Substrate strain engineering: an efficient strategy to enhance the catalytic activity of SACs on waved graphene for e-NRR,Sustainable Energy & Fuels

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Substrate strain engineering: an efficient strategy to enhance the catalytic activity of SACs on waved graphene for e-NRR
Sustainable Energy & Fuels ( IF 5.0 ) Pub Date : 2020-05-14 , DOI: 10.1039/d0se00518e
Di Liu _{1,

2,

3} , Haoqiang Ai _{2,

3,

4,

5} , Wan Tong Lou _{6,

7,

8,

9} , Feifei Li _{1,

2,

3} , Kin Ho Lo _{2,

3,

4,

5} , Shuangpeng Wang _{1,

2,

3,

5,

10} , Hui Pan _{1,

2,

3,

5,

10}

Affiliation

Ammonia is an important chemical in both industry and agriculture. The production of ammonia in a green way is challenging. The electrochemical nitrogen reduction reaction (e-NRR) has been proposed for this purpose. However, this technology is still far from practical applications due to low production, which is mainly because of inefficient electrocatalysts. In this work, we have designed a series of single-atom catalysts (SACs) anchored on waved graphene (wG) for efficient e-NRR and systematically investigated the effect of curvature on the catalytic performance based on first-principles calculations. Eight SACs (V, Cr, Mn, Fe, Co, Ni, Cu, and Pt) anchored on waved graphene with various curvatures (0–50%) have been studied. We found that the curvature strongly affected the formation, catalytic activity, and selectivity of SACs for e-NRR: (1) the formation possibility of SACs on wG was considerably enhanced on increasing the curvature. (2) The free energies for the rate-determining steps of SAC-V-wG, SAC-Mn-wG, and SAC-Cr-wG were less than 1.0 eV, leading to high catalytic activity for e-NRR. In particular, SAC-Mn-wG exhibited higher activity for e-NRR than SAC-Mn on flat graphene. (3) The three systems had higher selectivity for e-NRR than for HER, which could be further improved by compression. Thus, we conclude that SAC-Mn-wG is the best SAC on wG for e-NRR because of its easy fabrication, good catalytic performance and high selectivity. We believe that our findings can provide new insights in reported experimental results and guidance for the design of novel SACs with high performance for e-NRR.

中文翻译：

底物应变工程：一种有效的策略，以增强SACs在波动石墨烯上的e-NRR催化活性

氨气在工业和农业中都是重要的化学物质。以绿色方式生产氨具有挑战性。为此已经提出了电化学氮还原反应（e-NRR）。然而，由于产量低，该技术仍与实际应用相距甚远，这主要是由于电催化剂效率低下。在这项工作中，我们设计了一系列固定在波浪形石墨烯（wG）上的单原子催化剂（SAC），以实现有效的e-NRR，并基于第一性原理计算系统地研究了曲率对催化性能的影响。研究了八种SAC（V，Cr，Mn，Fe，Co，Ni，Cu和Pt）锚定在具有不同曲率（0％至50％）的波浪形石墨烯上。我们发现曲率强烈影响SAC对e-NRR的形成，催化活性和选择性：（1）随着曲率的增加，SAC在wG上形成的可能性大大提高。（2）用于SAC-V-wG，SAC-Mn-wG和SAC-Cr-wG的速率确定步骤的自由能小于1.0eV，导致对e-NRR的高催化活性。尤其是，SAC-Mn-wG在平面石墨烯上的e-NRR活性高于SAC-Mn。（3）这三种系统对e-NRR的选择性高于对HER的选择性，可以通过压缩进一步提高。因此，我们得出结论，对于e-NRR，SAC-Mn-wG是wG上最好的SAC，因为它易于制造，良好的催化性能和高选择性。我们相信，我们的发现可以为报告的实验结果提供新的见解，并为设计具有高性能e-NRR的新型SAC提供指导。

更新日期：2020-06-30

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