氮化锰催化剂在温和条件下合成氨中的应用

IF 13.1 1区 化学 Q1 CHEMISTRY, PHYSICAL
Weiye Qu, Pranav Roy, Canhui Wang, Lu Ma, Fan Bu, Xinsui Zhang, Zimin He, Michael Tsapatsis, Brandon C. Bukowski* and Chao Wang*, 
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引用次数: 0

摘要

开发先进的氨(NH3)合成催化材料对于提高工业Haber-Bosch工艺的能源效率至关重要。本文报道了一种用于低温NH3合成的ζ相氮化锰(MnN0.43)催化剂。合成的MnN0.43催化剂由碳壳保护,允许在环境条件下存储和处理空气敏感金属氮化物。原位活化后,MnN0.43催化剂在250 ~ 350℃条件下具有较高的NH3合成活性,优于传统的贵金属Ru/MgO催化剂。动力学、化学吸附、同位素标记和计算研究的结合表明,氮空位介导的结合机制解释了催化增强。我们的工作强调了地球上丰富的过渡金属氮化物在催化温和条件NH3合成方面的巨大潜力。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Earth-Abundant Manganese Nitride Catalysts for Mild-Condition Ammonia Synthesis

Earth-Abundant Manganese Nitride Catalysts for Mild-Condition Ammonia Synthesis

Developing advanced catalytic materials for mild-condition ammonia (NH3) synthesis is essential for improving the energy efficiency of the industrial Haber-Bosch process. Here, we report a ζ-phase manganese nitride (MnN0.43) catalyst for low-temperature NH3 synthesis. The as-synthesized MnN0.43 catalyst is protected by a carbon shell, allowing for the storage and processing of the air-sensitive metal nitride under ambient conditions. After activation in situ, the MnN0.43 catalyst exhibits high activity for NH3 synthesis at 250–350 °C, surpassing the conventional noble metal based Ru/MgO catalyst. A combination of kinetic, chemisorption, isotope labeling and computational studies indicate that a nitrogen vacancy-mediated associative mechanism accounts for the catalytic enhancements. Our work highlights the great potential of earth-abundant transition metal nitrides for catalyzing mild-condition NH3 synthesis.

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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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