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One-pot hydrolytic hydrogenation of carbohydrates to hexitols catalyzed by Ru loaded P and Si-containing hierarchical porous biochars with excellent catalytic efficiency
Cellulose ( IF 5.7 ) Pub Date : 2022-06-07 , DOI: 10.1007/s10570-022-04650-2
Shuainan Chen, Feng Mao, Shimin Tang, Zheng Yi, Huanhuan Zhang, Jialuo She, Bo Yang, Chao Zhang, Yachun Liu, Zaihui Fu

The one-pot hydrolytic hydrogenation of carbohydrates to sugar alcohols is one of the important value-added transformations of biomass, but the hydrolysis efficiency of carbohydrates in this one-pot conversion is still limited by the high cleavage energy of their β-1,4-glycosidic bonds and the concomitant serious side-reactions. Therefore, it is necessary to develop the new acidic carriers to improve the key first-step hydrolysis. This paper discloses that a forestry processing waste bamboo powder can be converted into the P and Si-containing porous biochar (PSBC) via inserting silica sol, impregnating concentrated phosphoric acid (H3PO4) and heating carbonization. Due to the improved porosity and strong acidity of PSBC and its affinity to β-1,4-glycosidic bonds, this new acid carrier exhibits an outstanding catalysis performance for the hydrolysis of cellulose, cellobiose, especially sucrose and inulin, affording ca. 76.2% glucose yield in cellulose hydrolysis at 150 °C. More importantly, PSBC can efficiently and uniformly load Ru nanometer particles (average size of 1.5 nm) to fabricate 1%Ru/PSBC as an excellent bifunctional catalyst for the one-pot conversion of these carbohydrates to hexitols, affording ca. 85.2% hexitols with 51.7 h−1 turnover frequency in the one-pot conversion of cellulose under 150 °C and 3 MPa H2 pressure. This work not only provides an effective strategy for the preparation of biomass-derived bifunctional catalysts, but also it opens up new voyages for the development of efficient bio-refining.

Graphical abstract

Ru-loaded P and Si-containing porous biochar (1% Ru/PSBC) is an excellent bifunctional catalyst for the hydrolytic hydrogenation of carbohydrates under relatively mild conditions, affording ca. 85.2% hexitols with 51.7 h−1 TOF in the one-pot conversion of cellulose.



中文翻译:

具有优异催化效率的负载钌的含磷和硅的分级多孔生物炭催化碳水化合物一锅水解加氢制己糖醇

碳水化合物一锅水解加氢制糖醇是生物质重要的增值转化之一,但碳水化合物在这一一锅转化过程中的水解效率仍受限于其β-1,4的高裂解能-糖苷键和伴随的严重副反应。因此,有必要开发新的酸性载体来改善关键的第一步水解。本文公开了一种林业加工废竹粉通过插入硅溶胶、浸渍浓磷酸(H 3 PO 4) 和加热碳化。由于 PSBC 改善的孔隙率和强酸性及其对 β-1,4-糖苷键的亲和力,这种新型酸性载体对纤维素、纤维二糖,尤其是蔗糖和菊粉的水解表现出出色的催化性能,可提供ca。在 150 °C 下纤维素水解中的葡萄糖产率为 76.2%。更重要的是,PSBC 可以高效且均匀地负载 Ru 纳米颗粒(平均尺寸为 1.5 nm),以制造 1%Ru/PSBC 作为将这些碳水化合物一锅转化为己糖醇的优异双功能催化剂,提供ca。在 150 °C 和 3 MPa H 2下纤维素的一锅转化率中,85.2% 己糖醇的周转频率为 51.7 h -1压力。该工作不仅为生物质衍生双功能催化剂的制备提供了有效的策略,也为高效生物精炼的发展开辟了新的航程。

图形概要

负载 Ru 的 P 和 Si 多孔生物炭(1% Ru/PSBC)是一种优异的双功能催化剂,用于在相对温和的条件下对碳水化合物进行水解加氢,可提供 ca。在纤维素的一锅法转化中具有 51.7 h -1 TOF 的85.2% 己糖醇。

更新日期:2022-06-07
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