<p>The selective conversion of biomass-derived alcohols to nitrogen-containing organic chemicals, such as the highly valuable imine, is a significant challenge due to the complex tandem process of C–N coupling and multiple reaction pathways. The photocatalytic coupling of biomass-derived alcohols with NH<sub>3</sub> using renewable energy offers a sustainable way to produce imines, but requires the development of suitable photocatalysts. In this work, we present a promising high-entropy sulfide photocatalyst (NiSnCaZnInS) with integrated multifunctional sites. Using benzyl alcohol (BA) as an example, we achieved an imine yield of 1240 μmol <InlineEquation ID="IEq1"><EquationSource Format="TEX">\({{\mbox{g}}}_{{\mbox{cat}}}^{-1}\)</EquationSource><EquationSource Format="MATHML"><math><msubsup><mrow><mstyle><mtext>g</mtext></mstyle></mrow><mrow><mstyle><mtext>cat</mtext></mstyle></mrow><mrow><mo>−</mo><mn>1</mn></mrow></msubsup></math></EquationSource></InlineEquation> for 5 hours, with a selectivity of 91.7%. The photocatalytic performance can be attributed to the special configuration of the high-entropy surface, which provides ideal catalytic sites for the cascade coupling reaction. This work highlights the great potential of high-entropy materials in photocatalytic reactions, providing a sustainable and effective approach to the photocatalytic conversion of biomass derivatives into valuable chemicals.</p>

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High-entropy photocatalyst enabling collaborative cascade C–N coupling for converting benzyl alcohol to imine

  • Nengcong Yang,
  • Yi Shu,
  • Zhian Chen,
  • Zhuwei Cao,
  • Haiqun Cao,
  • Sheng Ye,
  • Yujie Xiong

摘要

The selective conversion of biomass-derived alcohols to nitrogen-containing organic chemicals, such as the highly valuable imine, is a significant challenge due to the complex tandem process of C–N coupling and multiple reaction pathways. The photocatalytic coupling of biomass-derived alcohols with NH3 using renewable energy offers a sustainable way to produce imines, but requires the development of suitable photocatalysts. In this work, we present a promising high-entropy sulfide photocatalyst (NiSnCaZnInS) with integrated multifunctional sites. Using benzyl alcohol (BA) as an example, we achieved an imine yield of 1240 μmol \({{\mbox{g}}}_{{\mbox{cat}}}^{-1}\)gcat1 for 5 hours, with a selectivity of 91.7%. The photocatalytic performance can be attributed to the special configuration of the high-entropy surface, which provides ideal catalytic sites for the cascade coupling reaction. This work highlights the great potential of high-entropy materials in photocatalytic reactions, providing a sustainable and effective approach to the photocatalytic conversion of biomass derivatives into valuable chemicals.