Monolayer triphosphates MP3 ( M = Sn, Ge) with excellent basal catalytic activity for hydrogen evolution reaction
Monolayer triphosphates MP3 ( M = Sn, Ge) with excellent basal catalytic activity for hydrogen evolution reaction
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单层三磷酸盐 MP3 ( M = Sn, Ge) 对析氢反应具有优异的基础催化活性
DOI：
10.1039/c9nr03255j
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发表时间：
2019
期刊：
影响因子：
6.7
通讯作者：
Zeng Xiao Cheng
中科院分区：
文献类型：
--
作者：
Wu Hong Hui;Huang He;Zhong Jie;Yu Song;Zhang Qiaobao;Zeng Xiao Cheng
原子厚度的二维材料由于其新颖的性质和在纳米器件中的应用前景而受到人们的广泛关注。采用密度泛函理论（DFT）方法研究了几种新预测的二维三磷化物GeP3、SnP3和InP3单分子膜对析氢反应的催化活性.计算结果表明，GeP3和SnP3单分子膜具有较好的氢吸附自由能，是HER的活性催化剂。特别地，GeP3的氢吸附吉布斯自由能（ΔGH*）为0.024 eV，与贵金属（PGM）催化剂Pt相比，该值甚至更有利。此外，2D GeP3和SnP3与石墨烯衬底本质上相容，使得HER性能可以通过与石墨烯片构建混合多层来改善。从GeP3或SnP3到石墨烯的电荷转移（估计为0.1278e或0.2157e）可以显著提高电导率并促进电催化活性。虽然GeP3和SnP3的电子能带结构可以通过外部应变来调节，但我们发现GeP3和SnP3单层的HER性能实际上对外部应变不敏感，这是催化应用所需的特征。具有几乎为零的吉布斯自由能的HER的理想性质使得2D GeP3和SnP3有希望成为未来在电催化中应用的候选者。
Atomically thin two-dimensional (2D) materials have received intense research interest due to their novel properties and promising applications in nanodevices. By using density functional theory (DFT) calculations, we investigate catalytic activities of several newly predicted two-dimensional (2D) triphosphides GeP3, SnP3 and InP3 monolayers for hydrogen evolution reaction (HER). The calculation results show that GeP3 and SnP3 monolayers are active catalysts for HER with suitable free energy of hydrogen adsorption in the basal plane. In particular, the Gibbs free energy of hydrogen adsorption (ΔGH*) of GeP3 is 0.024 eV, a value even more favorable compared to the precious-group-metal (PGM) catalyst Pt. Moreover, the 2D GeP3 and SnP3 are intrinsically compatible with the graphene substrate so that the HER performance can be improved via building a hybrid multilayer with graphene sheet. The charge transfer from GeP3 or SnP3 to graphene, estimated to be 0.1278e or 0.2157e, can significantly enhance the electric conductivity and promote the electrocatalytic activity. Although the electronic band structure of GeP3 and SnP3 can be tuned by external strain, we find that the HER performance of GeP3 and SnP3 monolayer is actually insensitive to the external strain, a feature desirable for the catalytic application. The desirable properties for HER with nearly zero Gibbs free energy render 2D GeP3 and SnP3 promising candidates for future application in electrocatalysis.