Controlling electrode/electrolyte interfacial chemistry is critically important for improved K+ storage, but the influences of binder chemistry on electrolyte decomposition and interfacial properties are still poorly understood. Herein, sodium carboxymethyl cellulose (CMC)‐based, and polyvinylidene fluoride (PVDF)‐based graphite electrodes are introduced as model systems to quantify the electrolyte decomposition, solid electrolyte interphase (SEI) formation, and the corresponding kinetic evolution transition. A noncatalytic electrolyte reduction path on the CMC‐based electrode and a catalytic reduction path on the PVDF‐based electrode are identified, in terms of the reduction overpotential and product selectivity. The electrolyte reduction and/or SEI formation are found to occur in a successive, two‐step manner, starting with the electrochemical reduction at a potential above 0.35 V where no potassiation has happened (step I), and followed by the thermodynamically accelerated electrolyte reduction at a potential below 0.35 V (step II). Kinetics analysis reveals the former is charge transfer‐controlled for both CMC and PVDF‐based electrodes, and the latter involves a kinetic transition to SEI resistance controlled for the PVDF system, while it is charge transfer‐controlled for the CMC system. All these examples, highlight that binder chemistry plays a dominant role in the electrolyte decomposition and electrode/electrolyte interfacial properties, and promote a better fundamental understanding of electrolyte reduction.

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As an ideal anode material of lithium metal for highenergy-density batteries, the development of lithium metal batteries (LMBs) has been limited by the Li dendrite's growth and accumulation of dead Li. To solve this problem, a highly elastic artificial polymer layer coated on the surface Li anode by rapid ultraviolet radical polymerization is developed. The clad poly-(methyl methacrylate-acrylic acid-sulfobetaine methacrylate) (P-(MMA-AA-SBMA)) terpolymer not only shows good interfacial compatibility with Li metal due to the surface formation process by in situ light solidification but also contains functional anion groups of −COO − and −SO 3 − , contributing the convenient channels to regulate the transport of Li ions. Ascribed from the stable interface of clad Li and the suppressed decomposition reaction of the liquid electrolyte in the later cycle stage, the Li||LiCoO 2 full cell exhibits good cycle stability, maintaining 96% of initial capacity after 100 cycles in 1C rate between 3 and 4.35 V, compared with that of 67% for bare Li. Thus, the artificial polymer cladding promotes the electrochemical stability of Li metal, providing a facile way for application in high-energy-density LMBs.