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A Co3O4/graphdiyne heterointerface for efficient ammonia production from nitrates

CHEN Zhao-yang ZHAO Shu-ya LUAN Xiao-yu ZHENG Zhi-qiang YAN Jia-yu XUE Yu-rui

陈朝阳, 赵淑雅, 栾晓雨, 郑志强, 闫佳玉, 薛玉瑞. Co3O4/石墨炔异质界面用于高效硝酸根制氨. 新型炭材料(中英文), 2024, 39(1): 142-151. doi: 10.1016/S1872-5805(24)60834-6
引用本文: 陈朝阳, 赵淑雅, 栾晓雨, 郑志强, 闫佳玉, 薛玉瑞. Co3O4/石墨炔异质界面用于高效硝酸根制氨. 新型炭材料(中英文), 2024, 39(1): 142-151. doi: 10.1016/S1872-5805(24)60834-6
CHEN Zhao-yang, ZHAO Shu-ya, LUAN Xiao-yu, ZHENG Zhi-qiang, YAN Jia-yu, XUE Yu-rui. A Co3O4/graphdiyne heterointerface for efficient ammonia production from nitrates. New Carbon Mater., 2024, 39(1): 142-151. doi: 10.1016/S1872-5805(24)60834-6
Citation: CHEN Zhao-yang, ZHAO Shu-ya, LUAN Xiao-yu, ZHENG Zhi-qiang, YAN Jia-yu, XUE Yu-rui. A Co3O4/graphdiyne heterointerface for efficient ammonia production from nitrates. New Carbon Mater., 2024, 39(1): 142-151. doi: 10.1016/S1872-5805(24)60834-6

Co3O4/石墨炔异质界面用于高效硝酸根制氨

doi: 10.1016/S1872-5805(24)60834-6
基金项目: 国家重点研发计划项目(2022YFA1204500, 2022YFA1204501, 2022YFA1204503, 2018YFA0703501);山东省泰山学者青年专家项目(tsqn201909050);山东省自然科学基金(ZR2020ZD38, ZR2021JQ07)
详细信息
    通讯作者:

    薛玉瑞, 教授. E-mail:yrxue@sdu.edu.cn

  • 中图分类号: TQ519

A Co3O4/graphdiyne heterointerface for efficient ammonia production from nitrates

Funds: This work was supported by the National Key Research and Development Project of China (2022YFA1204500, 2022YFA1204501, 2022YFA1204503, 2018YFA0703501), the Taishan Scholars Youth Expert Program of Shandong Province (tsqn201909050), and the Natural Science Foundation of Shandong Province (ZR2020ZD38, ZR2021JQ07)
More Information
  • 摘要: 硝酸根还原反应(NtRR)是一种合成氨(NH3)的有效方法。催化剂的合成包括2步简单的工艺:首先在炭布(CC)上合成Co3O4纳米线,然后以六乙炔基苯(HEB)为前驱体在Co3O4表面生长石墨炔(GDY)(110 °C, 10 h),从而可控合成Co3O4/GDY纳米线异质结催化剂。高分辨率扫描电镜(SEM)、透射电镜(HRTEM)、X射线光电子能谱(XPS)和拉曼表征等证实了Co3O4/GDY异质界面的成功合成,界面处形成的独特的sp-C―Co键以及GDY与Co之间的不完全电荷转移为催化反应提供了持续的电子供应,保证了NtRR的高效进行。Co3O4/GDY在NtRR中展现了优异催化性能,其NH3产率(YNH3)和法拉第效率(FE)分别达到了0.78 mmol h−1 cm−2 和92.45%。这项工作为在温和条件下,从废水中高性能生产氨的异质结构提供了一种通用方法。
  • FIG. 2916.  FIG. 2916.

    FIG. 2916..  FIG. 2916.

    Figure  1.  The synthetic routes of the Co3O4/GDY

    Figure  2.  Morphological characterizations of samples. (a) Low- and (b, c) high-magnification SEM images of the Co3O4. (d) Low- and (e, f) high-magnification SEM images of the as-prepared Co3O4/GDY. (g) EDS mapping of C, O and Co in Co3O4/GDY nanowires. (h) Contact angle measurements of Co3O4/GDY. (i) Optical photos of Co3O4/GDY

    Figure  3.  (a-c) HRTEM images of the Co3O4. (d-f) HRTEM images of the Co3O4/GDY. (e) The high distribution of Co3O4 in Co3O4/GDY. (f) Boundary between Co3O4 and GDY. (g) Low- and (h, i) high-magnification HRTEM images of GDY on the surface of Co3O4/GDY

    Figure  4.  (a) Raman spectra of Co3O4 and Co3O4/GDY. (b) C 1s XPS spectra of Co3O4 and Co3O4/GDY. (c) Co 2p XPS spectra of Co3O4 and Co3O4/GDY. (d) O 1s XPS spectra of Co3O4 and Co3O4/GDY. O represents the Co-O bond; O is assigned as the ―OH on the surface; O is considered to originate from environmental contamination. (e) Schematic illustration of the electron transfer at the GDY-Co3O4 interfaces of Co3O4/GDY. (f) The current density differences (Δj= jajc) are plotted against scan rates. (g) Nyquist plots of Co3O4 and Co3O4/GDY. (h) Co 2p XPS spectra of Co3O4/GDY after NtRR. (i) Schematic diagram of charge changes in Co3O4/GDY during the NtRR process

    Figure  5.  NtRR performance tests. (a) Schematic representation of the NO3-to-NH3 conversion. (b) Linear sweep voltammetry curves of the samples in 0.5 mol L−1 K2SO4 +0.1 mol L−1 NO3−+ and pure 0.5 mol L−1 K2SO4 aqueous solutions. (c) Current density-time curves of Co3O4/GDY at different potentials in 0.5 mol L−1 K2SO4 + 0.1 mol L−1 NO3. The YNH3 and FE of (d) Co3O4 and (e) Co3O4/GDY in 0.5 mol L−1 K2SO4 + 0.1 mol L−1 NO3. (f) Stability tests of Co3O4/GDY at −1.05 V (vs. RHE). (g) YNH3 and FE of Co3O4/GDY at −1.05 V (vs. RHE) with and without NO3. (h) Proportion of products. (i) NtRR performance comparison to other catalysts. (j-l) Insitu ATR-FTIR spectra of Co3O4/GDY during NtRR

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  • 收稿日期:  2023-09-21
  • 录用日期:  2023-12-19
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