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
相关论文
共 50 条
  • [11] Tracking the critical roles of Cu+ and Cu0 sites and the optimal Cu+/Cu0 ratio for CH3OH steam reforming (MTSR) to manufacture H2
    Ma, Jiamei
    Mao, Lei
    Du, Haoxuan
    Zhong, Jingkang
    Jiang, Lifang
    Liu, Xiaofei
    Xu, Junwei
    Xu, Xianglan
    Fang, Xiuzhong
    Wang, Xiang
    CHEMICAL ENGINEERING JOURNAL, 2024, 496
  • [12] The effect of the amount of ammonia on the Cu0/Cu+ ratio of Cu/SiO2 catalyst for the hydrogenation of dimethyl oxalate to ethylene glycol
    Li, Feng
    Lu, Chun-Shan
    Li, Xiao-Nian
    CHINESE CHEMICAL LETTERS, 2014, 25 (11) : 1461 - 1465
  • [13] Cu/Cu+ Synergetic Effect in Cu2O/Cu/CF Electrocatalysts for Efficient Nitrate Reduction to Ammonia
    Shen, Zhaoran
    Yan, Jiabiao
    Wang, Min
    Xing, Lidan
    Huang, Bingji
    Zhou, Hangyan
    Li, Wenbo
    Chen, Lisong
    Shi, Jianlin
    ACS SUSTAINABLE CHEMISTRY & ENGINEERING, 2023, 11 (25) : 9433 - 9441
  • [14] Coupling of LaFeO3-Plasma Catalysis and Cu+/Cu0 Electrocatalysis for Direct Ammonia Synthesis from Air
    Cui, Yi
    Yang, Hui
    Dai, Chengyi
    Ren, Pengju
    Song, Chunshan
    Ma, Xiaoxun
    INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2022, 61 (14) : 4816 - 4823
  • [15] Synergetic effect between Cu0 and Cu+ in the Cu-Cr catalysts for hydrogenolysis of glycerol
    Xiao, Zihui
    Wang, Xinkui
    Xiu, Jinghai
    Wang, Yuemin
    Williams, Christopher T.
    Liang, Changhai
    CATALYSIS TODAY, 2014, 234 : 200 - 207
  • [16] Catalytic hydrogenation of CO2 to DME on surface Cu via highly efficient electron redistribution at the Cu0/Cu+ interface
    Chen, Xiaorui
    Su, Tongming
    Luo, Xuan
    Xie, Xinling
    Qin, Zuzeng
    Ji, Hongbing
    SURFACES AND INTERFACES, 2024, 48
  • [17] Interface tuning of Cu+/Cu0 by zirconia for dimethyl oxalate hydrogenation to ethylene glycol over Cu/SiO2 catalyst
    Yujun Zhao
    Huanhuan Zhang
    Yuxi Xu
    Shengnian Wang
    Yan Xu
    Shengping Wang
    Xinbin Ma
    Journal of Energy Chemistry , 2020, (10) : 248 - 256
  • [18] In Situ Engineering of the Cu+/Cu0 Interface to Boost C2+ Selectivity in CO2 Electroreduction
    Du, Ruian
    Li, Tan
    Wu, Qiqi
    Wang, Peng
    Yang, Xianfeng
    Fan, Yan
    Qiu, Yongcai
    Yan, Keyou
    Wang, Pei
    Zhao, Yun
    Zhao, Wei-Wei
    Chen, Guangxu
    ACS APPLIED MATERIALS & INTERFACES, 2022, 14 (32) : 36527 - 36535
  • [19] Concentration Optimization of Localized Cu0 and Cu+ on Cu-Based Electrodes for Improving Electrochemical Generation of Ethanol from Carbon Dioxide
    Lu, Hong
    Wang, Guan
    Zhou, Yong
    Wotango, Aselefech Sorsa
    Wu, Jiahao
    Meng, Qi
    Li, Ping
    INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES, 2022, 23 (16)
  • [20] Unraveling the roles of Cu0 and Cu+ in CuZnAl catalyst for CO hydrogenation to higher alcohols
    Wang, Kejing
    Liu, Yongjun
    Li, Zhiwen
    Cui, Nan
    Sun, Lei
    Huang, Wei
    INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2024, 80 : 999 - 1010