Yang Zi-Rui, Wang Shang-Qing, Wang Jing, Zhou Ai-Ju, Xu Chang-Wei
Guangzhou Key Laboratory for Environmentally Functional Materials and Technology, School of Chemistry and Chemical Engineering, Guangzhou University, Guangzhou, 510006, China.
Guangzhou Key Laboratory for New Energy and Green Catalysis, Guangzhou University, Guangzhou, 510006, China.
Sci Rep. 2017 Nov 13;7(1):15479. doi: 10.1038/s41598-017-15060-x.
Carbon material containing nickel, nitrogen and sulfur (Ni-NSC) has been synthesized using metal-organic frameworks (MOFs) as precursor by annealing treatment with a size from 200 to 300 nm. Pd nanoparticles supported on the Ni-NSC (Pd/Ni-NSC) are used as electrocatalysts for ethanol oxidation in alkaline media. Due to the synergistic effect between Pd and Ni, S, N, free OH radicals can form on the surface of Ni, N and S atoms at lower potentials, which react with CHCO intermediate species on the Pd surface to produce CHCOO and release the active sites. On the other hand, the stronger binding force between Pd and co-doped N and S is responsible for enhancing dispersion and preventing agglomeration of the Pd nanoparticles. The Pd(20 wt%)/Ni-NSC shows better electrochemical performance of ethanol oxidation than the traditional commercial Pd(20 wt%)/C catalyst. Onset potential on the Pd(20 wt%)/Ni-NSC electrode is 36 mV more negative compared with that on the commercial Pd(20 wt%)/C electrode. The Pd(20 wt%)/Ni-NSC in this paper demonstrates to have excellent electrocatalytic properties and is considered as a promising catalyst in alkaline direct ethanol fuel cells.
以金属有机框架材料(MOFs)为前驱体,通过退火处理合成了尺寸为200至300纳米、含有镍、氮和硫的碳材料(Ni-NSC)。负载在Ni-NSC上的钯纳米颗粒(Pd/Ni-NSC)用作碱性介质中乙醇氧化的电催化剂。由于钯与镍、硫、氮之间的协同效应,在较低电位下,镍、氮和硫原子表面可形成游离羟基自由基,这些自由基与钯表面的CHCO中间物种反应生成CHCOO并释放活性位点。另一方面,钯与共掺杂的氮和硫之间较强的结合力有助于增强钯纳米颗粒的分散性并防止其团聚。与传统的商业Pd(20 wt%)/C催化剂相比,Pd(20 wt%)/Ni-NSC表现出更好的乙醇氧化电化学性能。Pd(20 wt%)/Ni-NSC电极的起始电位比商业Pd(20 wt%)/C电极负36 mV。本文中的Pd(20 wt%)/Ni-NSC表现出优异的电催化性能,被认为是碱性直接乙醇燃料电池中有前景的催化剂。