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Cu2ZnSnSxSe4-x (CZTSSe) counter electrodes (CEs) in dye-sensitized solar cells (DSSCs) are commonly developed with porous structures, but their high surface area could also retard electron transport processes owing to the abundant grain boundaries. Herein, we employed a convenient solution method and a rapid heating process to prepare well crystalline CZTSSe CEs in DSSCs. The influence of crystallization of CZTSSe film on DSSCs performances was discussed in depth. The thermogravimetric analysis, phase morphology, conductivity, and electrochemical characteristics of CZTSSe films were performed. It is found that the rapid heating process is beneficial to the formation of well crystalline film with large grains. As the porosity and grain boundaries in the bulk film are dramatically reduced with the enhanced crystallization, the charge transport process is gradually improved. Using cyclic voltammogram and electrochemical impedance spectroscopy measurements, we propose that the accelerating charge transport is of great importance to the photovoltaic performances of DSSCs due to their superior electrocatalytic activities. As the highest cell efficiency was achieved, well crystalline CZTSSe is an efficient CE catalytic material.

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CZTS exhibited apparently phase-dependent photocatalytic H2 evolution under visible light. Possible factors for the phase-dependent photocatalytic activity of CZTS were discussed in detail.