Enhanced N2 Adsorption and Activation by Combining Re Clusters and In Vacancies as Dual Sites for Efficient and Selective Electrochemical NH3 Synthesis,Nano Letters

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Enhanced N2 Adsorption and Activation by Combining Re Clusters and In Vacancies as Dual Sites for Efficient and Selective Electrochemical NH3 Synthesis
Nano Letters ( IF 9.6 ) Pub Date : 2024-01-03 , DOI: 10.1021/acs.nanolett.3c04416
Shaoquan Li _{1,

2} , Yi-Tao Liu ₃ , Yong-Chao Zhang ₁ , Yue Du ₁ , Jian Gao ₁ , Jingru Zhai ₄ , Yue Liang ₁ , Caidi Han ₁ , Xiao-Dong Zhu ₁

Affiliation

The electrochemical N₂ reduction reaction (NRR) is a green and energy-saving sustainable technology for NH₃ production. However, high activity and high selectivity can hardly be achieved in the same catalyst, which severely restricts the development of the electrochemical NRR. In₂Se₃ with partially occupied p-orbitals can suppress the H₂ evolution reaction (HER), which shows excellent selectivity in the electrochemical NRR. The presence of V_In can simultaneously provide active sites and confine Re clusters through strong charge transfer. Additionally, well-isolated Re clusters stabilized on In₂Se₃ by the confinement effect of V_In result in Re-V_In active sites with maximum availability. By combining Re clusters and V_In as dual sites for spontaneous N₂ adsorption and activation, the electrochemical NRR performance is enhanced significantly. As a result, the Re-In₂Se₃-V_In/CC catalyst delivers a high NH₃ yield rate (26.63 μg h^–1 cm^–2) and high FEs (30.8%) at −0.5 V vs RHE.

中文翻译：

通过结合 Re 团簇和空位作为双位点增强 N2 吸附和活化，实现高效、选择性电化学 NH3 合成

电化学N ₂还原反应(NRR)是一种绿色、节能、可持续的NH ₃生产技术。然而，在同一催化剂中很难同时实现高活性和高选择性，这严重限制了电化学NRR的发展。在₂ Se ₃中，部分占据的p轨道可以抑制H ₂析出反应(HER)，这在电化学NRR中表现出优异的选择性。 V _In的存在可以同时提供活性位点并通过强电荷转移限制 Re 团簇。此外，通过 V _In的限制效应，隔离良好的 Re 团簇稳定在 In ₂ Se ₃上，导致 Re-V _In活性位点具有最大的可用性。通过将Re簇和V _In结合作为自发N ₂吸附和活化的双位点，电化学NRR性能显着增强。因此，Re-In ₂ Se ₃ -V _In /CC 催化剂在 -0.5 V vs RHE 条件下具有高 NH ₃收率（26.63 μg h ^–1 cm ^–2 ）和高 FE（30.8%）。

更新日期：2024-01-03

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