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Abstract <p>This study addresses the key issues of low activity and slow reaction rates in supported nickel-based catalysts for the hydrogenation of <i>m</i>-dinitrobenzene (DNB). Density Functional Theory (DFT) calculations revealed that the Ni(111) crystal plane exhibits the highest adsorption energy for the reactant, indicating its potential advantage in DNB hydrogenation. Based on this, using KBr as a structure-directing agent, a supported catalyst with a high proportion of exposed Ni(111) planes was prepared by regulating the crystal plane orientation of nickel nanoparticles. Characterization techniques including XRD, TEM, N<sub>2</sub> physical adsorption-desorption, NH<sub>3</sub>-TPD, and XPS were used to systematically elucidate the mechanism of KBr’s regulation on crystal planes: KBr optimizes the exposure ratio of crystal planes by influencing the agglomeration-dispersion balance of particles. When the molar ratio of KBr to Ni is 50, the exposure proportion of the Ni(111) plane reached 80.81%. The prepared Ni-KBr-50/ZSM-5-Al catalyst exhibited optimal catalytic performance: DNB conversion reached 99.99% within 5&#xa0;min, and <i>m</i>-phenylenediamine (MPD) selectivity reached 99.99%, consistent with the DFT-predicted trend of “high adsorption energy crystal plane promotes reaction activity.” Additionally, catalyst stability tests showed excellent stability: Ni-KBr-50/ZSM-5-Al maintained a DNB conversion of 99.99% over 10 recycling experiments, with MPD selectivity still reaching 98.71% in the 10th cycle.</p> Graphic Abstract <p></p>

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Study on Ni Catalyst Crystal Plane Orientation and Its Effect on Hydrogenation Performance of m-Dinitrobenzene

  • 期刊论文

  • 发表日期：

    2025年11月4日

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  • Hongwei Li,
  • Pengju Lei,
  • Zhibin Liu,
  • Jichong Xia,
  • Shoudeng Wang,
  • Guixian Li,
  • Xinhong Zhao,
  • Dong Ji

摘要

Abstract

This study addresses the key issues of low activity and slow reaction rates in supported nickel-based catalysts for the hydrogenation of m-dinitrobenzene (DNB). Density Functional Theory (DFT) calculations revealed that the Ni(111) crystal plane exhibits the highest adsorption energy for the reactant, indicating its potential advantage in DNB hydrogenation. Based on this, using KBr as a structure-directing agent, a supported catalyst with a high proportion of exposed Ni(111) planes was prepared by regulating the crystal plane orientation of nickel nanoparticles. Characterization techniques including XRD, TEM, N2 physical adsorption-desorption, NH3-TPD, and XPS were used to systematically elucidate the mechanism of KBr’s regulation on crystal planes: KBr optimizes the exposure ratio of crystal planes by influencing the agglomeration-dispersion balance of particles. When the molar ratio of KBr to Ni is 50, the exposure proportion of the Ni(111) plane reached 80.81%. The prepared Ni-KBr-50/ZSM-5-Al catalyst exhibited optimal catalytic performance: DNB conversion reached 99.99% within 5 min, and m-phenylenediamine (MPD) selectivity reached 99.99%, consistent with the DFT-predicted trend of “high adsorption energy crystal plane promotes reaction activity.” Additionally, catalyst stability tests showed excellent stability: Ni-KBr-50/ZSM-5-Al maintained a DNB conversion of 99.99% over 10 recycling experiments, with MPD selectivity still reaching 98.71% in the 10th cycle.

Graphic Abstract