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Hydrogen isotope separation by tunneling effect used graphene-based heterogeneous electrocatalysts in electrochemical hydrogen pumping

Yasuda, Satoshi   ; Matsushima, Hisayoshi*; Terasawa, Tomoo   ; Yano, Masahiro   ; Asaoka, Hidehito  ; Gueriba, J.*; Di$~n$o, W.*; Fukutani, Katsuyuki

We fabricated heterogeneous electrode with layered structures consisting of palladium and graphene layers and reported D2 enrichment from hydrogen and deuterium mixture gas using polymer electrolyte membrane electrochemical hydrogen pumping used the fabricated electrode. Mass spectroscopic analysis demonstrated significant bias voltage dependence of hydrogen/deuterium (H/D) separation ability and the H/D value decreases as the bias voltage increases. Theoretical analysis showed that the observed high H/D at low bias voltage stems from hydrogen isotopes tunneling through atomically-thick graphene during the electrochemical reaction, and the bias dependent H/D results in a transition from the quantum tunneling regime to classical over- barrier regime for hydrogen isotopes transfer via the graphene. These findings provide new insight for a novel economical methodology of efficient hydrogen isotope enrichment.

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