Zhang Tong, Ren Peng, Qin Yuman, Vuong Thanh Huyen, Cunha Ana V, Havenith Remco W A, Rabeah Jabor, Das Shoubhik
Department of Chemistry, University of Antwerp, Antwerp, 2020, Belgium.
Department of Chemistry, University of Bayreuth, 95447, Bayreuth, Germany.
Adv Sci (Weinh). 2025 Jun;12(21):e2415339. doi: 10.1002/advs.202415339. Epub 2025 Mar 31.
Formic acid (FA) and its salt are recognized as valuable molecules for various industries such as textiles and pharmaceuticals. Currently, the global demand of FA and its salts stands at 1.137 million metric tons per year, necessitating the development of sustainable methods to meet the future demands. While numerous approaches are developed for the generation of FA but the requirement of harsh reaction conditions to achieve them is unavoidable. On the other hand, the world production of biomass is estimated at 146 billion metric tons per year and that can be considered as a prospective source of FA and their salts. Additionally, cellulose accounts for approximately 35-45% of the biomass composition. Considering this, a visible-light-mediated approach is presented to produce formate directly from biomass at room temperature as well as at atmospheric pressure. In this approach, selective generation of hydroxyl radical has been achieved which later converted sugars, cellulose, and hemicellulose into formate. Furthermore, the conversion of cellulose-rich daily-life materials such as discarded paper into the product through a series of flow experiments is demonstrated. Finally, mechanistic investigations including electron paramagnetic resonance (EPR) spectroscopy, and density functional theory (DFT) calculations are conducted to gain insights into the underlying reaction mechanism.
甲酸(FA)及其盐类被认为是纺织和制药等多个行业的重要分子。目前,全球对FA及其盐类的需求量为每年113.7万吨,因此有必要开发可持续的方法来满足未来需求。虽然已经开发了许多生成FA的方法,但实现这些方法不可避免地需要苛刻的反应条件。另一方面,全球每年生物质产量估计为1460亿吨,这可被视为FA及其盐类的潜在来源。此外,纤维素约占生物质成分的35%-45%。考虑到这一点,本文提出了一种可见光介导的方法,可在室温及大气压下直接从生物质中生产甲酸盐。在该方法中,已实现了羟基自由基的选择性生成,随后将糖类、纤维素和半纤维素转化为甲酸盐。此外,通过一系列流动实验展示了将废弃纸张等富含纤维素的日常生活材料转化为产品的过程。最后,进行了包括电子顺磁共振(EPR)光谱和密度泛函理论(DFT)计算在内的机理研究,以深入了解潜在的反应机理。