Dostagir Nazmul Hasan Md, Suzuki Yusuke, Song Zhiyi, Kobayashi Hirokazu, Shrotri Abhijit, Fukuoka Atsushi
Institute for Catalysis, Hokkaido University, Kita 21 Nishi 10, Kita-ku, Sapporo, Hokkaido 001-0021, Japan.
Komaba Institute for Science, The University of Tokyo, 3-8-1 Komaba, Meguro-ku, Tokyo 153-8902, Japan.
ACS Omega. 2025 May 31;10(22):23058-23063. doi: 10.1021/acsomega.5c01102. eCollection 2025 Jun 10.
Hydrolysis of cellulose to glucose is a challenging and crucial step in the field of biomass conversion to fuels and value-added chemicals. Despite the abundance of cellulose, its recalcitrant crystalline structure presents a challenge for its depolymerization to smaller molecules. Conventional heterogeneous catalysts are unable to access glycosidic bonds in cellulose, necessitating cost-consuming pretreatments such as ball-milling. Here, we report a novel approach based on heterogeneous molecular moieties that adsorb on the cellulose surface and hydrolyze cellulose. Three compounds featuring an adsorption domain in the form of a pyrene moiety and vicinal carboxylic acids as an active site were synthesized and tested. By harnessing the cellulose-binding properties of pyrene and the weak acidic functional groups for hydrolysis, these compounds demonstrated enhanced rates of hydrolysis without the need for pretreatment. Glucose yield was increased at a mild temperature of 150 °C in water in the presence of molecular compounds. This work shows a new design idea that can overcome the issues associated with solid acid catalysts for the hydrolysis of crystalline cellulose.
纤维素水解为葡萄糖是生物质转化为燃料和增值化学品领域中一个具有挑战性的关键步骤。尽管纤维素储量丰富,但其顽固的晶体结构对其解聚为小分子构成了挑战。传统的多相催化剂无法作用于纤维素中的糖苷键,因此需要诸如球磨等成本高昂的预处理。在此,我们报道了一种基于吸附在纤维素表面并水解纤维素的多相分子部分的新方法。合成并测试了三种化合物,它们具有芘部分形式的吸附域和邻位羧酸作为活性位点。通过利用芘的纤维素结合特性和用于水解的弱酸性官能团,这些化合物在无需预处理的情况下表现出更高的水解速率。在分子化合物存在下,于150℃的温和水温中,葡萄糖产率得以提高。这项工作展示了一种新的设计理念,可克服与用于结晶纤维素水解的固体酸催化剂相关的问题。