Effective Electrochemical Nitrogen Reduction through π Back-donation Process in Mn3+ of Mn-doped g-C3N4

IF 2.3 4区 化学 Q3 CHEMISTRY, PHYSICAL Catalysis Letters Pub Date : 2024-07-08 DOI:10.1007/s10562-024-04772-1
Yijin Ma, Yinpeng Lu, Chang Li, Liangqing Hu, Hexin Zhang, Jing Feng
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Abstract

Ammonia (NH3) synthesis via nitrogen reduction reaction under mild conditions is challenging due to the difficulty of activating nitrogen. Herein, Mn-doped g-C3N4 (x-Mn-CN, x = 5, 10, and 15) catalysts with efficiency NRR performance were synthesized. The resulting 5-Mn-CN exhibits higher NRR performance (NH3 yield rate: 15.2 μg h−1 mgcat−1, Faradaic efficiency: 7.1%) at -0.4 V (vs. RHE) than others. It is found that the active sites of Mn3+ are generated by electron transfer from Mn2+ to the N of g-C3N4, and active N2 through the π back-donation process. This is evidenced by the experimental result that the NH3 yield rate of 5-Mn-CN significantly decreases from 15.2 μg h−1 mgcat−1 to 2.6 μg h−1 mgcat−1 after lowering the concentration of Mn3+. The concentration of Mn3+ is reduced by treating the catalyst in the ethylenediaminetetraacetic acid disodium salt (EDTA-2Na) solution. This study enhances the understanding of N2 activation and provides insights into the transition metal-doped g-C3N4 as NRR catalysts.

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通过掺杂锰的 g-C3N4 中 Mn3+ 的 π 背负过程实现有效的电化学氮还原
由于氮难以活化,在温和条件下通过氮还原反应合成氨(NH3)具有挑战性。在此,我们合成了具有高效 NRR 性能的掺锰 g-C3N4(x-Mn-CN,x = 5、10 和 15)催化剂。与其他催化剂相比,5-Mn-CN 在-0.4 V(相对于 RHE)电压下表现出更高的 NRR 性能(NH3 产率:15.2 μg h-1 mgcat-1,Faradaic 效率:7.1%)。研究发现,Mn3+ 的活性位点是通过 Mn2+ 与 g-C3N4 的 N 之间的电子转移产生的,而活性 N2 则是通过 π 反向捐赠过程产生的。实验结果表明,降低 Mn3+ 浓度后,5-Mn-CN 的 NH3 产率从 15.2 μg h-1 mgcat-1 显著降至 2.6 μg h-1 mgcat-1。在乙二胺四乙酸二钠盐(EDTA-2Na)溶液中处理催化剂可降低 Mn3+ 的浓度。这项研究加深了人们对 N2 活化的理解,并为过渡金属掺杂的 g-C3N4 作为 NRR 催化剂提供了深入的见解。
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来源期刊
Catalysis Letters
Catalysis Letters 化学-物理化学
CiteScore
5.70
自引率
3.60%
发文量
327
审稿时长
1 months
期刊介绍: Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.
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