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Mo-based catalysts for CH4/H2S reforming to hydrogen production: effect of hydroxyl concentration of the support

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Abstract

High concentration of H2S in acidic natural gas will lead to poisoning of catalysts for hydrogen production by methane steam reforming, thus limiting the further use of natural gas. Reforming CH4 by H2S can be considered as an alternative route to hydrogen production from methane. This process not only achieves the removal of H2S but also obtains chemical raw material CS2 and clean energy H2. By impregnating the Mo source on SiO2 treated with hydrogen peroxide and then using the catalyst in the CH4/H2S reforming reaction, we surprisingly found that the conversion rate of CH4 and H2S increased from 28 and 32% to 34% and 43%, respectively, after hydrogen peroxide treatment. The H2 production rate and the yield of CS2 increased from 20 mmolH2/(gMo*min) and 52% to 30 mmolH2/(gMo*min) and 65%, respectively. Combining with characterization methods such as X-ray diffraction (XRD), hydrogen temperature programmed reduction (H2-TPR), 1H-based solid-state nuclear magnetic resonance (1H MAS NMR), X-ray photoelectron spectroscopy (XPS), Raman spectra (RS), and transmission electron microscopy (TEM), we found that the hydroxyl concentration of the support increased after hydrogen peroxide treatment, which led to the strengthening of the force between the metal and the support, which was easy to form low-level and small-size MoS2, exposing more active sites, and further improving the catalytic activity. This method provides a new idea for hydrogen production by CH4/H2S reforming and the development of high-performance MoS2-based catalysts.

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Funding

The authors wish to acknowledge the financial support provided by the National Natural Science Foundation of China (21968015, 22006059, 42030712, and 21966018), Excellent Youth Project of Natural Science Foundation of Yunnan Province (202201AW070007), Young Academic and Technical Leader Raising Foundation of Yunnan Province (202205AC160011), and Key Project of Natural Science Foundation of Yunnan Province (no. 202101AS070026).

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Authors and Affiliations

  1. Faculty of Chemical Engineering, Kunming University of Science and Technology, Kunming, 650500, People’s Republic of China

    Ke Li, Yuqiu Zhu, Zixuan Wang, Dingkai Chen, Yongming Luo & Dedong He

  2. The Innovation Team for Volatile Organic Compounds Pollutants Control and Resource Utilization of Yunnan Province, Kunming, 650500, People’s Republic of China

    Ke Li, Yuqiu Zhu, Zixuan Wang, Dingkai Chen, Yongming Luo & Dedong He

  3. The Higher Educational Key Laboratory for Odorous Volatile Organic Compounds Pollutants Control of Yunnan Province, Kunming, 650500, People’s Republic of China

    Ke Li, Yuqiu Zhu, Zixuan Wang, Dingkai Chen, Yongming Luo & Dedong He

  4. Yunnan Research Academy of Eco-environmental Sciences, Kunming, 650034, People’s Republic of China

    Wenwei Wu

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  1. Ke Li
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  2. Yuqiu Zhu
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Contributions

Ke Li: conceptualization, methodology, investigation, data curation, and writing. Yuqiu Zhu: visualization, software, and methodology. Zixuan Wang: visualization, resources, and validation. Dingkai Chen: conceptualization, data curation, project administration, and supervision. Wenwei Wu: formal analysis, data curation, review and editing, and supervision. Yongming Luo: conceptualization, resources, and funding acquisition. Dedong He: conceptualization, project administration, and funding acquisition.

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Correspondence to Dingkai Chen.

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Li, K., Zhu, Y., Wang, Z. et al. Mo-based catalysts for CH4/H2S reforming to hydrogen production: effect of hydroxyl concentration of the support. Environ Sci Pollut Res 30, 70884–70896 (2023). https://doi.org/10.1007/s11356-023-27222-8

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