DFT Study of Hydrogen Storage by Spillover on Graphene with Boron Substitution
DFT Study of Hydrogen Storage by Spillover on Graphene with Boron Substitution
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DOI：
10.1021/jp200038b
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发表时间：
2011-04
影响因子：
3.7
通讯作者：
Hong-Yu Wu;Xiaofeng Fan;J. Kuo;Weiqiao Deng
中科院分区：
文献类型：
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作者：
Hong-Yu Wu;Xiaofeng Fan;J. Kuo;Weiqiao Deng
通过第一性原理计算研究了硼掺杂石墨烯上的氢溢出机制。通过在石墨烯中掺入硼，我们的理论研究表明，B掺杂可以显著增强H原子和金属团簇在衬底上的吸附强度。B掺杂石墨烯上牢固结合的催化金属可以有效地将H2分子解离成H原子，并且H原子更可能从H饱和金属的桥位迁移到支撑石墨烯片上。对BC 3片的进一步研究给出了H迁移和扩散过程的足够低的活化势垒;因此，与未掺杂的石墨烯情况相比，预期在环境条件下更多的H原子通过H溢出吸附在BC 3衬底上。我们的结果与最近的实验结果一致，微孔碳通过硼取代具有增强的吸氢能力，这意味着B掺杂与溢出是一种有效的方法。
The hydrogen spillover mechanism on B-doped graphene was explicitly investigated by first-principles calculations. By the incorporation of boron into graphene, our theoretical investigation shows that B doping can substantially enhance the adsorption strength for both H atoms and the metal cluster on the substrate. The firmly bound catalytic metal on B-doped graphene can effectively dissociate H2 molecules into H atoms, and the H atom is more likely to migrate from the bridge site of the H-saturated metal to the supporting graphene sheet. Further investigation on the BC3 sheet gives sufficiently low activation barriers for both H migration and diffusion processes; thus, more H atoms are expected to adsorb on BC3 substrate via H spillover under ambient conditions compared with the undoped graphene case. Our result is in good agreement with recent experimental findings that microporous carbon has an enhanced hydrogen uptake via boron substitution, implying that B doping with spillover is an effective approa...