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<p>Liquid organic hydrogen carriers (LOHCs) represent a highly promising strategy for hydrogen storage and long-distance transport, offering a safe and economically viable solution to key infrastructure challenges. The effective application of LOHCs requires dehydrogenation catalysts that strike an optimal balance between activity and stability. Herein, we report a precisely engineered CoO<sub><i>x</i></sub>-modified Pt/Al<sub>2</sub>O<sub>3</sub> catalytic system that exhibits outstanding performance in the dehydrogenation of perhydro-dibenzyltoluene (H18-DBT). Systematic investigations identify a critical CoO<sub><i>x</i></sub> loading threshold at 1 wt%, at which the catalyst achieves a maximum dehydrogenation degree (DoD) of 93% and a H<sub>2</sub> production rate of <InlineEquation ID="IEq1"> <EquationSource Format="TEX">\(20.98\times 10^{3}\ \text{mol}_{\mathrm{H}_{2}}\cdot \text{mol}_{\text{Pt}}^{-1}\cdot \mathrm{h}^{-1}\)</EquationSource> <EquationSource Format="MATHML"><math display="block"> <mn>20.98</mn> <mo>×</mo> <msup> <mn>10</mn> <mrow> <mn>3</mn> </mrow> </msup> <msub> <mtext>mol</mtext> <mrow> <msub> <mrow> <mi mathvariant="normal">H</mi> </mrow> <mrow> <mn>2</mn> </mrow> </msub> </mrow> </msub> <mo>⋅</mo> <msubsup> <mtext>mol</mtext> <mrow> <mtext>Pt</mtext> </mrow> <mrow> <mo>−</mo> <mn>1</mn> </mrow> </msubsup> <mo>⋅</mo> <msup> <mrow> <mi mathvariant="normal">h</mi> </mrow> <mrow> <mo>−</mo> <mn>1</mn> </mrow> </msup> </math></EquationSource> </InlineEquation> at 300 °C for dehydrogenation, outperforming all the catalysts reported in the literature. However, increasing the Co loading from 1 to 10 wt% results in a sharp decline in DoD from 93% to 7.2%. With the increasing CoO<sub><i>x</i></sub> content, the cobalt species initially form amorphous CoO clusters, which subsequently transform into crystalline Co<sub>3</sub>O<sub>4</sub>. The amorphous CoO is found to be the key species responsible for enhanced dehydrogenation activity by increasing the electron density and reducing the particle size of Pt, thereby promoting dehydrogenation while suppressing the hydrogenation capability.</p>

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Critical role of CoO modification on Pt/Al2O3 for efficient H18-DBT dehydrogenation in LOHC systems

  • 期刊论文

  • 发表日期：

    2026年4月1日

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  • Ligang Zhang,
  • Rudong Liu,
  • Chang Xu,
  • Chuanze Feng,
  • Sicong Qiu,
  • Nian Lei,
  • Kuo Liu,
  • Tao Zhang

摘要

Liquid organic hydrogen carriers (LOHCs) represent a highly promising strategy for hydrogen storage and long-distance transport, offering a safe and economically viable solution to key infrastructure challenges. The effective application of LOHCs requires dehydrogenation catalysts that strike an optimal balance between activity and stability. Herein, we report a precisely engineered CoOx-modified Pt/Al2O3 catalytic system that exhibits outstanding performance in the dehydrogenation of perhydro-dibenzyltoluene (H18-DBT). Systematic investigations identify a critical CoOx loading threshold at 1 wt%, at which the catalyst achieves a maximum dehydrogenation degree (DoD) of 93% and a H2 production rate of \(20.98\times 10^{3}\ \text{mol}_{\mathrm{H}_{2}}\cdot \text{mol}_{\text{Pt}}^{-1}\cdot \mathrm{h}^{-1}\) 20.98 × 10 3 mol H 2 ⋅ mol Pt − 1 ⋅ h − 1 at 300 °C for dehydrogenation, outperforming all the catalysts reported in the literature. However, increasing the Co loading from 1 to 10 wt% results in a sharp decline in DoD from 93% to 7.2%. With the increasing CoOx content, the cobalt species initially form amorphous CoO clusters, which subsequently transform into crystalline Co3O4. The amorphous CoO is found to be the key species responsible for enhanced dehydrogenation activity by increasing the electron density and reducing the particle size of Pt, thereby promoting dehydrogenation while suppressing the hydrogenation capability.