Theoretical investigations on SiC2 siligraphene as promising metal-free catalyst for oxygen reduction reaction
Theoretical investigations on SiC2 siligraphene as promising metal-free catalyst for oxygen reduction reaction
复制标题
SiC2硅石墨烯作为有前景的氧还原反应无金属催化剂的理论研究
DOI：
10.1016/j.jpowsour.2015.09.014
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发表时间：
2015-12-20
影响因子：
9.2
通讯作者：
Li, Youyong
中科院分区：
文献类型：
--
作者：
Dong, Huilong;Lin, Bin;Li, Youyong
设计和发现高性能的无金属氧还原电催化材料对燃料电池的发展至关重要。通过密度泛函理论（DFT）计算，我们研究了SiC 2硅化石墨烯（g-SiC 2）作为无金属氧化还原催化剂的潜在应用。与传统的Pt（111）相比，g-SiC 2对O-2分子和其他ORR中间体具有更高的吸附亲和力，并表现出良好的抗CO中毒能力。详细的LH和ER机制，在催化ORR的g-SiC 2模拟和讨论，无论是在酸性和碱性环境。我们发现，在碱性环境中，g-SiC 2提出了一个非常低的激活势垒（0.16 eV）的速率决定步骤（RDS），并显示在平衡电位没有过电位。我们的理论模拟验证了具有交替排列的Si和C原子的siligraphene在碱性环境中具有作为ORR催化剂的巨大潜力。(C)2015 Elsevier B. V.版权所有。
The design and discovery of high-performance metal-free catalytic materials for oxygen reduction reaction (ORR) electrocatalysis is vital for the development of fuel cells. By performing density functional theory (DFT) calculations, we investigate the potential applications of SiC2 siligraphene (g-SiC2) as metal-free ORR catalyst. The g-SiC2 exhibits higher adsorption affinity for the O-2 molecule and other ORR intermediates than the traditional Pt (111), and shows good tolerance against CO poisoning. The detailed LH and ER mechanisms in catalyzing ORR by g-SiC2 are simulated and discussed, both in acidic and alkaline environment. We find that, in alkaline environment, the g-SiC2 presents a very low activation barrier (0.16 eV) for the rate determining step (RDS) and shows no overpotential at the equilibrium potential. Our theoretical simulations validate that the siligraphene with alternatively arranged Si and C atoms holds great potential as ORR catalyst in alkaline environment. (C) 2015 Elsevier B.V. All rights reserved.