Pacific Northwest National Laboratory, Richland, WA, 99352, USA.
Faculty of Chemistry and Pharmacy, University of Sofia, Sofia, 1126, Bulgaria.
Nat Commun. 2021 Oct 15;12(1):6033. doi: 10.1038/s41467-021-26157-3.
CO oxidation is of importance both for inorganic and living systems. Transition and precious metals supported on various materials can oxidize CO to CO. Among them, few systems, such as Au/TiO, can perform CO oxidation at temperatures as low as -70 °C. Living (an)aerobic organisms perform CO oxidation with nitrate using complex enzymes under ambient temperatures representing an essential pathway for life, which enables respiration in the absence of oxygen and leads to carbonate mineral formation. Herein, we report that CO can be oxidized to CO by nitrate at -140 °C within an inorganic, nonmetallic zeolitic system. The transformation of NO and CO species in zeolite as well as the origin of this unique activity is clarified using a joint spectroscopic and computational approach.
CO 的氧化在无机和生命系统中都很重要。负载在各种材料上的过渡金属和贵金属可以将 CO 氧化为 CO。其中,像 Au/TiO 这样的少数体系可以在低至-70°C 的温度下进行 CO 氧化。在有氧和无氧的环境中,生活(需氧)生物体利用复杂的酶和硝酸盐来氧化 CO,这是生命的一个重要途径,它使呼吸在没有氧气的情况下进行,并导致碳酸盐矿物的形成。在此,我们报告了在无机非金属沸石体系中,硝酸盐可以在-140°C 下将 CO 氧化为 CO。我们使用联合光谱和计算方法,阐明了沸石中 NO 和 CO 物种的转化以及这种独特活性的起源。