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调控碳化钼催化剂中的碳空位和低配位钼位点用于生物质光热催化转化为氢燃料

Regulating Carbon Vacancies and Undercoordinated Mo Sites in MoC Catalysts Toward Photo-Thermal Catalytic Conversion of Biomass Into H Fuel.

作者信息

Chen Yan, Cheng Miao, Ma Chi, Wang Zi-Yi, Tang Ji-Ping, Li Naixu, Guan Jie, Yuan Yong-Jun

机构信息

College of Materials and Environmental Engineering, Hangzhou Dianzi University, Hangzhou, 310018, People's Republic of China.

School of Chemistry, and Chemical Engineering, Southeast University, Nanjing, 211189, People's Republic of China.

出版信息

Small. 2025 Feb;21(6):e2409502. doi: 10.1002/smll.202409502. Epub 2024 Dec 25.

DOI:10.1002/smll.202409502
PMID:39722154
Abstract

The conversion of biomass into chemical fuels is exciting but quite challenging in the development of an effective conversion strategy to generate easily-separated products without energy consumption. Herein, a lignocellulosic biomass-to-H conversion system via photo-thermal catalysis over MoC hierarchical nanotube catalysts in an acidic solution, in which the lignocellulose is hydrolyzed to small organic molecules (such as glucose, etc) by dilute HSO, and then the resulting glucose is oxidized by MoC catalyst to generate H are reported. During the photo-thermal catalytic processes, the carbon vacancy in MoC catalysts results in the generation of undercoordinated Mo sites, which act as active sites for both biomass oxidation and H generation reactions. Thus, the successful photo-thermal catalytic conversion of common agricultural and forestry biomass including polar wood chip, bamboo, wheat straw, rice straw, corncob, and rice hull into H fuel is realized, and the highest H generation rate achieves 30 µmol g h in the wheat straw system. Outwork affords efficient noble-metal-free catalysts with adjustable active sites for photo-thermal catalytic conversion of lignocellulosic biomass into H.

摘要

在开发一种有效的转化策略以在无能量消耗的情况下生成易于分离的产物时,将生物质转化为化学燃料令人兴奋但颇具挑战性。在此,报道了一种在酸性溶液中通过MoC分级纳米管催化剂进行光热催化的木质纤维素生物质制氢转化系统,其中木质纤维素被稀硫酸水解为小分子有机化合物(如葡萄糖等),然后所得葡萄糖被MoC催化剂氧化以生成氢气。在光热催化过程中,MoC催化剂中的碳空位导致产生低配位的Mo位点,这些位点充当生物质氧化和氢气生成反应的活性位点。因此,实现了包括极地木屑、竹子、小麦秸秆、稻草、玉米芯和稻壳在内的常见农林生物质向氢燃料的成功光热催化转化,并且在小麦秸秆系统中最高产氢速率达到30 μmol g⁻¹ h⁻¹。这项工作提供了具有可调节活性位点的高效无贵金属催化剂,用于将木质纤维素生物质光热催化转化为氢气。

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