Eisele Lisa, Hulaj Bletë, Podsednik Maximilian, Laudani Francesco, Ayala Pablo, Cherevan Alexey, Foelske Annette, Limbeck Andreas, Eder Dominik, Bica-Schröder Katharina
Institute of Applied and Synthetic Chemistry, TU Wien Getreidemark 9/163 1060 Wien Austria
KAI Kompetenzzentrum Automobil- und Industrieelektronik GmbH Argentinierstraße 8 1040 Wien Austria.
RSC Sustain. 2024 Jul 17;2(9):2524-2531. doi: 10.1039/d4su00194j. eCollection 2024 Aug 28.
Photocatalytic production of CO from CO has the potential for safe and atom-economic production of feedstock chemicals carbonylation chemistry. We developed novel ionic liquid-based polymeric materials through radical copolymerisation of 1-butyl-3-vinylimidazolium chloride and photocatalytically active Re- and Ru-complexes that serve as the CO reduction catalyst and photosensitiser, respectively. The crosslinked polymeric framework allows for the facile immobilisation of molecular organometallic complexes for use as heterogenised catalysts; moreover, the involved imidazolium core units co-catalyze the reduction of CO covalent interaction. The ratio of sensitiser and catalyst was analysed by laser ablation inductively coupled plasma mass spectroscopy (LA-ICP-MS) and set in relation to results from photocatalytic experiments. Ultimately, the heterogenous polymeric framework showed high selectivity for CO formation on photocatalytic CO reduction with improved stability to the corresponding homogenous system.
通过光催化将一氧化碳转化为一氧化碳有潜力实现安全且原子经济的原料化学品生产——羰基化化学。我们通过1-丁基-3-乙烯基咪唑氯化物与分别作为一氧化碳还原催化剂和光敏剂的具有光催化活性的铼和钌配合物进行自由基共聚,开发了新型离子液体基聚合物材料。交联的聚合物骨架允许分子有机金属配合物轻松固定,用作多相催化剂;此外,所涉及的咪唑核心单元通过共价相互作用共同催化一氧化碳的还原。通过激光烧蚀电感耦合等离子体质谱法(LA-ICP-MS)分析了光敏剂和催化剂的比例,并将其与光催化实验结果相关联。最终,这种多相聚合物骨架在光催化一氧化碳还原生成一氧化碳方面表现出高选择性,并且相对于相应的均相体系具有更高的稳定性。