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Ni-loaded Co-NC catalysts for promoting electrocatalytic nitrate reduction to ammonia
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2024-08-20 , DOI: 10.1039/d4cy00942h Fang Zhao, Yidi Liu, Chengjie Li, Zhen Yuan, Qianqian Hua, Liguo Gao, Xuefeng Ren, Peixia Yang, Anmin Liu
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2024-08-20 , DOI: 10.1039/d4cy00942h Fang Zhao, Yidi Liu, Chengjie Li, Zhen Yuan, Qianqian Hua, Liguo Gao, Xuefeng Ren, Peixia Yang, Anmin Liu
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The Haber–Bosch process, the traditional method of ammonia synthesis, uses hydrogen derived from steam reforming of hydrocarbons; and involves harsh operating conditions of high temperatures (300–600 °C) and pressures (200–400 atm), expending a vast amount of energy each year. Recently, there has been a lot of interest in the electrochemical nitrogen reduction process (NRR) to NH3, which is inspired by natural microbial nitrogen fixation. However, the stable N
N violent hydrogen evolution reaction hindered the development of the NRR. In comparison, the electrocatalytic nitrate reduction reaction (NO3RR) has significant advantages. The much lower dissociation energy of N
O (204 kJ mol−1) is required; nitrate is widespread in surface water. Herein, an electrocatalyst loaded with Ni onto CoZn@ZIF by a simple impregnation method is reported, which possesses a nitrogen-doped graphitic carbon structure after pyrolytic carbonization. Detailed experiments showed that the NiCo-NC catalyst significantly accelerated the NO3RR compared to Co-NC. NiCo-NC exhibited remarkable NO3RR activity. At −0.6 V and −1.1 V, ammonia yields of 5.01 mg cm−2 h−1 and 10.12 mg cm−2 h−1 were obtained, with FEs reaching 92.75% and 96.65%, respectively. The catalyst showed excellent electrochemical stability in 24-hour electrolysis experiments and five-cycle stability tests. Meanwhile, 15N isotope labeling experiments further verified the source of N in NH4+ from NO3−.
中文翻译:
负载镍的Co-NC催化剂促进电催化硝酸盐还原成氨
哈伯-博世工艺是传统的氨合成方法,使用来自碳氢化合物蒸汽重整的氢气;并且涉及高温(300-600°C)和高压(200-400 atm)的恶劣工作条件,每年消耗大量能源。最近,人们对受自然微生物固氮作用启发的电化学氮还原过程(NRR)生成NH 3产生了很大的兴趣。然而,稳定的N
N剧烈的析氢反应阻碍了NRR的发展。相比之下,电催化硝酸盐还原反应(NO 3 RR)具有显着的优势。 N 的解离能低得多
需要O (204 kJ mol -1 );硝酸盐广泛存在于地表水中。本文报道了一种通过简单的浸渍方法将Ni负载到CoZn@ZIF上的电催化剂,该催化剂在热解碳化后具有氮掺杂的石墨碳结构。详细的实验表明,与Co-NC相比,NiCo-NC催化剂显着加速了NO 3 RR。 NiCo-NC表现出显着的NO 3 RR活性。在-0.6 V和-1.1 V下,氨收率分别为5.01 mg cm -2 h -1和10.12 mg cm -2 h -1 ,FE分别达到92.75%和96.65%。该催化剂在24小时电解实验和五次循环稳定性测试中表现出优异的电化学稳定性。 同时, 15 N同位素标记实验进一步验证了NH 4 +中N的来源为NO 3 - 。
更新日期:2024-08-20
![[triple bond, length as m-dash]](https://www.rsc.org/images/entities/char_e002.gif)
![[double bond, length as m-dash]](https://www.rsc.org/images/entities/char_e001.gif)
中文翻译:
![](https://scdn.x-mol.com/jcss/images/paperTranslation.png)
负载镍的Co-NC催化剂促进电催化硝酸盐还原成氨
哈伯-博世工艺是传统的氨合成方法,使用来自碳氢化合物蒸汽重整的氢气;并且涉及高温(300-600°C)和高压(200-400 atm)的恶劣工作条件,每年消耗大量能源。最近,人们对受自然微生物固氮作用启发的电化学氮还原过程(NRR)生成NH 3产生了很大的兴趣。然而,稳定的N
![[triple bond, length as m-dash]](https://www.rsc.org/images/entities/char_e002.gif)
![[double bond, length as m-dash]](https://www.rsc.org/images/entities/char_e001.gif)