Alivand Masood S, Mazaheri Omid, Wu Yue, Zavabeti Ali, Christofferson Andrew J, Meftahi Nastaran, Russo Salvy P, Stevens Geoffrey W, Scholes Colin A, Mumford Kathryn A
Department of Chemical Engineering, The University of Melbourne, Melbourne, Vic, 3010, Australia.
School of Agriculture and Food, Faculty of Veterinary and Agricultural Sciences, The University of Melbourne, Melbourne, Vic, 3010, Australia.
Nat Commun. 2022 Mar 10;13(1):1249. doi: 10.1038/s41467-022-28869-6.
Catalytic solvent regeneration has attracted broad interest owing to its potential to reduce energy consumption in CO separation, enabling industry to achieve emission reduction targets of the Paris Climate Accord. Despite recent advances, the development of engineered acidic nanocatalysts with unique characteristics remains a challenge. Herein, we establish a strategy to tailor the physicochemical properties of metal-organic frameworks (MOFs) for the synthesis of water-dispersible core-shell nanocatalysts with ease of use. We demonstrate that functionalized nanoclusters (FeO-COOH) effectively induce missing-linker deficiencies and fabricate mesoporosity during the self-assembly of MOFs. Superacid sites are created by introducing chelating sulfates on the uncoordinated metal clusters, providing high proton donation capability. The obtained nanomaterials drastically reduce the energy consumption of CO capture by 44.7% using only 0.1 wt.% nanocatalyst, which is a ∽10-fold improvement in efficiency compared to heterogeneous catalysts. This research represents a new avenue for the next generation of advanced nanomaterials in catalytic solvent regeneration.
催化溶剂再生因其在二氧化碳分离中具有降低能耗的潜力而备受关注，这使得工业能够实现《巴黎气候协定》的减排目标。尽管最近取得了进展，但开发具有独特特性的工程酸性纳米催化剂仍然是一项挑战。在此，我们建立了一种策略，用于调整金属有机框架（MOF）的物理化学性质，以合成易于使用的水分散性核壳纳米催化剂。我们证明，功能化纳米团簇（FeO-COOH）在MOF的自组装过程中有效地诱导了连接体缺失缺陷并制造了介孔。通过在未配位的金属簇上引入螯合硫酸盐来创建超强酸位点，从而提供高质子供体能力。所获得的纳米材料仅使用0.1 wt.%的纳米催化剂就能将二氧化碳捕获的能耗大幅降低44.7%，与多相催化剂相比，效率提高了约10倍。这项研究为催化溶剂再生中的下一代先进纳米材料开辟了一条新途径。
