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<p>Photoreforming cellulose to simultaneously produce 5-hydroxymethylfurfural (5-HMF) and hydrogen represents a promising strategy for harnessing solar energy. However, the development of highly efficient photocatalysts for this reaction remains a challenge, and the influence of cellulose’s crystalline structure on conversion efficiency is not well understood. In this study, a Pt-modified g-C<sub>3</sub>N<sub>4</sub>–Bi<sub>3</sub>TiNbO<sub>9</sub> heterojunction photocatalyst was synthesized to explore the photocatalytic reforming of four crystalline forms of cellulose. The results demonstrate that the crystalline structure of cellulose significantly affects hydrogen and 5-HMF production, with the order of activity being cellulose III &gt; IV &gt; II &gt; I. Among the cellulose types tested, cellulose III exhibited the highest performance, achieving 51.8&#xa0;μmol&#xa0;g⁻<sup>1</sup>&#xa0;h⁻<sup>1</sup> of hydrogen and 113.4&#xa0;μmol&#xa0;g⁻<sup>1</sup>&#xa0;h⁻<sup>1</sup> of 5-HMF, surpassing the yields from cellulose I, II, and IV when using the Pt<sub>1.0</sub>–g-C<sub>3</sub>N<sub>4</sub>–Bi<sub>3</sub>TiNbO<sub>9</sub>(2:1) heterojunction. Additionally, a lower degree of polymerization of cellulose was found to favor the coproduction of hydrogen and 5-HMF, as it enhances the breakdown of cellulose via reactive species. Factors such as cellulose powder size, solution pH, and catalyst-cellulose interactions were also shown to influence the yields. Density functional theory (DFT) calculations revealed an electron migration of 0.019684e between the O 2<i>p</i> and Bi 6<i>p</i> orbitals of Bi<sub>3</sub>TiNbO<sub>9</sub>(220) and the C 2<i>p</i> and N 2<i>p</i> orbitals of g-C<sub>3</sub>N<sub>4</sub>, confirming interfacial electron transfer. The calculated adsorption energies followed the trend: cellulose IV (− 1.72&#xa0;eV) &gt; I (− 1.73&#xa0;eV) &gt; II (− 1.94&#xa0;eV) &gt; III (− 2.07&#xa0;eV), consistent with experimental results, except for cellulose IV.</p> Graphical abstract <p></p>

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Enhanced hydrogen and 5-hydroxymethylfurfural (5-HMF) production via photoreforming of cotton cellulose: role of cellulose allomorphs in Pt–g-C3N4–Bi3TiNbO9 catalysis

  • 期刊论文

  • 发表日期：

    2025年3月13日

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  • Xiang-Tao Xuan,
  • Hui Zhang,
  • Jia-Le Yao,
  • Ya-Ping Miao,
  • Wei Fan,
  • Xiang-Zhi Dong,
  • Chen-Min Dai,
  • Jiao-Jiao Miao

摘要

Photoreforming cellulose to simultaneously produce 5-hydroxymethylfurfural (5-HMF) and hydrogen represents a promising strategy for harnessing solar energy. However, the development of highly efficient photocatalysts for this reaction remains a challenge, and the influence of cellulose’s crystalline structure on conversion efficiency is not well understood. In this study, a Pt-modified g-C3N4–Bi3TiNbO9 heterojunction photocatalyst was synthesized to explore the photocatalytic reforming of four crystalline forms of cellulose. The results demonstrate that the crystalline structure of cellulose significantly affects hydrogen and 5-HMF production, with the order of activity being cellulose III > IV > II > I. Among the cellulose types tested, cellulose III exhibited the highest performance, achieving 51.8 μmol g⁻1 h⁻1 of hydrogen and 113.4 μmol g⁻1 h⁻1 of 5-HMF, surpassing the yields from cellulose I, II, and IV when using the Pt1.0–g-C3N4–Bi3TiNbO9(2:1) heterojunction. Additionally, a lower degree of polymerization of cellulose was found to favor the coproduction of hydrogen and 5-HMF, as it enhances the breakdown of cellulose via reactive species. Factors such as cellulose powder size, solution pH, and catalyst-cellulose interactions were also shown to influence the yields. Density functional theory (DFT) calculations revealed an electron migration of 0.019684e between the O 2p and Bi 6p orbitals of Bi3TiNbO9(220) and the C 2p and N 2p orbitals of g-C3N4, confirming interfacial electron transfer. The calculated adsorption energies followed the trend: cellulose IV (− 1.72 eV) > I (− 1.73 eV) > II (− 1.94 eV) > III (− 2.07 eV), consistent with experimental results, except for cellulose IV.

Graphical abstract