Electronic structural descriptors for hydrogen evolution and superior catalytic activity of graphene based structures
Electronic structural descriptors for hydrogen evolution and superior catalytic activity of graphene based structures
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用于析氢的电子结构描述符和基于石墨烯的结构的优异催化活性
DOI：
10.1016/j.apsusc.2021.151009
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发表时间：
2021-08
影响因子：
6.7
通讯作者：
Li Xi-Bo
中科院分区：
文献类型：
--
作者：
Huang Bo-Ying;Yu Guang-Qiang;Yin Wen-Jin;Zheng Feipeng;Li Xi-Bo
在催化剂中引入缺陷和基质是设计非均相催化剂的两种可行途径。识别和理解催化表面的原子、电子结构和吸附物结合能力之间的关系是至关重要的。本文以二维Mo 2C为衬底，在不同缺陷的石墨烯上的氢析出为例，探讨了它们之间的关系。从缺陷和衬底支撑的石墨烯的电子性质中提取了三个可行的电子结构描述符，包括局域原子的pandpz带中心、电子向局域原子的转移和复合结构的形变电荷密度.结果表明，这些描述符可以定量预测氢的结合能，定性预测氢的吸附顺序。定域能带中心的描述符来源于位原子与吸附质的杂化。原子结构、电子结构与结合能的关系可以应用于其它表面，并有助于揭示结构-活性的本质根源。通过对缺陷或衬底原子结构的调整，可以获得合适的氢结合能力和上级析氢性能。基于石墨烯的几种结构具有上级的析氢活性：S3 NV 1-G、S2 NV 2-G@Mo2C、N1-G@Mo2C和N2-G@Mo2C的交换电流密度分别预测为0.811、0.963、0.712和1.860 mA/cm 2。特别是后两种化合物，它们的负界面结合能和形成N1和N2缺陷的能量可互换性，保证了它们的稳定性和实验上的易合成性，增强了它们的潜在应用。
Defect and substrate introduced into catalyst are two feasible routes toward design of heterogeneous catalysts. It is vital to identify and understand the relationships among atomic, electronic structures and adsorbate binding ability of the catalytic surfaces. Herein, hydrogen evolution on different defect graphene with and without two-dimensional (2D) Mo2C substrate are selected as examples to explore the relationships. Three feasible electronic structural descriptors, includingpandpzband centers of local atoms, electron transfer to local atoms, and deformation charge densities of composite structures, are exacted from electronic properties of the defect and substrate-supported graphene. It is found that those descriptors could predict the hydrogen binding energy quantitatively, and the hydrogen adsorption order qualitatively. The descriptor of localpandpzband centers originate from hybridization between the site atom and adsorbate. It is believed that the relationship of atomic structure, electronic structure and binding energy may be applied to other surfaces, and shed light on the nature origin of the structure–activity on electrochemistry. By tuning the descriptors by atomic structure of defect or substrate, suitable hydrogen binding ability and superior hydrogen evolution performance of graphene could be achieved. Several structures based on graphene own superior hydrogen evolution activity: the exchange current densities of S3NV1-G, S2NV2-G@Mo2C, N1-G@Mo2C, and N2-G@Mo2C are predicted to be 0.811, 0.963, 0.712, and 1.860 mA/cm2, respectively. Especially the last two ones, their negative interfacial binding energies, and the energy favorability of forming N1and N2defects, ensure their stabilities and easy syntheses in experiment, and enhance their potential applications.
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