Electron-deficient cobalt nanocrystals for promoted nitrate electrocatalytic reduction to synthesize ammonia

被引:43
|
作者
Yang, Baopeng [1 ,2 ]
Zhou, Yulong [1 ]
Huang, Zhencong [1 ]
Mei, Binbao [3 ]
Kang, Qing [4 ]
Chen, Gen [1 ]
Liu, Xiaohe [5 ]
Jiang, Zheng [3 ]
Liu, Min [2 ]
Zhang, Ning [1 ]
机构
[1] Cent South Univ, Sch Mat Sci & Engn, Changsha 410083, Peoples R China
[2] Cent South Univ, Sch Phys & Elect, Changsha 410083, Peoples R China
[3] Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Shanghai 201800, Peoples R China
[4] Univ Jinan, Inst Surface Anal & Chem Biol, Jinan 250022, Peoples R China
[5] Zhengzhou Univ, Sch Chem Engn, Zhengzhou 450001, Peoples R China
基金
中国国家自然科学基金;
关键词
Nitrate reduction reactions; Ammonia synthesis; Pyridine nitrogen doped carbon; Cobalt metal; Electron-deficient state;
D O I
10.1016/j.nanoen.2023.108901
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 Co-based electrocatalysts are promising for NO3- reduction reactions to synthesize NH3. However, NH3 yielding efficiencies over oxidation state Co compounds and electron-rich Co metal are still low due to the difficulties in simultaneously satisfying both NO3- adsorption and NHx hydrogenation. Herein, an electrondeficient Co nanocrystals is designed by interacting Co with pyridine nitrogen to promote the electrocatalytic NO3- reductions to synthesize NH3. Theoretical calculations predict that pyridine nitrogen modifications induce the electron-deficiency in Co nanoparticles, facilitating both the NO3- adsorption and energy-barrier decrease of *NH to *NH2. A pyridine nitrogen-doped carbon modified Co nanocrystals (Co/PN-C) are thus fabricated. The Xray photoelectron and absorption near-edge spectroscopies confirm the electron-deficient state of Co metal in as prepared Co/PN-C materials. The Co/PN-C exhibits a high Faraday efficiency of 97.8 +/- 2.0% toward NH3 generation, a remarkable NO3- removal efficiency of approximate 100%, and an outstanding NH3 yield rate of 109 mg h-1 cm-2 with a current density of 1.3 A cm-2. These performances are significantly higher than mostly reported Co-based electrocatalysts. In-situ Raman and Fourier-transform infrared spectra further confirm that Co/PN-C promotes NO3- adsorption and *NH hydrogenation to form NH3. This work gives effective strategy to tune electron-deficient Co nanocrystals for promoted NO3- electrocatalytic reduction to synthesize NH3.
引用
收藏
页数:9
相关论文
共 50 条
  • [31] Bronsted acid-promoted aziridination of electron-deficient olefins
    Li, Juan
    Fu, Yao
    Guo, Qing-Xiang
    TETRAHEDRON, 2008, 64 (49) : 11167 - 11174
  • [32] Electrocatalytic reduction of nitrate by in situ generated cobalt nanoparticles
    Ghosh, Moumita
    Ibrar, Maha
    Smith, Jeremy M.
    CHEMICAL COMMUNICATIONS, 2022, 58 (30) : 4783 - 4786
  • [33] Synergistic integration of copper and cobalt-MOF for high-efficiency electrocatalytic nitrate reduction to ammonia
    Xin, Chengjie
    Wei, Yu-Ping
    Bai, Jia-qi
    Chen, Jingshuai
    Sun, Song
    Mao, Chang-Jie
    JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING, 2025, 13 (01):
  • [34] Synergistic Integration of Amorphous Cobalt Phosphide with a Conductive Channel for Highly Efficient Electrocatalytic Nitrate Reduction to Ammonia
    Qi, Ruikai
    Wang, Zhiwei
    Zhong, Mengxiao
    Wang, Ce
    Bai, Fuquan
    Lu, Xiaofeng
    SMALL, 2024, 20 (20)
  • [35] Theory-guided construction of electron-deficient sites via removal of lattice oxygen for the boosted electrocatalytic synthesis of ammonia
    Zhang, Li
    Jiao, Shilong
    Tan, Xin
    Yuan, Yuliang
    Xiang, Yu
    Zeng, Yu-Jia
    Qiu, Jingyi
    Peng, Ping
    Smith, Sean C.
    Huang, Hongwen
    NANO RESEARCH, 2021, 14 (05) : 1457 - 1464
  • [36] Theory-guided construction of electron-deficient sites via removal of lattice oxygen for the boosted electrocatalytic synthesis of ammonia
    Li Zhang
    Shilong Jiao
    Xin Tan
    Yuliang Yuan
    Yu Xiang
    Yu-Jia Zeng
    Jingyi Qiu
    Ping Peng
    Sean C. Smith
    Hongwen Huang
    Nano Research, 2021, 14 : 1457 - 1464
  • [37] Difluorocarbene transfer from a cobalt complex to an electron-deficient alkene
    Goswami, Monalisa
    de Bruin, Bas
    Dzik, Wojciech I.
    CHEMICAL COMMUNICATIONS, 2017, 53 (31) : 4382 - 4385
  • [38] Cobalt-catalyzed asymmetric cyclopropanation of electron-deficient olefins
    Chen, Ying
    Ruppel, Joshua V.
    Zhang, X. Peter
    JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2007, 129 (40) : 12074 - +
  • [39] Cobalt-catalyzed asymmetric cyclopropanation of electron-deficient olefins
    Chen, Ying
    Ruppel, Joshua V.
    Zhang, X. Peter
    Journal of the American Chemical Society, 2007, 129 (40): : 12074 - 12075
  • [40] On the Lewis base-promoted alkynylation of electron-deficient fluorobenzenes with trimethylsilylacetylenes
    Sanji, Takanobu
    Watanabe, Satoru
    Iyoda, Tomokazu
    TETRAHEDRON LETTERS, 2016, 57 (17) : 1921 - 1924