Impact of electron transfer of atomic metals on adjacent graphyne layers on electrochemical water splitting,Nanoscale

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Impact of electron transfer of atomic metals on adjacent graphyne layers on electrochemical water splitting
Nanoscale ( IF 5.8 ) Pub Date : 2020/03/06 , DOI: 10.1039/c9nr10579d
Xiaoping Gao _{1,

2,

3,

4} , Liang Mei _{4,

5,

6,

7} , Yanan Zhou _{4,

8,

9,

10} , Zhemin Shen _{1,

2,

3,

4}

Affiliation

Efficient electrocatalysts are needed for both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER), while the influence of electron transfer from the adjacent layer of multilayered electrocatalysts on their catalytic performance is usually neglected. Here, we used the single cobalt atom trapped graphyne catalyst (Co@GY) to study the feasibility of modulating its water-splitting catalytic activity through interfacial electron transfer. A series of Co@GY/transition-metal doped graphyne double-layered structures (Co@GY/GY and Co@GY/TM@GY, TM = Mn, Fe, Co, Ni, Cu) are systematically evaluated for water splitting via theoretical computations. The electronic structure analyses of different stacking cases revealed that the atomic metals on the adjacent TM@GY layer remarkably tune the electronic structures of the Co atom in the Co@GY layer. A strong linear correlation between ΔG_H* and the d band center of the Co atom was found, suggesting that the HER activity on the Co atom can be tailored by adjusting the TM on the adjacent TM@GY layer with different d-electron occupations. The volcano-type trend of OER catalytic performance is obtained to show the best Co@GY/Ni@GY catalyst for the OER with an over-potential of 0.38 V, indicating that higher catalytic performance arises from moderate interfacial electron transfer. These results arouse a re-thinking of the intrinsic activity origins of single-atom catalysts (SACs) and offer a new strategy for the structure designing of SACs.

中文翻译：

原子金属电子转移到相邻石墨烯层上对电化学水分解的影响

析氢反应（HER）和析氧反应（OER）都需要高效的电催化剂，而从多层电催化剂的相邻层转移电子对其催化性能的影响通常被忽略。在这里，我们使用了单个钴原子捕获的石墨烯催化剂（Co @ GY）来研究通过界面电子转移调节其水分解催化活性的可行性。@ GY /过渡金属的一系列的Co掺杂graphyne双层结构（共@ GY / GY和Co @ GY / TM @ GY，TM =锰，铁，钴，镍，铜）的系统的评价的水分解通过理论计算。对不同堆积情况的电子结构分析表明，相邻TM @ GY层上的原子金属显着调节Co @ GY层中Co原子的电子结构。ΔG _{H *}之间的线性关系很强并发现了Co原子的d带中心，这表明可以通过调节相邻d @ GY层上具有不同d电子职业的TM来定制对Co原子的HER活性。获得了OER催化性能的火山型趋势，显示出对OER最好的Co @ GY / Ni @ GY催化剂，其过电势为0.38 V，这表明较高的催化性能来自于适度的界面电子转移。这些结果引起了对单原子催化剂（SAC）固有活性起源的重新思考，并为SAC的结构设计提供了新的策略。

更新日期：2020-04-09

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