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<p>H<sub>2</sub>S capture and valorization from polluted natural gas offer environmental and resource recovery benefits, but current approaches produce moderate-value sulfur with intensive carbon footprint. Herein, we develop an electrochemical deep oxidation method that converts H<sub>2</sub>S from polluted natural gas into value-added K<sub>2</sub>SO<sub>4</sub> using in-situ cathodically generated H<sub>2</sub>O<sub>2</sub>. We first validate this concept using commercial H<sub>2</sub>O<sub>2</sub> and then in-situ generated H<sub>2</sub>O<sub>2</sub> in H-cell, revealing the importance of high H<sub>2</sub>O<sub>2</sub> concentration for deep H<sub>2</sub>S oxidation, especially sluggish S<sub>2</sub>O<sub>3</sub><sup>2−</sup>-to-SO<sub>3</sub><sup>2−</sup> conversion. We then showcase its application potential in 4-cm<sup>2</sup> and then 100-cm<sup>2</sup> flow reactor with high interfacial H<sub>2</sub>O<sub>2</sub> concentration and large current, with the latter achieving H<sub>2</sub>S removal (100,000 ppm to &lt;15 ppm), &gt;70% K<sub>2</sub>SO<sub>4</sub> selectivity, and 100-h stable operation. Life-cycle assessment and techno-economic analysis confirm the strategy’s sustainability advantages and economic viability. We finally extend this method to produce a 1.4 wt% H<sub>2</sub>SO<sub>4</sub> solution by modifying the flow reactor with a solid-electrolyte type.</p>

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Electrochemical valorization of H2S in natural gas to sulfate under mild conditions

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2025年8月4日

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  • Chunyu Zhang,
  • An-Zhen Li,
  • Bo-Jun Yuan,
  • Xiang Liu,
  • Yuanbo Liu,
  • Kejian Kong,
  • Qiujin Shi,
  • Yixuan Zhang,
  • Yiqi Luo,
  • Shengnan Li,
  • Hua Zhou,
  • Haohong Duan

摘要

H2S capture and valorization from polluted natural gas offer environmental and resource recovery benefits, but current approaches produce moderate-value sulfur with intensive carbon footprint. Herein, we develop an electrochemical deep oxidation method that converts H2S from polluted natural gas into value-added K2SO4 using in-situ cathodically generated H2O2. We first validate this concept using commercial H2O2 and then in-situ generated H2O2 in H-cell, revealing the importance of high H2O2 concentration for deep H2S oxidation, especially sluggish S2O32−-to-SO32− conversion. We then showcase its application potential in 4-cm2 and then 100-cm2 flow reactor with high interfacial H2O2 concentration and large current, with the latter achieving H2S removal (100,000 ppm to <15 ppm), >70% K2SO4 selectivity, and 100-h stable operation. Life-cycle assessment and techno-economic analysis confirm the strategy’s sustainability advantages and economic viability. We finally extend this method to produce a 1.4 wt% H2SO4 solution by modifying the flow reactor with a solid-electrolyte type.