B-based catalysts are widely studied in the oxidative dehydrogenation of propane (ODHP) owing to their high selectivity. Correspondingly, two species, B−O oligomers and rings, have been recognized as active centers in B-based catalysts. To answer the essential question of whether B−O oligomers or ring species are more selective for ODHP, two AlB 2 catalysts enriched with B−O rings (R-AlB 2 ) and abundant B(OH) x O 3−x oligomers (O-AlB 2 ) were designed and compared herein. When tested in ODHP, R-AlB 2 exhibits an olefin yield of 30.2% at 500 °C, which is 2.3 times that of O-AlB 2 . Additionally, R-AlB 2 was stable for up to 200 h without deterioration. Multiple characterizations, including in situ Fourier transform infrared spectroscopy and theoretical calculations, demonstrate that B−O rings are more advantageous for producing propylene (C 3 = ) via a dehydration pathway with lower energy barriers and ethylene (C 2 = ) via two other reaction pathways (direct cracking of propane and oxidative coupling of methyl) B(OH) x O 3−x is primarily responsible for producing few C 3 = .
Since sluggish Li + desolvation leads to severe capacity degradation of carbon anodes at subzero temperatures, it is urgently desired to modulate electron configurations of surface carbon atoms toward high capacity for Li-ion batteries. Herein, a carbon-based anode material (O-DF) was strategically synthesized to construct the Riemannian surface with a positive curvature, which exhibits a high reversible capacity of 624 mAh g −1 with an 85.9% capacity retention at 0.1 A g −1 as the temperature drops to −20 °C. Even if the temperature drops to −35 °C, the reversible capacity is still effectively retained at 160 mAh g −1 after 200 cycles. Various characterizations and theoretical calculations reveal that the Riemannian surface effectively tunes the low-temperature sluggish Li + desolvation of the interfacial chemistry via locally accumulated charges of non-coplanar sp x (2 < x < 3) hybridized orbitals to reduce the rate-determining step of the energy barrier for the charge-transfer process. Ex-situ measurements further confirm that the sp x -hybridized orbitals of the pentagonal defect sites should denote more negative charges to solvated Li + adsorbed on the Riemannian surface to form stronger Li−C coordinate bonds for Li + desolvation, which not only enhances Li-adsorption on the curved surface but also results in more Li + insertion in an extremely cold environment.
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