In situ reconstruction enhanced dual-site catalysis towards nitrate electroreduction to ammonia

被引：35
作者：
Cai, Jiahao [1 ]
Qin, Shuaibo [2 ]
Akram, Muhammad Awais [1 ]
Hou, Xiangdie [3 ]
Jin, Peng [2 ]
Wang, Feng [1 ]
Zhu, Botao [1 ]
Li, Xiaohong [3 ]
Feng, Lai [1 ]
机构：
[1] Soochow Univ, Coll Energy, Soochow Inst Energy & Mat Innovat, Jiangsu Key Lab Adv Carbon Mat & Wearable Energy, Suzhou 215006, Peoples R China
[2] Hebei Univ Technol, Sch Mat Sci & Engn, Tianjin 300130, Peoples R China
[3] Soochow Univ, Coll Chem Chem Engn & Mat Sci, Key Lab Hlth Chem & Mol Diag Suzhou, Suzhou 215006, Peoples R China
来源：
JOURNAL OF MATERIALS CHEMISTRY A | 2022年 / 10卷 / 23期
基金：
中国国家自然科学基金;
关键词：
BIFUNCTIONAL ELECTROCATALYSTS; COPPER; SPECTROSCOPY; CHALLENGES; REDUCTION; SURFACES; OXIDES;
D O I：
10.1039/d2ta01772e
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：
Electro-reduction of nitrate to ammonia (e-NRA) has been considered as a facile and promising approach to eliminate nitrate pollution and produce ammonia (NH<INF>3</INF>) under ambient conditions. Nevertheless, in recent state-of-the-art studies, high faradaic efficiency towards NH<INF>3</INF> (FE<INF>NH<INF>3</INF></INF>) was usually achieved with a very negative working potential (vs. RHE) or high overpotential, which causes not only low cost-efficiency but also structural degradation in electrocatalysts. In this work, we utilize the strategy of in situ electrochemical reconstruction to develop a highly efficient and durable electrocatalyst Ru&Cu/Cu<INF>2</INF>O (denoted as i-Cu<INF>5</INF>Ru<INF>1</INF>O<INF>x</INF>) towards alkaline e-NRA. As a result, highly selective production of NH<INF>3</INF> can be achieved with an optimal FE<INF>NH<INF>3</INF></INF> of around 95% even at a positive working potential of 0.1 V (vs. RHE) or a small overpotential of 0.59 V. The catalyst shows no obvious degradation after consecutive e-NRA for 10 h. In addition, density functional theory (DFT) computations reveal that the excellent catalytic performance of Ru&Cu/Cu<INF>2</INF>O could be attributed to the synergy of the Cu/Ru dual-site, which results in significantly enhanced adsorption of NO<INF>3</INF>- ion and a more favorable proton supply for the hydrogenation during e-NRA. This work thus highlights the importance of dual-site synergy towards the electrochemical process with multiple elementary steps.
引用
收藏
页码：12669 / 12678
页数：10
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