Ultralow overpotential nitrate reduction to ammonia via a three-step relay mechanism

被引：540

作者：

Han, Shuhe ^{[1
]}

Li, Hongjiao ^{[2
]}

Li, Tieliang ^{[1
]}

Chen, Fanpeng ^{[1
]}

Yang, Rong ^{[1
]}

Yu, Yifu ^{[1
]}

Zhang, Bin ^{[1
,3
]}

机构：

[1] Tianjin Univ, Inst Mol Plus, Sch Sci, Dept Chem, Tianjin, Peoples R China

[2] Sichuan Univ, Sch Chem Engn, Chengdu, Sichuan, Peoples R China

[3] Tianjin Univ, Frontiers Sci Ctr Synthet Biol, Tianjin Key Lab Mol Optoelect Sci, Minist Educ, Tianjin, Peoples R China

来源：

NATURE CATALYSIS | 2023年 / 6卷 / 05期

基金：

中国国家自然科学基金;

关键词：

ELECTROCHEMICAL REDUCTION; ELECTROCATALYSTS; EVOLUTION; CATALYSTS; ELECTRODES; DINITROGEN; WATER;

D O I：

10.1038/s41929-023-00951-2

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Ammonia plays a substantial role in agriculture and the next generation of carbon-free energy supply. Electrocatalytic nitrate reduction to NH3 is attractive for nitrate removal and NH3 production under ambient conditions. However, the energy efficiency is limited by the high reaction overpotential. Here we propose a three-step relay mechanism composed of a spontaneous redox reaction, electrochemical reduction and electrocatalytic reduction to overcome this issue. RuxCoy alloys were designed and adopted as model catalysts. Ru15Co85 exhibits an onset potential of +0.4 V versus reversible hydrogen electrode, and an energy efficiency of 42 +/- 2%. The high performance results in a low production cost of US$0.49 +/- 0.02 per kilogram of ammonia. The high nitrate reduction performances on Ru15Fe85 and Ru15Ni85 also highlight the promising potential of the relay mechanism.

引用

页码：402 / 414

页数：13

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