Highly efficient N2 electroreduction to NH3 on Cu7.2S4/C with sulfur vacancies synthesized using a continuous microchannel reactor

被引:3
作者
Yang, Chenxia [1 ]
Tang, Ying [1 ]
Liu, Xianghao [1 ]
Zhang, Mei [1 ]
Pu, Jingwen [1 ]
Yang, Qian [1 ]
Zhao, Yunxia [1 ]
Gao, Huiping [1 ]
Wang, Gang [1 ]
Yu, Feng [1 ,2 ]
机构
[1] Shihezi Univ, Sch Chem & Chem Engn, Key Lab Green Proc Chem Engn Xinjiang Bingtuan, Shihezi 832003, Peoples R China
[2] Shihezi Univ, Bingtuan Ind Technol Res Inst, Carbon Neutralizat & Environm Catalyt Technol Lab, Shihezi 832003, Peoples R China
基金
中国国家自然科学基金;
关键词
Metal-organic framework; Sulfur vacancy; Nitrogen reduction reaction; Microchannel reactor; ELECTROCHEMICAL NITROGEN REDUCTION; ONE-STEP SYNTHESIS; AMMONIA-SYNTHESIS; CATALYSTS; N-2; ELECTROCATALYSTS; TEMPERATURE; DEFECT; WATER;
D O I
10.1016/j.ijhydene.2024.04.092
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
The electrochemical nitrogen reduction reaction (NRR) has emerged as a sustainable and environmental-friendly alternative for ammonia synthesis compared with conventional Haber-Bosch process. However, considerable challenges persist in developing cost-effective catalysts for NRR. Herein, Cu7.2S4/C was synthesized using a continuous microchannel reactor followed by carbonization sulfurization at 600 degrees C. The as-prepared Cu7.2S4/C catalyst, featuring abundant sulfur vacancies, exhibited outstanding electrochemical performance for NRR, achieving an ammonia yield of 52 mu g h-1 mg- 1 theory calculations suggest that sulfur vacancies contribute to a decrease in Gibbs free energy during N2-activated hydrogenation, thereby facilitating adsorption of N2 and formation of Cu-N bonds at catalytic active centers. This study introduces a novel strategy for synthesizing economical and efficient NRR electrocatalysts based on transition metal-based metal-organic frameworks.
引用
收藏
页码:251 / 258
页数:8
相关论文
共 70 条
  • [1] Metal-Sulfur Linkages Achieved by Organic Tethering of Ruthenium Nanocrystals for Enhanced Electrochemical Nitrogen Reduction
    Ahmed, Muhammad Ibrar
    Liu, Chuangwei
    Zhao, Yong
    Ren, Wenhao
    Chen, Xianjue
    Chen, Sheng
    Zhao, Chuan
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2020, 59 (48) : 21465 - 21469
  • [2] Nickel Nanoflowers with Controllable Cation Vacancy for Enhanced Electrochemical Nitrogen Reduction
    Bai, Fan
    Qu, Xin
    Li, Cong
    Liu, Shuo
    Sun, Jie
    Chen, Xu
    Yang, Wensheng
    [J]. ACS APPLIED MATERIALS & INTERFACES, 2022, 14 (24) : 28033 - 28043
  • [3] Electrocatalysis of N2 to NH3 by HKUST-1 with High NH3 Yield
    Cao, Yueming
    Li, Peipei
    Wu, Tengteng
    Liu, Meiling
    Zhang, Youyu
    [J]. CHEMISTRY-AN ASIAN JOURNAL, 2020, 15 (08) : 1272 - 1276
  • [4] Ambient dinitrogen electrocatalytic reduction for ammonia synthesis
    Chen, Aling
    Xia, Bao Yu
    [J]. JOURNAL OF MATERIALS CHEMISTRY A, 2019, 7 (41) : 23416 - 23431
  • [5] Lattice-Confined Single-Atom Fe1Sx on Mesoporous TiO2 for Boosting Ambient Electrocatalytic N2 Reduction Reaction
    Chen, Jiayin
    Kang, Yikun
    Zhang, Wei
    Zhang, Zhenghao
    Chen, Yan
    Yang, Yi
    Duan, Linlin
    Li, Yefei
    Li, Wei
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2022, 61 (27)
  • [6] Pd1Cu Single-Atom Alloys for High-Current-Density and Durable NO-to-NH3 Electroreduction
    Chen, Kai
    Xiang, Jiaqi
    Guo, Yali
    Liu, Xijun
    Li, Xingang
    Chu, Ke
    [J]. NANO LETTERS, 2024, 24 (02) : 541 - 548
  • [7] Iridium single-atom catalyst for highly efficient NO electroreduction to NH3
    Chen, Kai
    Wang, Guohui
    Guo, Yali
    Ma, Dongwei
    Chu, Ke
    [J]. NANO RESEARCH, 2023, 16 (07) : 8737 - 8742
  • [8] Amorphous MoS3 enriched with sulfur vacancies for efficient electrocatalytic nitrogen reduction
    Chu, Ke
    Nan, Haifeng
    Li, Qingqing
    Guo, Yali
    Tian, Ye
    Liu, Wuming
    [J]. JOURNAL OF ENERGY CHEMISTRY, 2021, 53 : 132 - 138
  • [9] NO hydrogenation to NH3 over FeCu/TiO2 catalyst with improved activity
    Cui, Dan
    Li, Yanqin
    Pan, Keke
    Liu, Jinbao
    Wang, Qiang
    Liu, Minmin
    Cao, Peng
    Dan, Jianming
    Dai, Bin
    Yu, Feng
    [J]. FRONTIERS OF CHEMICAL SCIENCE AND ENGINEERING, 2023, 17 (12) : 1973 - 1985
  • [10] Bimetallic Cooperative Cleavage of Dinitrogen to Nitride and Tandem Frustrated Lewis Pair Hydrogenation to Ammonia
    Doyle, Laurence R.
    Wooles, Ashley J.
    Liddle, Stephen T.
    [J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2019, 58 (20) : 6674 - 6677