| Resumo: | Some metals belonging to groups IV and V show a high permeability to hydrogen and have been studied as possible alternatives to palladium in membranes for hydrogen purification/separation in order to increase their sustainability and decrease their costs. However, to date, very few alloys among those metals have been investigated, and no membrane studies based on 4–5 element alloys with low or zero Pd content and quasi-amorphous structure have been reported so far. In this work, new membranes based on ZrVTi- and ZrVTiPd alloys were tested for the first time for this application. The unprecedented deposition of micrometric-based multilayers was performed via high-power impulse magnetron sputtering onto porous alumina substrates. Dense Pd/Zr<sub>x</sub>V<sub>y</sub>Ti<sub>z</sub>Pd<sub>w</sub>/Pd multilayers were obtained. The composition of the alloys, morphology and structure, hydrogen permeance, selectivity, and resistance to embrittlement were tested and analyzed depending on the deposition conditions, and the membrane with the enhanced performance was tuned. The environmental impact of these membranes was also investigated to ascertain the sustainability of these alloys relative to more common Pd<sub>77</sub>Ag<sub>23</sub> and V<sub>93</sub>Pd<sub>7</sub> thin-film membranes using a life cycle assessment analysis. The results showed that the partial substitution of Pd can efficiently lead to a decrease in the environmental impacts of the membranes.
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