Electrochemical valorization of H2S in natural gas to sulfate under mild conditions
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 <15 ppm), >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.
Authors
- An-Zhen Li (ORCID: https://orcid.org/0009-0005-6651-659X)
- Y. Liu (ORCID: https://orcid.org/0009-0005-8684-6211)
- Qiujin Shi
- Kejian Kong
- Hua Zhou (ORCID: https://orcid.org/0000-0002-7521-5837)
- Yiqi Luo (ORCID: https://orcid.org/0000-0002-4556-0218)
- Yi-Xuan Zhang (ORCID: https://orcid.org/0000-0003-4849-3660)
- Xiang Liu (ORCID: https://orcid.org/0009-0003-2233-7499)
- Chunyu Zhang (ORCID: https://orcid.org/0000-0002-5183-5337)
- Bo‐Jun Yuan
- Haohong Duan (ORCID: https://orcid.org/0000-0003-3210-0068)
- Shengnan Li
Institutions
- Quzhou University (CN)
- Tianjin haihe hospital (CN)
- Beijing University of Chemical Technology (CN)
- Tsinghua University (CN)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-08-04
- DOI
- https://doi.org/10.1038/s41467-025-62445-y
- Citations
- 3
- Primary Topic
- Industrial Gas Emission Control
- Type
- article
- Field-Weighted Citation Impact
- 2.14
Funders
- National Natural Science Foundation of China
- Tsinghua University