Screening of metal–organic frameworks for efficient electrocatalytic nitrogen reduction

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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Abstract

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.