrogen Evolution Activity of Ruthenium Phosphides Encapsulated in Nitrogen- and Phosphorous-Codoped Hollow Carbon Nanospheres
Hydrogen Evolution Activity of Ruthenium Phosphides Encapsulated in Nitrogen- and Phosphorous-Codoped Hollow Carbon Nanospheres
复制标题
氮磷共掺杂空心碳纳米球包裹磷化钌的析氢活性
DOI：
10.1002/cssc.201702010
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发表时间：
2018-02-22
期刊：
影响因子：
8.4
通讯作者：
Liu, Chen-Guang
中科院分区：
文献类型：
--
作者：
Chi, Jing-Qi;Gao, Wen-Kun;Liu, Chen-Guang
采用苯胺-吡咯共聚物纳米球分散钌离子，然后通过气相磷化的方法制备了包裹在均匀的N，P共掺杂空心碳纳米球（RuPx@NPC）中的RuPx纳米粒子。所制备的RuPx@NPC具有均匀的核-壳中空纳米球结构，其中RuPx NPs为核，N，P共掺杂的碳（NPC）为壳。这种策略整合了中空纳米结构的许多优点，其提供了导电基底和非金属元素的掺杂。在高温下，所获得的薄NPC壳不仅可以保护RuPx NPs的高活性相免受电解质中的聚集和腐蚀，而且还允许电子结构的变化，从而通过N，P共掺杂大大提高电荷转移速率。优化的RuPx@NPC样品在900 ℃下表现出类似Pt的析氢反应（HER）性能，并在酸性、碱性和中性溶液中具有长期耐久性。该反应在0.5 M H2SO4、1.0 M KOH和1.0 M磷酸盐缓冲盐水中分别需要51、74和110 mV的小过电位（10 mA cm-2）。本工作为通过无机-有机杂化方法设计独特的磷掺杂碳异质结构作为优良的HER电催化剂提供了一种新的途径。
RuPx nanoparticles (NPs) encapsulated in uniform N,P-codoped hollow carbon nanospheres (RuPx@NPC) have been synthesized through a facile route in which aniline-pyrrole copolymer nanospheres are used to disperse Ru ions followed by a gas phosphorization process. The as-prepared RuPx@NPC exhibits a uniform core-shell hollow nanospherical structure with RuPx NPs as the core and N,P-codoped carbon (NPC) as the shell. This strategy integrates many advantages of hollow nanostructures, which provide a conductive substrate and the doping of a nonmetal element. At high temperatures, the obtained thin NPC shell can not only protect the highly active phase of RuPx NPs from aggregation and corrosion in the electrolyte but also allows variation in the electronic structures to improve the charge-transfer rate greatly by N,P codoping. The optimized RuPx@NPC sample at 900 degrees C exhibits a Pt-like performance for the hydrogen evolution reaction (HER) and long-term durability in acidic, alkaline, and neutral solutions. The reaction requires a small overpotential of only 51, 74, and 110 mV at 10 mA cm(-2) in 0.5 M H2SO4, 1.0 M KOH, and 1.0 M phosphate-buffered saline, respectively. This work provides a new way to design unique phosphide-doped carbon heterostructures through an inorganic-organic hybrid method as excellent electrocatalysts for HER.