Kostera Sylwia, Gonsalvi Luca
Istituto di Chimica dei Composti Organometallici (ICCOM), Consiglio Nazionale delle Ricerche (CNR), Via Madonna del Piano 10, 50019, Sesto Fiorentino (Florence), Italy.
ChemSusChem. 2025 Mar 15;18(6):e202400639. doi: 10.1002/cssc.202400639. Epub 2024 Nov 27.
In the quest for sustainable hydrogen production, the use of biomass-derived feedstock is gaining importance. Acceptorless Dehydrogenation (AD) in the presence of efficient and selective catalysts has been explored worldwide as a suitable method to produce hydrogen from hydrogen-rich simple organic molecules. Among these, glycerol and sugars have the advantage of being inexpensive, abundant, and obtainable from fatty acid basic hydrolysis (biodiesel industry) and from biomass by biochemical and thermochemical processing, respectively. Although heterogeneous catalysts are more widely used for hydrogen production from biomass-based feedstock, the harsh reaction conditions often limit their applicability due to the deactivation of active sites caused by the coking of carbonaceous materials. Moreover, heterogeneous catalysts are more difficult to fine-tune than homogeneous counterparts, and the latter also allow for high process selectivities under milder conditions. The present Concept article summarizes the main features of the most active homogeneous catalysts reported for glycerol and monosaccharides AD. In order to directly compare hydrogen production efficiencies, the choice of literature works was limited to reports where hydrogen was clearly quantified by yields and turnover numbers (TONs). The types of transition metals and ligands are discussed, together with a perspective view on future challenges of homogeneous AD reactions for practical applications.
在寻求可持续制氢的过程中,使用生物质衍生原料正变得越来越重要。在高效且选择性的催化剂存在下进行的无受体脱氢反应(AD)已在全球范围内被探索为一种从富含氢的简单有机分子中制氢的合适方法。其中,甘油和糖类具有价格低廉、来源丰富的优势,分别可从脂肪酸碱性水解(生物柴油行业)以及通过生物质的生化和热化学加工获得。尽管多相催化剂在基于生物质的原料制氢中应用更为广泛,但由于含碳物质的结焦导致活性位点失活,苛刻的反应条件常常限制了它们的适用性。此外,多相催化剂比均相催化剂更难进行微调,而均相催化剂在更温和的条件下也能实现高的过程选择性。本概念文章总结了报道的用于甘油和单糖AD的最具活性的均相催化剂的主要特点。为了直接比较制氢效率,文献作品的选择仅限于通过产率和周转数(TONs)明确量化氢气的报道。文中讨论了过渡金属和配体的类型,并对均相AD反应在实际应用中的未来挑战给出了前瞻性观点。