Highly Selective Electrochemical Nitrate to Ammonia Conversion by Dispersed Ru in a Multielement Alloy Catalyst

被引:34
|
作者
Yang, Meiqi [1 ,2 ]
Li, Boyang [3 ]
Li, Shuke [4 ]
Dong, Qi [4 ]
Huang, Zhennan [4 ]
Zheng, Sunxiang [1 ,2 ]
Fang, Ying [3 ]
Zhou, Guangye [1 ,2 ]
Chen, Xi [1 ,2 ]
Zhu, Xiaobo [1 ,2 ]
Li, Tangyuan [4 ]
Chi, Miaofang [5 ]
Wang, Guofeng [3 ]
Hu, Liangbing [4 ]
Ren, Zhiyong Jason [1 ,2 ]
机构
[1] Princeton Univ, Dept Civil & Environm Engn, Princeton, NJ 08544 USA
[2] Princeton Univ, Andlinger Ctr Energy & Environm, Princeton, NJ 08544 USA
[3] Univ Pittsburgh, Dept Mech Engn & Mat Sci, Pittsburgh, PA 15260 USA
[4] Univ Maryland, Dept Mat Sci & Engn, College Pk, MD 20742 USA
[5] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37932 USA
基金
美国国家科学基金会;
关键词
electrochemical nitrate reduction; ammonia; multielement alloy catalyst; industrial wastewater; acidic; OXYGEN REDUCTION; WASTE-WATER; DENITRIFICATION; NITROGEN; TRENDS; ELECTROREDUCTION; ELECTRODES; MECHANISM; PLATINUM; METHANOL;
D O I
10.1021/acs.nanolett.3c01978
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Electrochemical reduction of nitrate to ammonia (NH3) converts an environmental pollutant to a critical nutrient.However,current electrochemical nitrate reduction operations based on monometallicand bimetallic catalysts are limited in NH3 selectivityand catalyst stability, especially in acidic environments. Meanwhile,catalysts with dispersed active sites generally exhibit a higher atomicutilization and distinct activity. Herein, we report a multielementalloy nanoparticle catalyst with dispersed Ru (Ru-MEA) with othersynergistic components (Cu, Pd, Pt). Density functional theory elucidatedthe synergy effect of Ru-MEA than Ru, where a better reactivity (NH3 partial current density of -50.8 mA cm(-2)) and high NH3 faradaic efficiency (93.5%) is achievedin industrially relevant acidic wastewater. In addition, the Ru-MEAcatalyst showed good stability (e.g., 19.0% decay in FENH3 in three hours). This work provides a potential systematic and efficientcatalyst discovery process that integrates a data-guided catalystdesign and novel catalyst synthesis for a range of applications.
引用
收藏
页码:7733 / 7742
页数:10
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