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<p>The new supported mesoporous nanoparticles RuNPs, decorated as RuNPs@[KIT-6]-NH<sub>2</sub> <b>4</b> and RuNPs@[KIT-6]-NH<sub>2</sub>-imid <b>5</b>, were synthesized by a chemical modification of silica surface procedure utilizing the [KIT-6] <b>1</b>, then RuCl<sub>3</sub>.3H<sub>2</sub>O reduced by sodium borohydride. RuNPs <b>4</b> and <b>5</b> were characterised by <sup>29</sup>Si solid-state NMR, SEM, XPS, and TEM. The influence of different factors, for example, reaction time, temperature, catalyst loading, and concentration of NBH<sub>4</sub>, were examined to achieve the best catalytic conditions. RuNPs <b>4</b> and <b>5</b> catalyse the release of H<sub>2</sub> from sodium borohydride with remarkable proficiencies, and RuNP <b>5</b> catalyst was found to be more effective than its counterpart <b>4</b>. The hydrolytic reaction generates H<sub>2</sub> in the presence of (2 mg, 0.18 mol) of catalyst <b>5</b> at 20 °C conducting 163.3 mole<sub>H2</sub> mol<sub>cat</sub><sup>−1</sup>&#xa0;min<sup>−1</sup> of TOF. The study of kinetics discovered that the hydrogen generation process is first order with activation energy E<sub>a</sub> of 35.7 kJ mol<sup>−1</sup> for both catalysts <b>5</b> and <b>4</b>. The RuNPs <b>5</b> efficacy for the H<sub>2</sub> production reaction of NaBH<sub>4</sub> was conducted in D<sub>2</sub>O and H<sub>2</sub>O showed that the catalytic process is significantly more rapid in water than in D<sub>2</sub>O indicating the solvent isotope KIE <i>k</i><sub><i>H</i></sub><i>/k</i><sub><i>D</i></sub> = 1.5 which is consistent with the determination step of rate includes cleavage of O–H of H<sub>2</sub>O. This difference in this initial value of rate may be due to not occurring the bond cleavage of B–OD in the determination step of rate. Furthermore, the good repeatability of catalytic hydrolysis for RuNPs based [KIT]-NH<sub>2</sub>-imid mesoporous silica <b>5</b> retains 87% of the primary catalytic activity after the 4th runs.</p>

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Synthesis of enhanced imidazolium ionic liquid and amino immoblised mesoporous silica supported ruthenium nanoparticle for H2 generation from NaBH4

  • 期刊论文

  • 发表日期：

    2025年3月12日

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  • Hind Alshaikh

摘要

The new supported mesoporous nanoparticles RuNPs, decorated as RuNPs@[KIT-6]-NH2 4 and RuNPs@[KIT-6]-NH2-imid 5, were synthesized by a chemical modification of silica surface procedure utilizing the [KIT-6] 1, then RuCl3.3H2O reduced by sodium borohydride. RuNPs 4 and 5 were characterised by 29Si solid-state NMR, SEM, XPS, and TEM. The influence of different factors, for example, reaction time, temperature, catalyst loading, and concentration of NBH4, were examined to achieve the best catalytic conditions. RuNPs 4 and 5 catalyse the release of H2 from sodium borohydride with remarkable proficiencies, and RuNP 5 catalyst was found to be more effective than its counterpart 4. The hydrolytic reaction generates H2 in the presence of (2 mg, 0.18 mol) of catalyst 5 at 20 °C conducting 163.3 moleH2 molcat−1 min−1 of TOF. The study of kinetics discovered that the hydrogen generation process is first order with activation energy Ea of 35.7 kJ mol−1 for both catalysts 5 and 4. The RuNPs 5 efficacy for the H2 production reaction of NaBH4 was conducted in D2O and H2O showed that the catalytic process is significantly more rapid in water than in D2O indicating the solvent isotope KIE kH/kD = 1.5 which is consistent with the determination step of rate includes cleavage of O–H of H2O. This difference in this initial value of rate may be due to not occurring the bond cleavage of B–OD in the determination step of rate. Furthermore, the good repeatability of catalytic hydrolysis for RuNPs based [KIT]-NH2-imid mesoporous silica 5 retains 87% of the primary catalytic activity after the 4th runs.