共掺杂促进了Mo2N-Co催化剂上的等离子体催化合成氨

IF 4.5 3区 工程技术 Q2 ENGINEERING, CHEMICAL
Yutong Feng, Bianbian Gao, Guoqiang Cao, Donghai Hu, Yuting Jiao, Chunyu Li, Jiantao Zhao, Yitian Fang
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引用次数: 0

摘要

氨因其高氢密度(17.8 wt %)和温和的液化条件而成为一种很有前途的储氢载体。等离子体催化合成氨是一种环境条件下绿色合成氨的替代合成途径。在本研究中,开发了共掺杂Mo2N-Co催化剂来增强等离子体催化合成氨,重点研究了Co/Mo摩尔比和操作参数的影响。在所测试的催化剂中,Mo2N-Co1具有最高的合成氨速率和能效。最佳操作条件包括N2:H2 = 1:1的进料比和较高的放电功率。以Mo2N-Co1为原料,在N2:H2 = 1:1的进料比和57 W的放电功率下,氨合成速率为11925µmol·g−1·h−1,能量效率为3.6 g- nh3·kWh−1。x射线衍射、透射电镜、x射线光电子能谱、电子顺磁共振、氢程序升温还原、氨程序升温脱附等综合表征表明,Co掺杂引入了丰富的氮空位和弱酸性表面,有利于氨的脱附和电子转移。利用光学发射光谱确定了关键的反应中间体,为Mo2N-Co催化剂协同等离子体催化合成氨的反应机制提供了深入的见解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Co-doping facilitated plasma-catalytic ammonia synthesis over Mo2N-Co catalysts

Ammonia is a promising hydrogen storage carrier due to its high hydrogen density (17.8 wt %) and mild liquefaction conditions. Plasma-catalytic ammonia synthesis is an alternative synthesis route regarding green ammonia generation at ambient conditions. In this study, Co-doped Mo2N-Co catalysts were developed to enhance plasma-catalytic ammonia synthesis, with a focus on the effects of Co/Mo molar ratios and operating parameters. Among the catalysts tested, Mo2N-Co1 possessed the highest ammonia synthesis rate and energy efficiency. Optimal operating conditions including a feed ratio of N2:H2 = 1:1 and a higher discharge power is favored. An ammonia synthesis rate of 11925 µmol·g−1·h−1 and an energy efficiency of 3.6 g-NH3·kWh−1 were achieved over Mo2N-Co1 at a feed ratio of N2:H2 = 1:1 and a discharge power of 57 W. Comprehensive characterizations, including X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, electron paramagnetic resonance, hydrogen temperature-programmed reduction, and ammonia temperature-programmed desorption, demonstrated that Co doping introduced abundant nitrogen vacancies and weak acidic surface, both of which facilitated ammonia desorption and electron transfer. Key reactive intermediates were identified using optical emission spectroscopy, providing insight into the proposed reaction mechanism for this synergistic plasma-catalytic ammonia synthesis over Mo2N-Co catalysts.

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来源期刊
CiteScore
7.60
自引率
6.70%
发文量
868
审稿时长
1 months
期刊介绍: Frontiers of Chemical Science and Engineering presents the latest developments in chemical science and engineering, emphasizing emerging and multidisciplinary fields and international trends in research and development. The journal promotes communication and exchange between scientists all over the world. The contents include original reviews, research papers and short communications. Coverage includes catalysis and reaction engineering, clean energy, functional material, nanotechnology and nanoscience, biomaterials and biotechnology, particle technology and multiphase processing, separation science and technology, sustainable technologies and green processing.
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