Zhang Chunyu, Li An-Zhen, Yuan Bo-Jun, Liu Xiang, Liu Yuanbo, Kong Kejian, Shi Qiujin, Zhang Yixuan, Luo Yiqi, Li Shengnan, Zhou Hua, Duan Haohong
Department of Chemistry, Tsinghua University, Beijing, China.
Haihe Laboratory of Sustainable Chemical Transformations, Tianjin, China.
Nat Commun. 2025 Aug 4;16(1):7175. doi: 10.1038/s41467-025-62445-y.
HS 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 HS from polluted natural gas into value-added KSO using in-situ cathodically generated HO. We first validate this concept using commercial HO and then in-situ generated HO in H-cell, revealing the importance of high HO concentration for deep HS oxidation, especially sluggish SO-to-SO conversion. We then showcase its application potential in 4-cm and then 100-cm flow reactor with high interfacial HO concentration and large current, with the latter achieving HS removal (100,000 ppm to <15 ppm), >70% KSO 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% HSO solution by modifying the flow reactor with a solid-electrolyte type.
从污染天然气中捕获并利用硫化氢具有环境和资源回收效益，但目前的方法产生的中等价值硫磺碳足迹较大。在此，我们开发了一种电化学深度氧化方法，该方法利用原位阴极产生的羟基自由基将污染天然气中的硫化氢转化为增值硫酸钾。我们首先使用商业羟基自由基验证了这一概念，然后在H型电解池中使用原位产生的羟基自由基，揭示了高浓度羟基自由基对于深度氧化硫化氢的重要性，尤其是对于缓慢的亚硫酸根到硫酸根的转化。然后，我们展示了其在4厘米和100厘米流动反应器中的应用潜力，反应器具有高界面羟基自由基浓度和大电流，后者实现了硫化氢去除（从100,000 ppm降至<15 ppm）、>70%的硫酸钾选择性以及100小时的稳定运行。生命周期评估和技术经济分析证实了该策略的可持续性优势和经济可行性。我们最终通过用固体电解质类型改造流动反应器，扩展了该方法以生产1.4 wt%的硫酸溶液。
