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<p>The high hydrogen desorption density (19.6&#xa0;wt%) of ammonia borane (AB) makes it one of the most promising chemical hydrogen storage materials. Developing cost-effective catalysts is the key for accelerating the hydrolysis of AB. Herein, we present a straightforward synthesis method for the Cu<sub>2</sub>O decorated CoO catalyst derived from ZIF-67 precursors using carbothermal shock (~ 1&#xa0;s) in air. The obtained results demonstrate that a small amount of Cu<sub>2</sub>O doping into CoO synergistically enhances AB hydrolysis, resulting in an almost fivefold increase in turnover frequency (TOF = 97 <InlineEquation ID="IEq1"> <InlineMediaObject> <ImageObject Color="BlackWhite" FileRef="12598_2025_3290_Article_IEq1.gif" Format="GIF" Height="19" Rendition="HTML" Resolution="72" Type="Linedraw" Width="42" /> </InlineMediaObject> <EquationSource Format="TEX">\(\text{mol}_{\text{H}_{2}}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mtext>mol</mtext> <msub> <mtext>H</mtext> <mn>2</mn> </msub> </msub> </math></EquationSource> </InlineEquation> mol<sub>CoO</sub><sup>−1</sup>&#xa0;min<sup>−1</sup> at 298&#xa0;K). Further studies indicated that the incorporation of Cu<sub>2</sub>O alters the electronic distribution of the surface of catalysts, introducing more oxygen vacancies and increasing the pyridinic nitrogen content. The increased oxygen vacancies effectively enhanced the adsorption and activation ability of active sites for reactants (H<sub>2</sub>O and AB), while the targeting effect of pyridinic nitrogen enhances the dispersion of the catalyst. Theoretical analysis reveals that CoO plays a key role in the dissociation of H<sub>2</sub>O, while minor doping with Cu<sub>2</sub>O substantially reduces the dissociation energy barrier of AB. This research provides a novel strategy for the design and efficient preparation of AB hydrolysis catalysts for efficient hydrogen production.</p> Graphical abstract <p></p>

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Carbothermal shock fabrication of CoO-Cu2O nanocomposites on N-doped porous carbon for enhanced hydrolysis of ammonia borane

  • 期刊论文

  • 发表日期：

    2025年3月27日

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  • Jun-Rui Zhang,
  • Yun-Qi Jia,
  • Fei Chu,
  • Nuo Lei,
  • Jia-Peng Bi,
  • Hai-Ying Qin,
  • Mi-Li Liu,
  • Yu-Xiao Jia,
  • Lan Zhang,
  • Lin Jiang,
  • Liu-Zhang Ouyang,
  • Xue-Zhang Xiao

摘要

The high hydrogen desorption density (19.6 wt%) of ammonia borane (AB) makes it one of the most promising chemical hydrogen storage materials. Developing cost-effective catalysts is the key for accelerating the hydrolysis of AB. Herein, we present a straightforward synthesis method for the Cu2O decorated CoO catalyst derived from ZIF-67 precursors using carbothermal shock (~ 1 s) in air. The obtained results demonstrate that a small amount of Cu2O doping into CoO synergistically enhances AB hydrolysis, resulting in an almost fivefold increase in turnover frequency (TOF = 97 \(\text{mol}_{\text{H}_{2}}\) mol H 2 molCoO−1 min−1 at 298 K). Further studies indicated that the incorporation of Cu2O alters the electronic distribution of the surface of catalysts, introducing more oxygen vacancies and increasing the pyridinic nitrogen content. The increased oxygen vacancies effectively enhanced the adsorption and activation ability of active sites for reactants (H2O and AB), while the targeting effect of pyridinic nitrogen enhances the dispersion of the catalyst. Theoretical analysis reveals that CoO plays a key role in the dissociation of H2O, while minor doping with Cu2O substantially reduces the dissociation energy barrier of AB. This research provides a novel strategy for the design and efficient preparation of AB hydrolysis catalysts for efficient hydrogen production.

Graphical abstract