Efficient electrocatalytic desulfuration and synchronous hydrogen evolution from H2S via anti-sulfuretted NiSe nanowire array catalyst

Decreasing energy consumption of water splitting strategy by replacing oxygen evolution reaction (OER) with more facile sulfide oxidation reaction (SOR) to H2 evolution and value-added sulfur products is a promising technology. Nevertheless, the unsatisfactory catalyst long-term stability and passivation issues substantially limit the overall productivity. Herein, we report an anti-sulfuretted NiSe nanowire array catalyst on nickel foam (NiSe/NF), this catalyst exhibits a significantly reduced anode potential of 0.49 V vs. RHE at 100 mA cm−2 compared to the oxygen evolution reaction (1.78 V vs. RHE) and remains admirable stability for more than 500 h without passivation. Particularly, the skillful combination of UV–vis, in situ Raman, and attenuated total reflection Fourier transform infrared spectra, we reveal that S2-/HS- has been selectively converted to Sn2- and by-product S2O32- rather than sulfur, which avoids long-perplexing passivation issue of solid sulfur. For the first time, we demonstrate the feasibility of the system (SOR + HER) in a commercial membrane electrode assembly stack, which affords 19.0 mL min−1 H2 at a low cell voltage of 1.0 V with consuming the electricity of 2.63 kWh Nm−3 H2. This work provides a new avenue for low-cost H2 production by H2S electrooxidation desulfurization.