Constraining biorecalcitrance of carboxyl-rich alicyclic molecules in the ocean

IF 11.7 1区 综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES
Ruanhong Cai, Oliver J. Lechtenfeld, Zhenwei Yan, Yuanbi Yi, Xiaoxia Chen, Qiang Zheng, Boris P. Koch, Nianzhi Jiao, Ding He
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Abstract

Marine dissolved organic matter (DOM) is one of Earth’s largest long-term carbon reservoirs, critical to the global carbon cycle. A key breakthrough in understanding this pool is the identification of biorefractory carboxyl-rich alicyclic molecules (CRAM). Recent studies have challenged the biorecalcitrance of CRAM but lacked detailed molecular evidence. Using advanced online countergradient liquid chromatography–Fourier transform ion cyclotron resonance mass spectrometry to track microbial incubation, we revealed a wide spectrum of CRAM bioavailability regulated by molecular polarity. CRAM with lower polarity were preferentially degraded, whereas microbial reworking led to production of higher-polarity CRAM, characterized by increased oxidation state, nitrogen content, and aromaticity. Some microbially transformed CRAM were frequently detected in a global DOM dataset of 1485 seawater samples, suggesting their potential persistence in marine environments. This study provides molecular insights into the biorecalcitrance and transformation pathway of CRAM, underscoring the complexity and dynamic nature of marine organic carbon cycling.

Abstract Image

抑制海洋中富含羧基脂环分子的生物抗逆性
海洋溶解有机物(DOM)是地球上最大的长期碳库之一,对全球碳循环至关重要。了解这一群体的一个关键突破是鉴定出生物难降解的富羧基脂环分子(CRAM)。最近的研究对CRAM的生物顽固性提出了质疑,但缺乏详细的分子证据。利用先进的在线反梯度液相色谱-傅里叶变换离子回旋共振质谱法跟踪微生物培养,我们揭示了CRAM的生物利用度受分子极性调节的广谱谱。低极性的CRAM被优先降解,而微生物改造导致高极性的CRAM产生,其特征是氧化态、氮含量和芳香性增加。一些微生物转化的CRAM在1485个海水样本的全球DOM数据集中经常被检测到,这表明它们在海洋环境中可能存在。本研究为CRAM的生物顽抗和转化途径提供了分子视角,凸显了海洋有机碳循环的复杂性和动态性。
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来源期刊
Science Advances
Science Advances 综合性期刊-综合性期刊
CiteScore
21.40
自引率
1.50%
发文量
1937
审稿时长
29 weeks
期刊介绍: Science Advances, an open-access journal by AAAS, publishes impactful research in diverse scientific areas. It aims for fair, fast, and expert peer review, providing freely accessible research to readers. Led by distinguished scientists, the journal supports AAAS's mission by extending Science magazine's capacity to identify and promote significant advances. Evolving digital publishing technologies play a crucial role in advancing AAAS's global mission for science communication and benefitting humankind.
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