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Nano+Lett 2025 ; ? (?): ? Nephropedia Template TP
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Unpaired Electrons-Empowered Bridge-Site Lattice Oxygen for Efficient CO(2)-to-CH(4) Conversion via a CO(2)/H(2) Fuel Cell #MMPMID41389024
Liu Y; Hu J; Cui Z; Chen Y; Yu W; Hu Y; Guo S; Liu Y; Dong J; Guo Z
Nano Lett 2025[Dec]; ? (?): ? PMID41389024show ga
CO(2)/H(2) fuel cells represent a promising route for simultaneous CO(2) conversion and power generation, yet face efficiency limitations due to poor CO(2) activation. Effective reduction requires rapid electron transfer to CO(2)'s lowest unoccupied molecular orbital, which conventional catalysts struggle to achieve. Herein, we design a RuO(2)-based catalyst featuring abundant unpaired electrons that simultaneously enrich bridge-site lattice oxygen and metal centers. These electron enrichments enable efficient electron transfer to CO(2), significantly enhancing activation. In a CO(2)/H(2) fuel cell, this catalyst achieves a CO(2) conversion rate of 1242.5 mumol g(cat)(-1) h(-1) horizontal line 18 times that of RuO(2)/CNTs, while contributing 28.2% of electricity generation versus 1.5% for RuO(2)/CNTs. In situ Raman spectroscopy reveals enhanced activation through B(2g)-mode vibrations under CO(2). Experimental and theoretical analyses verify orbital hybridization involving both Ru 3d and O 2p orbitals with CO(2)'s pi* orbitals, synergistically promoting adsorption. This work establishes a dual-site activation strategy for developing CO(2) reduction catalysts.
Nano+Lett 2025 ; ? (?): ?
