The production of ultra-pure raw material is a crucial step to ensure the required background level in rare event searches. In this work, we establish an innovative technique developed to produce high-purity (99.999%) granular zinc. We demonstrate the effectiveness of the refining procedure by measuring the internal contaminations of the purified zinc with a high-purity germanium detector at the Laboratori Nazionali del Gran Sasso. The total activity of cosmogenic activated nuclides is measured at the level of a few mBq/kg, as well as limits on naturally occurring radionuclides are set to less than mBq/kg. The excellent radiopurity of the zinc sample allows us to search for electron capture with positron emission and neutrinoless double electron capture of $^{64}$Zn, setting the currently most stringent lower limits on their half-lives, $T_{1/2}^{varepsilonbeta^+} > 2.7 times 10^{21}text{yr}$ (90% C.I.), and $T_{1/2}^{0 u2varepsilon}> 2.6 times 10^{21}text{yr}$ (90% C.I.), respectively.
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