Dual-carbon cells are a promising candidate for new energy storage devices. Recently, a 4V asymmetric capacitor based on non-metal electrolytes has been proposed. Two kinds of mesocarbon microbeads（MCMB）samples with different treatments (potassium hydroxide activated MCMB and graphitized MCMB, labeled as AMCMB and GMCMB, respectively) have served as electrode materials in this study. The charge storage behaviors of MCMB electrodes are studied by in situ X-ray diffraction (XRD), in situ dilatometry and conventional electrochemical measurements. (−)AMCMB/GMCMB(+) is synergistically diagnosed as a superior electrode collocation from the viewpoint of structural changes, which consists of adequate activation (7.65% irrecoverable expansion) for AMCMB and suitable stretch (13.67% recoverable expansion) for GMCMB. The intercalation-induced activation of AMCMB is indiscernible in XRD patterns but becomes conspicuous as dilatometric responses. A quantitative correlation between the two in situ measurements is established in the research of GMCMB electrodes. Expansions in the two dimensions are closely related to the type and size of intercalated ions, the shrinkage behavior of electrodes is especially synchronous in the discharging process. These findings guide the design of advanced cells and emphasize the necessity combining in situ characterizations.

双碳电池是新能源存储设备的有前途的候选者。最近，已经提出了一种基于非金属电解质的4V不对称电容器。两种不同处理方式的中碳微珠（MCMB）样品（氢氧化钾活化的MCMB和石墨化的MCMB，分别标记为AMCMB和GMCMB）作为电极材料。MCMB电极的电荷存储行为进行了研究通过原位X射线衍射（XRD），在原地膨胀计和常规电化学测量。从结构变化的观点来看，（-）AMCMB / GMCMB（+）被协同诊断为优越的电极搭配，包括对AMCMB的充分活化（7.65％不可恢复的膨胀）和对GMCMB的适当拉伸（可恢复的13.6％的膨胀）。插层诱导的AMCMB激活在XRD模式中是不可识别的，但在膨胀测量响应中变得很明显。两者之间的定量关系原位测量是在GMCMB电极的研究中建立的。二维中的膨胀与嵌入离子的类型和大小密切相关，电极的收缩行为在放电过程中尤其同步。这些发现指导了先进细胞的设计，并强调了结合原位表征的必要性。