超薄 BN-Fe-Graphene 夹层结构中的温和极化电场可实现高效氮还原

IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Chinese Journal of Catalysis Pub Date : 2024-10-01 DOI:10.1016/S1872-2067(24)60114-2
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引用次数: 0

摘要

电催化 N2 还原反应(NRR)有望取代传统的 Haber-Bosch 技术,在环境条件下生产 NH3。电化学 NRR 的活性和选择性受限于催化剂诱导的强极化电场、正确的电子转移方向以及裸电极和活性位点之间的电子隧道距离。通过将化学气相沉积法与聚甲基丙烯酸甲酯转移法相耦合,制备出了一种用于电催化 NRR 的超薄夹层催化剂,即夹在超薄(电子隧道距离内)BN(催化剂层)和石墨烯薄膜(导电层)之间的铁原子(极化电场层)。夹层催化剂不仅能在外加电压下控制电子按正确方向转移到 BN 表面,还能在不暴露金属的情况下构建中性极化电场,从而抑制氢演化反应。夹层电催化剂 NRR 系统的 NH3 产率达到 8.9 μg h-1 cm-2,法拉第效率达到 21.7%。实验和密度泛函理论模拟研究了三种夹层催化剂(BN-Fe-G、BN-Fe-BN 和 G-Fe-G)在电催化 NRR 过程中对 N2 的吸附、活化和极化电场变化。在外加电压的驱动下,BN-Fe-G 诱导的中性极化电场导致了电催化 NRR 的高活性。
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Mild polarization electric field in ultra-thin BN-Fe-graphene sandwich structure for efficient nitrogen reduction
The electrocatalytic N2 reduction reaction (NRR) is expected to supersede the traditional Haber-Bosch technology for NH3 production under ambient conditions. The activity and selectivity of electrochemical NRR are restricted to a strong polarized electric field induced by the catalyst, correct electron transfer direction, and electron tunneling distance between bare electrode and active sites. By coupling the chemical vapor deposition method with the poly(methyl methacylate)-transfer method, an ultrathin sandwich catalyst, i.e., Fe atoms (polarized electric field layer) sandwiched between ultrathin (within electron tunneling distance) BN (catalyst layer) and graphene film (conducting layer), is fabricated for electrocatalytic NRR. The sandwich catalyst not only controls the transfer of electrons to the BN surface in the correct direction under applied voltage but also suppresses hydrogen evolution reaction by constructing a neutral polarization electric field without metal exposure. The sandwich electrocatalyst NRR system achieve NH3 yield of 8.9 μg h−1 cm−2 and Faradaic Efficiency of 21.7%. The N2 adsorption, activation, and polarization electric field changes of three sandwich catalysts (BN-Fe-G, BN-Fe-BN, and G-Fe-G) during the electrocatalytic NRR are investigated by experiments and density functional theory simulations. Driven by applied voltage, the neutral polarized electric field induced by BN-Fe-G leads to the high activity of electrocatalytic NRR.
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来源期刊
Chinese Journal of Catalysis
Chinese Journal of Catalysis 工程技术-工程:化工
CiteScore
25.80
自引率
10.30%
发文量
235
审稿时长
1.2 months
期刊介绍: The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.
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