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.

中文翻译：

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碳阳极上的黎曼表面可在 −35 °C 下存储锂离子

由于缓慢的 Li ⁺去溶剂化会导致碳负极在零下温度下严重的容量退化，因此迫切需要调节表面碳原子的电子构型以实现锂离子电池的高容量。在此，战略性地合成了一种碳基负极材料 (O-DF)，以构建具有正曲率的黎曼表面，其具有 624 mAh g ^{-1的高可逆容量，在 0.1 A g -1}下具有 85.9% 的容量保持率随着温度下降到-20°C。即使温度降至-35°C，可逆容量仍有效保持在160 mAh g ^–1200 次循环后。各种表征和理论计算表明，黎曼表面通过非共面 sp ^x (2 < x < 3) 杂化轨道的局部累积电荷有效地调节了界面化学的低温缓慢 Li ⁺去溶剂化，从而减少了速率决定步骤电荷转移过程的能垒。异位测量进一步证实，五边形缺陷位点的 sp ^x -杂化轨道应表示更多的负电荷，以使吸附在黎曼表面上的溶剂化 Li ⁺形成更强的 Li-C 配位^键去溶剂化，这不仅增强了Li在曲面上的吸附，而且在极冷的环境中导致更多的Li ⁺嵌入。