Can Si-doped graphene activate or dissociate O2 molecule?
Can Si-doped graphene activate or dissociate O2 molecule?
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DOI：
10.1016/j.jmgm.2012.11.009
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发表时间：
2013-02-01
影响因子：
2.9
通讯作者：
Wang, Xuan-zhang
中科院分区：
文献类型：
--
作者：
Chen, Ying;Yang, Xiao-chun;Wang, Xuan-zhang
近年来，氧分子在无金属催化剂上的吸附和解离已引起广泛关注，具有重要的基础和工业意义。在本工作中，我们利用密度泛函理论计算研究了O-2分子在原始和掺杂硅的石墨烯上的吸附和解离。我们发现O-2首先通过[2+1]或[2+2]环加成吸附在硅掺杂石墨烯上，吸附能分别为-1.439和-0.856 eV。随后，分子吸附的O-2可以通过不同的途径解离。在最有利的反应路径下，由于石墨烯中掺杂了硅，吸附的O-2的解离势垒从3.180 eV显著降低到0.206 eV。我们的研究结果可能有助于进一步开发有效的无金属氧还原反应催化剂，从而大大拓宽石墨烯的潜在应用范围。(C) 2012爱思唯尔公司版权所有。
Recently, the adsorption and dissociation of oxygen molecule on a metal-free catalyst has attracted considerable attention due to the fundamental and industrial importance. In the present work, we have investigated the adsorption and dissociation of O-2 molecule on pristine and silicon-doped graphene, using density functional theory calculations. We found that O-2 is firstly adsorbed on Si-doped graphene by [2+1] or [2+2] cycloaddition, with adsorption energies of -1.439 and -0.856 eV, respectively. Following this, the molecularly adsorbed O-2 can be dissociated in different pathways. In the most favorable reaction path, the dissociation barrier of adsorbed O-2 is significantly reduced from 3.180 to 0.206 eV due to the doping of silicon into graphene. Our results may be useful to further develop effective metal-free catalysts for the oxygen reduction reactions (ORRs), thus greatly widening the potential applications of graphene. (C) 2012 Elsevier Inc. All rights reserved.