Selective electrosynthesis of ammonia via nitric oxide electroreduction catalyzed by copper nanowires infused in nitrogen-doped carbon nanorods

Dinesh Dhanabal, Yuyeon Song, Seoyoung Jang, Sangaraju Shanmugam
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Abstract

The electrochemical nitric oxide reduction reaction (eNORR) is meticulously investigated as an alternative to the energy intensive Haber-Bosch process to produce Ammonia (NH). However, the eNORR is hindered by NH selectivity due to side reactions and mass-transfer limitations. In this work, we rationally designed copper nanowires (Cu NWs) infused in the lotus-root-like multi-nano-channels of the porous N-doped carbon nanorods (Cu-mNCNR) for a high selective eNORR to synthesize NH at ambient conditions. The optimized catalyst, Cu-mNCNR2, has achieved the highest NH Faradaic efficiency of 79% with NH yield rate of 34.5 μmol cm h at −0.4 V. Moreover, the Cu-mNCNR2 has demonstrated a vigorous performance in the 24 h continuous NO electrolysis to produce NH. Additionally, a prototype device, the Zn-NO battery, was demonstrated. This study shows that the rational design of a catalyst considering mass-transfer limitations is crucial to achieving high selective NH electrosynthesis in eNORR.
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在掺氮碳纳米棒中注入铜纳米线催化下,通过一氧化氮电还原选择性电合成氨
电化学一氧化氮还原反应(eNORR)作为生产氨气(NH)的高能耗哈伯-博什工艺的替代方法,受到了细致的研究。然而,由于副反应和传质的限制,eNORR 受阻于 NH 的选择性。在这项工作中,我们合理地设计了铜纳米线(Cu NWs),将其注入多孔掺杂 N 的碳纳米棒(Cu-mNCNR)的莲藕状多纳米通道中,从而在环境条件下合成高选择性 eNORR。优化后的催化剂 Cu-mNCNR2 在 -0.4 V 条件下的 NH 法拉第效率最高,达到 79%,NH 产率为 34.5 μmol cm h。此外,Cu-mNCNR2 在连续 24 小时电解 NO 生成 NH 的过程中表现出了强劲的性能。此外,还展示了 Zn-NO 电池的原型装置。这项研究表明,要在 eNORR 中实现高选择性 NH 电合成,合理设计催化剂并考虑质量转移限制至关重要。
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