Efficient electrocatalytic desulfuration and synchronous hydrogen evolution from H2S via anti-sulfuretted NiSe nanowire array catalyst
Efficient electrocatalytic desulfuration and synchronous hydrogen evolution from H2S via anti-sulfuretted NiSe nanowire array catalyst
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DOI：
10.1016/j.apcatb.2022.122255
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发表时间：
2023
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影响因子：
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通讯作者：
Chao Duan;Chun Tang;Shan Yu;Lina Li;Jinjin Li;Ying Zhou
中科院分区：
文献类型：
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作者：
Chao Duan;Chun Tang;Shan Yu;Lina Li;Jinjin Li;Ying Zhou
用更容易发生的硫化物氧化反应（SOR）取代析氧反应（OER）来生成析氢和硫的增值产物，从而降低水分解策略的能耗是一项很有前途的技术。然而，不理想的催化剂长期稳定性和钝化问题极大地限制了整体生产力。在此，我们报道了一种抗硫化NiSe纳米线阵列催化剂（NiSe/NF），该催化剂的阳极电位显著降低了0.49 Vvs。在100 mA cm−2下的RHE与1.78 Vvs的析氧反应相比。RHE)并且在不钝化的情况下保持超过500小时的令人钦佩的稳定性。特别是，我们巧妙地结合了UV-vis，in - situRaman和衰减全反射傅立叶变换红外光谱，我们发现S2-/ hs被选择性地转化为sn2和副产物s2o32，而不是硫，这避免了长期困扰固体硫的钝化问题。我们首次在商用膜电极组件堆栈中证明了该系统（SOR + HER）的可行性，该系统在1.0 V的低电池电压下提供19.0 mL min - 1h2，消耗2.63 kWh Nm - 3H2的电力。本研究为H2S电氧化脱硫低成本制氢提供了一条新途径。
Decreasing energy consumption of water splitting strategy by replacing oxygen evolution reaction (OER) with more facile sulfide oxidation reaction (SOR) to H2evolution 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 Vvs.RHE at 100 mA cm−2compared to the oxygen evolution reaction (1.78 Vvs.RHE) and remains admirable stability for more than 500 h without passivation. Particularly, the skillful combination of UV–vis,in situRaman, 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−1H2at a low cell voltage of 1.0 V with consuming the electricity of 2.63 kWh Nm−3H2. This work provides a new avenue for low-cost H2production by H2S electrooxidation desulfurization.