Well-dispersed pyrite-type RuS2 nanocrystals anchored on porous nitrogen and sulfur co-doped hollow carbon spheres for enhanced alkaline hydrogen evolution
Well-dispersed pyrite-type RuS2 nanocrystals anchored on porous nitrogen and sulfur co-doped hollow carbon spheres for enhanced alkaline hydrogen evolution
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DOI：
10.1016/j.cej.2021.129318
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发表时间：
2021-03
影响因子：
15.1
通讯作者：
Yujun Xu;Cuicui Du;Qi Shen;Junlin Huang;Xiaohua Zhang;Jinhua Chen
中科院分区：
文献类型：
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作者：
Yujun Xu;Cuicui Du;Qi Shen;Junlin Huang;Xiaohua Zhang;Jinhua Chen
在碱性条件下，放氢反应(HER)活性普遍受到抑制，这是由于与水解离相关的Volmer过程迟缓。因此，开发新的高活性和低成本的碱性制氢电催化剂是实现工业装置可持续水分离的迫切需要。黄铁矿型RuS2是一种很有潜力的碱性HER电催化剂，但相关研究尚处于起步阶段。本论文以氮硫共掺杂中空碳球(NSC)为载体，制备了分散良好的纳米RuS2纳米粒子(c-RuS2NPs)，并对其进行了电催化。掺杂氮、硫的导电多孔中空碳球作为载体，提供了丰富的锚定中心，改变了RuS2的电子结构，有利于增加活性中心，提高本征活性。此外，硫化Ru的结晶度调节也对其活性有显著影响。在1.0MKOH溶液中，c-RuS2NPs/Nsc催化剂表现出良好的电催化活性，在电流密度为10 mA/cm−2时，过电位为11 mV，Tafel斜率为35.4mV/−1。与商品铂/碳和已报道的硫化Ru基电催化剂相比，c-RuS2NPs/Nsc催化剂在碱性介质中具有更好的析氢性能。
The hydrogen evolution reaction (HER) activity in alkaline condition is generally suppressed due to sluggish water dissociation–related Volmer process. Consequently, developing new highly-active and cost-efficient electrocatalysts for the alkaline hydrogen production is greatly desirable for achieving sustainable water splitting in industrial plants. Pyrite-type RuS2is a potential excellent electrocatalyst for alkaline HER but the related research is still in its infancy. Herein, well-dispersed crystalline RuS2nanoparticles (c-RuS2NPs) with ultrasmall particle size anchored on porous nitrogen and sulfur co-doped hollow carbon spheres (NSC) are synthesized for alkaline HER electrocatalysis. The conductive and porous hollow carbon spheres with nitrogen and sulfur doping is used as the effective support to provide abundant anchoring sites and modify the electronic structure of RuS2, beneficial to increasing the active sites and improving the intrinsic activity. Furthermore, the crystallinity modulation of ruthenium sulfide also has a significant impact on HER activity. In 1.0 M KOH solution, the proposed c-RuS2NPs/NSC catalyst exhibits admirable activity for HER electrocatalysis with a low overpotential of 11 mV at a current density of 10 mA cm−2and a small Tafel slope of 35.4 mV dec−1. With low Ru loading, superior hydrogen evolution in alkaline media is achieved for c-RuS2NPs/NSC compared to the commercial Pt/C and the reported ruthenium-sulfide-based electrocatalysts.