用于电催化氮还原的单 Ru-N4 位点嵌入多孔碳,ACS Applied Materials & Interfaces

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用于电催化氮还原的单 Ru-N4 位点嵌入多孔碳
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-03-01 , DOI: 10.1021/acsami.2c21744
Zhiya Han _{1,

2} , Senhe Huang _{2,

3} , Jichao Zhang ₄ , Fu Wang ₅ , Sheng Han ₆ , Peng Wu ₁ , Mingyuan He ₁ , Xiaodong Zhuang _{2,

3}

Affiliation

氨是化学品、化肥和储能的有效原料。相对于传统的 Haber-Bosch 方法，电催化氮还原反应 (NRR) 是一种替代的、高效的、清洁的氨生产技术。单金属催化剂在 NRR 领域得到广泛研究。然而，关于如何精确调节单金属原子位点的配位环境以提高催化 NRR 性能的结论非常有限。在此，我们报告了一种 5,7 元碳环参与的多孔碳 (PC) 制备方法，用于单原子 Ru 嵌入 PC。作为电催化剂，此类材料表现出令人惊讶的有前途的催化 NRR 特性，NH ₃产率高达 67.8 ± 4.9 μg h ^–1 mg _cat^–1法拉第效率为 19.5 ± 0.6%，超过了大多数报道的单原子 NRR 催化剂。扩展的 X 射线吸收精细结构表明，拓扑缺陷的存在使 Ru-N 键从 1.48 增加到 1.56 Å，从而调节了单原子 Ru 活性位点的配位环境。_{密度泛函理论计算结果表明，N 2}的吸附到被拓扑缺陷包围的单原子 Ru 上，将 N≡N 键扩展到 1.146 Å，削弱了 N≡N 的强度并使其易受 NRR 的影响。总而言之，这项工作提供了一种新的设计策略，通过涉及拓扑缺陷和相应的围绕 Ru 单原子的大极化来提高催化 NRR 性能。这样的概念也可以应用于许多其他类型的能量存储和转换催化剂。

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Single Ru–N4 Site-Embedded Porous Carbons for Electrocatalytic Nitrogen Reduction

Ammonia is an effective feedstock for chemicals, fertilizers, and energy storage. The electrocatalytic nitrogen reduction reaction (NRR) is an alternative, efficient, and clean technology for ammonia production, relative to the traditional Haber–Bosch method. Single-metal catalysts are widely studied in the field of NRR. However, very limited conclusions have been made on how to precisely modulate the coordination environment of the single-metal-atom sites to boost catalytic NRR performance. Herein, we report a 5,7-membered carbon ring-involved porous carbon (PC) preparation toward single-atom Ru-embedded PCs. As electrocatalysts, such materials exhibit surprisingly promising catalytic NRR properties with an NH₃ yield rate of up to 67.8 ± 4.9 μg h^–1 mg_cat^–1 and a Faradaic efficiency of 19.5 ± 0.6%, exceeding those of most of the reported single-atom NRR catalysts. Extended X-ray absorption fine structure demonstrates that the presence of topological defects increases the Ru–N bond from 1.48 to 1.56 Å, modulating the coordination environment of the single-atom Ru active sites. Density functional theory-calculated results demonstrate that the adsorption of N₂ onto single-atom Ru surrounded by topological defects extends the N≡N bond to 1.146 Å, weakening the strength of N≡N and making it susceptible to the NRR. All in all, this work provides a new design strategy by involving topological defects and corresponding large polarization around the Ru single atom to boost the catalytic NRR performance. Such a concept can also be applied to many other kinds of catalysts for energy storage and conversion.

更新日期：2023-03-01

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