Guo Xiaomeng, Duan Xiaoguang, Ji Junyi, Fan Xiaobin, Li Yang, Zhang Fengbao, Zhang Guoliang, Zhu Yi-An, Peng Wenchao, Wang Shaobin
School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China.
School of Chemical Engineering, The University of Adelaide, Adelaide, SA 5005, Australia.
J Colloid Interface Sci. 2021 Feb 1;583:139-148. doi: 10.1016/j.jcis.2020.09.053. Epub 2020 Sep 23.
A rational design of electrode materials with both high electron conductivity and abundant of catalytic sites is essential for high-performance electrochemical reactions. Herein, a nitrogen and sulfur co-doped graphene (SNG) anchored on the interconnected conductive graphite foam (GF) is fabricated via drop-casting and in situ annealing. The SNG flakes are tightly immobilized on the GF surface, which can provide fast electron transfer rate and large electrolyte/electrode interfaces. The SNG@GF composite can be directly used as a free-standing electrode for electro-catalytic degradation of organic pollutants and overall water splitting. SNG@GF significantly enhanced the electrochemical activation of peroxymonosulfate (PMS) for catalytic oxidation. During the oxygen evolution reaction (OER), the SNG@GF exhibits an initial overpotential of 330 mV vs. RHE at 10 mA cm with a Tafel slope of 149 mV dec in 1 M KOH, which outperforms most of the reported metal-free catalysts. The density functional theory calculations are also used to unveil the S, N dual doping effects of carbon materials and their synergy in carbocatalysis. This study dedicates to developing multi-functional carbocatalysts for environmental and energy applications, and enables insights into carbocatalysis in electrochemistry.
设计兼具高电子导电性和丰富催化位点的电极材料对于高性能电化学反应至关重要。在此,通过滴铸法和原位退火制备了一种锚定在相互连接的导电石墨泡沫(GF)上的氮硫共掺杂石墨烯(SNG)。SNG薄片紧密固定在GF表面,可提供快速的电子转移速率和较大的电解质/电极界面。SNG@GF复合材料可直接用作自支撑电极,用于电催化降解有机污染物和全水解。SNG@GF显著增强了过一硫酸盐(PMS)的电化学活化以进行催化氧化。在析氧反应(OER)过程中,SNG@GF在1 M KOH中,在10 mA cm时相对于可逆氢电极(RHE)的初始过电位为330 mV,塔菲尔斜率为149 mV dec,优于大多数已报道的无金属催化剂。密度泛函理论计算还用于揭示碳材料的S、N双掺杂效应及其在碳催化中的协同作用。本研究致力于开发用于环境和能源应用的多功能碳催化剂,并深入了解电化学中的碳催化。