Synthesis of a ruthenium–graphene quantum dot–graphene hybrid as a promising single-atom catalyst for electrochemical nitrogen reduction with ultrahigh yield rate and selectivity,Journal of Materials Chemistry A

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Synthesis of a ruthenium–graphene quantum dot–graphene hybrid as a promising single-atom catalyst for electrochemical nitrogen reduction with ultrahigh yield rate and selectivity
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2021-10-11 , DOI: 10.1039/d1ta07158k
Li Ruiyi ₁ , He Keyang ₁ , Xu Pengwu ₁ , Wang Wendong ₁ , Li Nana ₁ , Zhu Haiyan ₁ , Li Zaijun ₁ , Liu Xiaohao ₁

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It is impossible for the hybrid of classical graphene and metal nanoparticles to break through the limitations of their inherent properties because graphene and metal nanoparticles are conductors. This study reports the synthesis of single atom ruthenium–histidine-functionalized graphene quantum dot–graphene hybrid (Ru–His–GQD–G). His–GQD is immobilized on graphene oxide (GO) via π–π stacking and then coordinated with Ru³⁺ ions. This is followed by reduction with ascorbic acid into GO gel and annealing at 400 °C at a slow heating rate of 0.5 °C min⁻¹. The resulting Ru–His–GQD–G shows a well-defined three-dimensional structure with a high Ru loading of 5.1 wt%, in which Ru atoms are evenly dispersed on graphene sheets. The intimate contact between His–GQD and Ru atom and graphene creates double Schottky heterojunctions. Ru–His–GQD–G exhibits ultrahigh catalytic activity for electrochemical nitrogen reduction. At a low potential of −0.05 V, the NH₃ yield rate reaches 226 μg mg⁻¹ h⁻¹ with the faradaic efficiency of 42.6%, which is better than that of reported electrocatalysts for nitrogen reduction. The experimental and theoretical investigations demonstrate that the Ru sites with His–GQD are the major active centers that permit nitrogen adsorption, stabilization of *NNH and destabilization of *H. This study also provides a way for the construction of graphene-based single-atom catalysts with excellent catalytic activity.

中文翻译：

钌-石墨烯量子点-石墨烯杂化物的合成作为具有超高产率和选择性的电化学氮还原的有前途的单原子催化剂

经典的石墨烯和金属纳米粒子的混合体不可能突破其固有性质的限制，因为石墨烯和金属纳米粒子是导体。本研究报告了单原子钌-组氨酸功能化石墨烯量子点-石墨烯杂化物（Ru-His-GQD-G）的合成。His-GQD通过π-π 堆积固定在氧化石墨烯 (GO)上，然后与 Ru ³⁺离子配位。然后用抗坏血酸还原成 GO 凝胶并在 400 °C 下以 0.5 °C min ^-1的缓慢加热速率退火. 所得的 Ru-His-GQD-G 显示出明确的三维结构，Ru 负载量为 5.1 wt%，其中 Ru 原子均匀地分散在石墨烯片上。His-GQD 与 Ru 原子和石墨烯之间的密切接触产生了双肖特基异质结。Ru-His-GQD-G 对电化学氮还原表现出超高的催化活性。在-0.05 V的低电位下，NH ₃产率达到226 μg mg ^-1 h ^-1法拉第效率为 42.6%，优于报道的氮还原电催化剂。实验和理论研究表明，具有 His-GQD 的 Ru 位点是允许氮吸附、*NNH 稳定和 *H 去稳定的主要活性中心。该研究也为构建具有优异催化活性的石墨烯基单原子催化剂提供了途径。

更新日期：2021-10-27

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