新闻动态

光照表层水体中羟基自由基驱动的甲烷生成过程

作者:Wang, J., Wu, B., Yao, Y., Chen, B., Peng, S. & Chu, C.

Methane (CH4) production is commonly associated with anaerobic microbial respiration, yet substantial CH4 production has been observed in aerobic surface waters, presenting the "aerobic methane paradox". Clarifying the mechanism behind aerobic CH4 production is essential for refining the global CH4 budget. Here, we demonstrate that sunlight-driven photochemical processes can effectively produce CH4 across various surface waters, including river, lake, and seawater. The CH4 formation rates ranged from 0.4 +/- 0.1 to 0.7 +/- 0.1 mu mol/m2/h in the daytime, which were 2.3- to 3.9-fold higher as compared to those driven by the decomposition of organic matter by methanogenic archaea in the nighttime. Such aerobic CH4 production stems from the rapid oxidation of naturally abundant methyl donors (e.g., dimethyl sulfoxide) by a photochemically produced hydroxyl radical (center dot OH), which yields a methyl radical (center dot CH3) and subsequently leads to CH4 production. Simulations on CH4 productions across varying seasons, latitudes, altitudes, and regions at the global scale suggest that the photochemical processes contribute to 35.3-70.7% of marine CH4 emissions. Our study highlights a ubiquitous yet previously overlooked photochemical source of CH4 production in surface waters, shedding light on the "aerobic methane paradox", which has implications on the global CH4 budget.

甲烷(CH₄)生成通常与厌氧微生物呼吸相关联,然而在好氧表层水体中已观测到可观的CH₄生成,即所谓“好氧甲烷悖论”(aerobic methane paradox)。阐明好氧CH₄生成的机制对于精化全球CH₄收支至关重要。研究证明,太阳光驱动的光化学过程可在河流、湖泊、海水等多种表层水体中有效生成CH₄。白天光化学CH₄生成速率为0.4 ± 0.1 至 0.7 ± 0.1 μmol·m⁻²·h⁻¹,比夜间由产甲烷古菌分解有机物驱动的生成速率高2.3-3.9倍。这种好氧CH₄生成源于天然丰度较高的甲基供体(如二甲基亚砜,DMSO)被光化学产生的羟基自由基(·OH)快速氧化:该反应先生成甲基自由基(·CH₃),进而生成CH₄。对全球不同季节、纬度、海拔与区域CH₄生成的模拟表明,光化学过程贡献了海洋CH₄排放的35.3%-70.7%。研究揭示了一个普遍存在却长期被忽视的表层水体CH₄生成的光化学来源,为“好氧甲烷悖论”提供了解释,并对全球CH₄收支具有重要意义。

(来源:Environmental Science & Technology 2026 Issue 22  DOI: 10.1021/acs.est.6c02525)