Double-edged sword effect of seawater in CH4 photo-oxidation to CH3OOH: Boosting C–H activation while reducing peroxidation

IF 6.5 1区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Catalysis Pub Date : 2025-06-19 DOI:10.1016/j.jcat.2025.116291

Weixin Li, Wenhao Zhou, Yufei Cui, Hui Yang, Yongqing Ma, Ganhong Zheng, Chuhong Zhu, Meiling Wang

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引用次数: 0

Abstract

Realizing methane (CH₄) direct converting to value-added liquid products with high selectivity still confronts huge challenges, particularly expensive catalyst costs and inferior catalyst stability. In this work, 0.6 M NaCl was firstly tentatively investigated for CH₄ conversion with presence of H₂O₂. Then renewable, scalable and economic seawater from the Yellow Sea is directly used for catalyzing CH₄ conversion to CH₃OOH, and it was found that seawater increased CH₃OOH production by fivefold (from 4.7–23.8 μmol h⁻¹), while reduced CO₂ production by four-fifths (from 37.0 %–7.4 %) during 8 h, demonstrating the double-edged sword effect of seawater: boosting C Abstract Image

H activation and reducing peroxidation. In addition, no performance degradation is observed at all during 8 h reaction, proving the good stability of seawater as catalyst for CH₄ conversion. Mechanism investigation indicates that in situ formed HOOCl play key roles in CH₄ activation and further conversion to CH₃OOH. This study highlights the effectiveness of seawater in energy conversion, which would bring huge economic benefits for the sustainable development and utilization of marine CH₄.

Abstract Image

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海水在CH4光氧化生成CH3OOH过程中的双刃剑效应：在促进C-H活化的同时减少过氧化作用

实现甲烷（CH4）直接转化为高选择性增值液体产品仍面临巨大挑战，特别是催化剂成本昂贵，催化剂稳定性差。本文首次初步研究了0.6 M NaCl在H2O2存在下对CH4的转化作用。结果表明，在8 h内，海水使CH4的产率提高了5倍（从4.7 μmol - 23.8 μmol h−1），同时使CO2的产率降低了5分之4（从37.0 % -7.4 %），显示了海水的双刃剑效应：促进CH活化和减少过氧化作用。此外，在8 h反应过程中没有观察到任何性能下降，证明了海水作为CH4转化催化剂的良好稳定性。机理研究表明，原位形成的HOOCl在CH4活化和进一步转化为CH3OOH中起关键作用。本研究凸显了海水能量转化的有效性，将为海洋CH4的可持续开发利用带来巨大的经济效益。

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来源期刊

Journal of Catalysis 工程技术-工程：化工

CiteScore

12.30

自引率

5.50%

发文量

447

审稿时长

31 days

期刊介绍： The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.