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<p>The development of efficient catalysts for ethane dehydrogenation (EDH) to ethylene remains a challenge due to the lack of direct material property-performance relationships at the most elementary level. Here, we introduce the first application of ZrO<sub>2</sub>-based catalysts for EDH in a chemical looping mode. Their performance in the first 1 minute, primarily via the oxidative dehydrogenation, highlights their potential for large-scale ethylene production. LaZrO<sub><i>x</i></sub> achieves a space-time yield of 2.26 <InlineEquation ID="IEq1"> <InlineMediaObject> <ImageObject Color="BlackWhite" FileRef="41467_2025_64246_Article_IEq1.gif" Format="GIF" Height="25" Rendition="HTML" Resolution="72" Type="Linedraw" Width="141" /> </InlineMediaObject> <EquationSource Format="TEX">\({{\mbox{kg}}}_{{{\mbox{C}}}_{2}{{\mbox{H}}}_{4}}\cdot {{\mbox{kg}}}_{{\mbox{cat}}}^{-1}\cdot {{\mbox{h}}}^{-1}\)</EquationSource> <EquationSource Format="MATHML"><math> <msub> <mrow> <mstyle> <mtext>kg</mtext> </mstyle> </mrow> <mrow> <msub> <mrow> <mstyle> <mtext>C</mtext> </mstyle> </mrow> <mrow> <mn>2</mn> </mrow> </msub> <msub> <mrow> <mstyle> <mtext>H</mtext> </mstyle> </mrow> <mrow> <mn>4</mn> </mrow> </msub> </mrow> </msub> <mo>⋅</mo> <msubsup> <mrow> <mstyle> <mtext>kg</mtext> </mstyle> </mrow> <mrow> <mstyle> <mtext>cat</mtext> </mstyle> </mrow> <mrow> <mo>−</mo> <mn>1</mn> </mrow> </msubsup> <mo>⋅</mo> <msup> <mrow> <mstyle> <mtext>h</mtext> </mstyle> </mrow> <mrow> <mo>−</mo> <mn>1</mn> </mrow> </msup> </math></EquationSource> </InlineEquation> at about 80% ethylene selectivity and 50% ethane conversion at 700 °C. Mechanistic studies have identified the reactivity and availability of lattice oxygen as crucial descriptors for mitigating coke formation and suppressing combustion reactions. These properties can be tuned by exposing less stable ZrO<sub>2</sub> crystal planes or incorporating metal-oxide promoters. Strongly adsorbed oxygen species can also participate in ethane oxidation. Thus, this study establishes a catalyst system for chemical looping EDH and provides insights for designing more efficient EDH catalysts.</p>

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Regulation of lattice oxygen reactivity of ZrO2 to promote efficient chemical looping oxidative dehydrogenation of ethane

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年9月29日

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  • Tao Zhang,
  • Tatiana Otroshchenko,
  • Vita A. Kondratenko,
  • Stephan Bartling,
  • Evgenii V. Kondratenko

摘要

The development of efficient catalysts for ethane dehydrogenation (EDH) to ethylene remains a challenge due to the lack of direct material property-performance relationships at the most elementary level. Here, we introduce the first application of ZrO2-based catalysts for EDH in a chemical looping mode. Their performance in the first 1 minute, primarily via the oxidative dehydrogenation, highlights their potential for large-scale ethylene production. LaZrOx achieves a space-time yield of 2.26 \({{\mbox{kg}}}_{{{\mbox{C}}}_{2}{{\mbox{H}}}_{4}}\cdot {{\mbox{kg}}}_{{\mbox{cat}}}^{-1}\cdot {{\mbox{h}}}^{-1}\) kg C 2 H 4 ⋅ kg cat − 1 ⋅ h − 1 at about 80% ethylene selectivity and 50% ethane conversion at 700 °C. Mechanistic studies have identified the reactivity and availability of lattice oxygen as crucial descriptors for mitigating coke formation and suppressing combustion reactions. These properties can be tuned by exposing less stable ZrO2 crystal planes or incorporating metal-oxide promoters. Strongly adsorbed oxygen species can also participate in ethane oxidation. Thus, this study establishes a catalyst system for chemical looping EDH and provides insights for designing more efficient EDH catalysts.