高效电催化氮还原金属有机框架的筛选

IF 3.5 3区工程技术 Q2 ENGINEERING, CHEMICAL

AIChE Journal Pub Date : 2024-12-05 DOI:10.1002/aic.18652

Jiawei Lin, Yuhang Li, Hongping Yan, Tingting Qi, Shijing Liang, Lilong Jiang

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引用次数: 0

摘要

在这项工作中，筛选了44种金属有机框架（MOFs）用于高效的电催化氮还原反应（eNRR）。用大正则蒙特卡罗方法计算了mof的44个金属活性中心的N2吸附等容热。结果表明，在所有筛选的元素中，p-块元素对N2的亲和力最高，这表明它们具有良好的eNRR催化潜力。此外，由于MIL-53 （Al）的毒性和成本相对较低，因此优先选择Al元素作为mof的金属中心。结合原位漫反射红外傅里叶变换（DRIFT）分析和理论计算，发现MIL-53 （Al）中N2主要被Al- o -Al结构的桥接氧所吸引。优化后的MIL-53 （Al）在−0.3 V下的NH3产率为74.55±1 μg h−1 mgcat−1，是目前文献报道的mof基eNRR催化剂中活性最高的。

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Screening of metal–organic frameworks for efficient electrocatalytic nitrogen reduction

In this work, 44 metal–organic frameworks (MOFs) are screened for efficient electrocatalytic nitrogen reduction reaction (eNRR). The isosteric heats of N₂ adsorption on the 44 metal active centers of MOFs are calculated by the grand canonical Monte Carlo method. It is found that p-block-elements exhibit the highest N₂ affinity among all screened elements, implying their excellent catalytic potentials for eNRR. Furthermore, the Al element is preferentially chosen as the metal center of MOFs (MIL-53 (Al)) owing to its relatively low toxicity and cost. Combined in situ Diffuse Reflectance Infrared Fourier Transform (DRIFT) analysis with theoretical calculation, we found that N₂ is mainly attracted by the bridging oxygen of Al-O-Al structure in the MIL-53 (Al). The optimized MIL-53 (Al) shows a superior activity with the NH₃ yield rate of 74.55 ± 1 μg h⁻¹ mg_cat⁻¹ at −0.3 V vs. Reversible Hydrogen Electrode (RHE), to our best knowledge, which is currently the highest activity of MOF-based catalyst for eNRR reported in the literature.

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来源期刊

AIChE Journal 工程技术-工程：化工

CiteScore

7.10

自引率

10.80%

发文量

411

审稿时长

3.6 months

期刊介绍： The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.