Rational Design of S-Scheme Heterojunction toward Efficient Photocatalytic Cellulose Reforming for H2 and Formic Acid in Pure Water,Advanced Materials

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Rational Design of S-Scheme Heterojunction toward Efficient Photocatalytic Cellulose Reforming for H2 and Formic Acid in Pure Water
Advanced Materials ( IF 27.4 ) Pub Date : 2023-10-08 , DOI: 10.1002/adma.202307962
Yang You ₁ , Shangxian Chen ₁ , Jie Zhao ₁ , Jianfeng Lin ₁ , Donglian Wen ₁ , Pengzhan Sha ₁ , Libo Li ₂ , Donglei Bu ₁ , Shaoming Huang _{1,

3}

Affiliation

Photocatalytic cellulose reforming usually requires harsh conditions due to its sluggish kinetics. Here, a hollow structural S-scheme heterojunction of ZnSe and oxygen vacancy enriched TiO₂, namely, h-ZnSe/Pt@TiO₂, is designed and fabricated, with which the photocatalytic reforming of cellulose for H₂ and formic acid is realized in pure water. H₂ and formic acid productivity of 1858 and 372 µmol g⁻¹ h⁻¹ and a steady H₂ evolution for 300 h are achieved with α-cellulose. Comparable photocatalytic activity can also be achieved using various cellulose sources. It is experimentally proven that the photogenerated charge transfer follows an S-scheme mechanism, which not only promotes the charge separation but also preserves the higher reductive and oxidative abilities of the ZnSe and TiO₂, respectively. Furthermore, the polyhydroxy species produced during cellulose degradation are favored to adsorb on the oxygen vacancy enriched TiO₂ surface, which promotes the photocatalytic reforming process and is accounted to the preservation of formic acid as the major solution-phase product. In addition, sequential reactions of oxidation of aldehydes and elimination of formic acid of the cellulose degradation process are revealed. This work provides a photocatalytic strategy to sustainably produce hydrogen and value-added chemicals from biomass under the most environmentally benign condition, i.e., pure water.

中文翻译：

S型异质结的合理设计，用于纯水中氢气和甲酸的高效光催化纤维素重整

由于其动力学缓慢，光催化纤维素重整通常需要苛刻的条件。本文设计并制备了ZnSe和富氧空位TiO ₂的中空结构S型异质结，即h-ZnSe/Pt@TiO ₂ ，实现了纤维素对H ₂和甲酸的光催化重整。纯净水。使用α-纤维素实现了1858和372 µmol g ^-1 h ^-1的H ₂和甲酸生产率以及300小时的稳定H ₂释放。使用各种纤维素源也可以实现相当的光催化活性。实验证明，光生电荷转移遵循S型机制，不仅促进了电荷分离，而且分别保留了ZnSe和TiO ₂较高的还原和氧化能力。此外，纤维素降解过程中产生的多羟基物质有利于吸附在富氧空位的TiO ₂表面上，这促进了光催化重整过程，并且有助于将甲酸保存为主要溶液相产物。此外，还揭示了纤维素降解过程中醛的氧化和甲酸的消除的连续反应。这项工作提供了一种光催化策略，可以在最环保的条件（即纯水）下从生物质中可持续地生产氢气和增值化学品。

更新日期：2023-10-08

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