Zeolite-mediated hybrid Cu+/Cu0 interface for electrochemical nitrate reduction to ammonia

被引:15
|
作者
Lv, Jiabao [1 ,2 ]
Wu, Angjian [1 ,2 ,3 ]
Wang, Liang [4 ]
Zhong, Yunhao [1 ]
Zeng, Zhihao [1 ]
Huang, Qunxing [1 ,3 ]
Lin, Xiaoqing [1 ]
Zhang, Hao [1 ]
Liu, Shaojun [1 ]
Liu, Qian [5 ]
Zhu, Songqiang [2 ]
Li, Xiaodong [1 ]
Yan, Jianhua [1 ]
Qi, Zhifu [2 ]
Bin Wu, Hao [5 ]
机构
[1] Zhejiang Univ, State Key Lab Clean Energy Utilizat, Hangzhou 310027, Zhejiang, Peoples R China
[2] Baima Lake Lab, Hangzhou 310053, Zhejiang, Peoples R China
[3] Zhejiang Univ, Jiaxing Res Inst, Lab Clean Energy & Carbon Neutral Zhejiang Prov, Jiaxing 314031, Peoples R China
[4] Zhejiang Univ, Coll Chem & Biol Engn, Key Lab Biomass Chem Engn, Minist Educ, Hangzhou 310027, Zhejiang, Peoples R China
[5] Zhejiang Univ, Inst Composites Sci Innovat InCSI, Sch Mat Sci & Engn, State Key Lab Silicon Mat, Hangzhou 310027, Peoples R China
来源
关键词
Electrochemical nitrate reduction reaction; Ammonia synthesis; In-situ Raman spectroscopy; Zeolite; Density functional theory; NITROGEN REDUCTION; RAMAN-SCATTERING; PERFORMANCE; WATER; CATALYSTS; EFFICIENT;
D O I
10.1016/j.jechem.2023.08.013
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The electrocatalytic conversion of reactive nitrogen species to ammonia is a promising strategy for efficient NH3 synthesis. In this study, we reveal that the hybrid Cu+/Cu0 interface is catalytically active for electrochemical ammonia synthesis from nitrate reduction. To maintain the hybrid Cu+/Cu0 state at negative reaction potentials, hydrophilic zeolite is used to modify Cu/Cu2O electrocatalyst, which demonstrates an impressive NH3 production rate of 41.65 mg h-1 cm-2 with-100% Faradaic efficiency of ammonia synthesis at-0.6 V vs. RHE. In-situ Raman spectroscopy unveil the high activity originates from the zeolite reconstruction at the electrode-electrolyte interface, which protects the valence state of Cu0/ Cu+ site under negative potential and promotes electrochemical activity towards NH3 synthesis.(c) 2023 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
引用
收藏
页码:136 / 143
页数:8
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