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Kesterite Cu2ZnSn(S, Se)4 (CZTSSe) solar cell has emerged as one of the mostpromising candidates for thin-film photovoltaics. However, severe charge lossesoccurring at the grain boundaries (GBs) of Kesterite polycrystalline absorbershas hindered the improvement of cell performance. Herein, we report a redoxreaction strategy involving palladium (Pd) to eliminate atomic vacancy defectssuch as VSn and VSe in GBs of the Kesterite absorbers. We demonstrate thatPdSex compounds could form during the selenization process and distribute atthe GBs and the absorber surfaces; thereby aid in the suppression of Sn and Sevolatilization loss and inhibiting the formation of VSn and VSe defects.Furthermore, Pd(II)/Pd(IV) serves as a redox shuttle, i.e., on one hand, Pd(II)captures Se vapor from the reaction environment to produce PdSe2, on the otherhand, PdSe2 provides Se atoms to the Kesterite absorber by being reduced toPdSe, thus contributing to the elimination of pre-existing VSe defects withinGBs. These effects collectively reduce defects and enhance the p-typecharacteristics of the Kesterite absorber, leading to a significant reductionin charge recombination loss within the cell. As a result, high-performanceKesterite solar cells with a total-area efficiency of 14.5% have been achieved.This remarkable efficiency increase benefited from the redox reaction strategyoffers a promising avenue for the precise regulation of defects in Kesteritesolar cells and holds generally significant implications for the exploration ofvarious other photovoltaic devices.

Defect Regulation by Palladium Incorporation towards Grain Boundaries of Kesterite solar cells