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A Bifunctional Catalyst for Green Ammonia Synthesis from Ubiquitous Air and Water
Advanced Materials ( IF 27.4 ) Pub Date : 2023-06-26 , DOI: 10.1002/adma.202303455
Rui Gao 1 , Tian-Yi Dai 1 , Zhe Meng 1 , Xue-Feng Sun 1 , Dong-Xue Liu 1 , Miao-Miao Shi 1 , Hong-Rui Li 1 , Xia Kang 1 , Bo Bi 1 , Yu-Tian Zhang 1 , Tong-Wen Xu 2 , Jun-Min Yan 1 , Qing Jiang 1
Affiliation  

Ammonia (NH3) is essential for modern agriculture and industry, and, due to its high hydrogen density and no carbon emission, it is also expected to be the next-generation of “clean” energy carrier. Herein, directly from air and water, a plasma-electrocatalytic reaction system for NH3 production, which combines two steps of plasma-air-to-NOx and electrochemical NOx reduction reaction (eNOxRR) with a bifunctional catalyst, is successfully established. Especially, the bifunctional catalyst of CuCo2O4/Ni can simultaneously promote plasma-air-to-NOx and eNOxRR processes. The easy adsorption and activation of O2 by CuCo2O4/Ni greatly improve the NOx production rate at the first step. Further, CuCo2O4/Ni can also resolve the overbonding of the key intermediate of *NO, and thus reduce the energy barrier of the second step of eNOxRR. Finally, the “green” NH3 production achieves excellent FENH3 (96.8%) and record-high NH3 yield rate of 145.8 mg h−1 cm−2 with large partial current density (1384.7 mA cm−2). Moreover, an enlarged self-made H-type electrolyzer improves the NH3 yield to 3.6 g h−1, and the obtained NH3 is then rapidly converted to a solid of magnesium ammonium phosphate hexahydrate, which favors the easy storage and transportation of NH3.

中文翻译:

从普遍存在的空气和水中合成绿色氨的双功能催化剂

氨(NH 3)对于现代农业和工业至关重要,而且由于其氢密度高且无碳排放,也有望成为下一代“清洁”能源载体。本文中,直接从空气和水中生产NH 3的等离子体电催化反应系统,其结合了等离子体-空气-NO x -和电化学NO x -还原反应(eNO x RR)与双功能催化剂的两个步骤,已成功建立。特别是,CuCo 2 O 4 /Ni双功能催化剂可以同时促进等离子体-空气-NO x -和eNO x RR过程。CuCo 2 O 4 /Ni对O 2的易吸附和活化大大提高了第一步NO x - 的产率。此外,CuCo 2 O 4 /Ni还可以解决* NO关键中间体的过键合问题,从而降低eNO x RR第二步的能垒。最后,“绿色”NH 3生产实现了优异的FE NH3 (96.8%)和创纪录的高NH 3产率145.8 mg h -1  cm -2以及大的部分电流密度(1384.7 mA cm -2 )。此外,自制的H型电解槽加大,NH 3收率提高至3.6 g h -1,所得NH 3迅速转化为六水磷酸镁铵固体,有利于NH 3的储存和运输。
更新日期:2023-06-26
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