物理化学学报

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通过强吸附H2O促进Co/Sr2.5Al4.5光热催化纤维素蒸汽重整制合成气

武继春, 张钰璐, 李远志, 江祥龙, 赵晨旭   

  1. 武汉理工大学酸盐科学与先进建材全国重点实验室, 湖北 武汉 430070
  • 收稿日期:2026-08-06 修回日期:2026-09-09 录用日期:2026-09-10
  • 通讯作者: 李远志 E-mail:liyuanzhi@whut.edu.cn
  • 基金资助:
    本工作得到国家自然科学基金(21972109)的资助。

Boosting photothermocatalytic cellulose steam reforming to syngas over Co/Sr2.5Al4.5 via strongly adsorbed H2O

Jichun Wu, Yulu Zhang, Yuanzhi Li, Xianglong Jiang, Chenxu Zhao   

  1. State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, Hubei Province, China
  • Received:2026-08-06 Revised:2026-09-09 Accepted:2026-09-10
  • Contact: Yuanzhi Li E-mail:liyuanzhi@whut.edu.cn

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摘要： 光热催化是一种具有前景且节能的纤维素蒸汽重整(Cellu-SR)路线；然而，其实际应用受到不良副产物生成的严重限制——尤其是焦油。在此，我们报道了一种负载于Sr改性Al2O3上的Co纳米颗粒催化剂(Co/Sr2.5Al4.5)，该催化剂在光热催化Cellu-SR中表现出优异性能。在光照下，该催化剂表现出很高的H2生成速率(5101.4 mmol g-1 h-1)和CO生成速率(3061.7 mmol g-1 h-1)，同时副产物生成被显著抑制——最突出的是焦油选择性低于20%。系统物理化学表征表明，优异性能归因于Sr的引入显著增强了H2O吸附。由此产生的表面吸附H2O更容易解离生成活性氧物种(O*)，可以高效地将纤维素衍生的热解中间体(CxHyOz)和碳物种(C*)氧化为合成气。更为关键的是，光照诱发了显著的光活化效应，削弱了表面Co-O键，促进了O*对C*的氧化，进一步促进了H2O高效参与重整。

关键词: 光热催化, 纤维素蒸汽重整, 钴基催化剂, 锶改性, 光活化

Abstract: Photothermocatalysis represents a promising, energy-efficient route for cellulose steam reforming (Cellu-SR); however, its practical implementation is severely limited by the undesired formation of byproducts—particularly tar. Herein, we report a Co nanoparticle catalyst supported on Sr-modified Al2O3 (Co/Sr2.5Al4.5) that achieves exceptional performance in photothermocatalytic Cellu-SR. Under illumination, this catalyst delivers remarkably high production rates of H2 (5101.4 mmol g-1 h-1) and CO (3061.7 mmol g-1 h-1), accompanied by markedly suppressed byproduct formation—most notably, a tar selectivity below 20%. Systematic physicochemical characterizations reveal that the outstanding performance is attributed to the introduction of Sr significantly enhances the H2O adsorption. The resulting surface-adsorbed H2O readily dissociates to generate reactive oxygen species (O*), which efficiently oxidize cellulose-derived pyrolysis intermediates (CxHyOz) and carbon species (C*) to syngas. Crucially, illumination induces a pronounced photoactivation effect on weaking the surface Co-O bonds, facilitating the oxidation of C* by O* and promoting the active participation of H2O in the reforming.

Key words: Photothermocatalysis, Cellulose steam reforming, Co-based catalyst, Sr modification, Photoactivation