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Heterogeneous electrocatalysis closely relies on the electronic structure of the catalytic materials. The ferroelectric‐to‐paraelectric phase transition of the materials also involves a change in the state of electrons that could impact the electrocatalytic activity, but such correlation remains unexplored. Here, we demonstrate experimentally and theoretically that the intrinsic electrocatalytic activity could be regulated as exampled by hydrogen evolution reaction catalysis over two‐dimensional ferroelectric CuInP2S6. The obvious discontinuity in the overpotential and apparent activation energy values for CuInP2S6 electrode are illustrated during the ferroelectric‐to‐paraelectric phase transition caused by copper displacement around Tc point (318 K), revealing the ferroelectro‐catalytic effect on thermodynamics and kinetics of electrocatalysis. When loading Pt single atom on the CuInP2S6, the paraelectric phase one showed an improved hydrogen evolution activity with smaller apparent activation energy over the ferroelectric phase counterpart. This is attributed to the copper hopping between two sulfur planes, which alternate between strong and weak H adsorption at the Pt sites to simultaneously promote H+ reactant adsorption and H2 product desorption. [ABSTRACT FROM AUTHOR]

Large‐scale implementation of all‐solid‐state lithium batteries is impeded by the physical limitations of the interface between the electrode and solid electrolyte; specifically, high resistance and poor stability, as well as poor compatibility with Li+ migration. We report double ionic–electronic transfer interface layers grown at electrode–electrolyte interfaces by in situ polymerization of 2,2′‐bithiophene in polyethylene oxide (PEO) electrolyte. For all‐solid‐state LiFePO4∥PT‐PEO‐PT∥Li cells, the formation of a conductive polythiophene (PT) layer at the cathode–electrolyte interface resulted in an at least sevenfold decrease in interface resistance, and realized a capacity retention of about 94 % after 1000 cycles along with a lower polarization voltage under a rate of 2 C. The mixed ionic–electronic conductive layers imparted superior interface stability and contact while keeping good compatibility with the Li anode. [ABSTRACT FROM AUTHOR]