Yuan Hezhong, Guan Tong, Wang Yu, Yuan Qianhui, Liu Enfeng, Zeng Qingfei
Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control and Collaborative Innovation Center of Atmospheric Environment and Equipment Technology (CICAEET), School of Environmental Science and Engineering, Nanjing University of Information Science and Technology, Nanjing 210044, China.
Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control and Collaborative Innovation Center of Atmospheric Environment and Equipment Technology (CICAEET), School of Environmental Science and Engineering, Nanjing University of Information Science and Technology, Nanjing 210044, China.
Water Res. 2025 Sep 1;283:123871. doi: 10.1016/j.watres.2025.123871. Epub 2025 May 20.
Stable organic carbon (OC) burial into lacustrine sediments was the important C fixation path for atmospheric C reduction. However, OC retention effect and stability mechanisms in sediments was still unclear at the molecular scale during the burial period. Chronology and OC fractions were measured for the sediments from two freshwater lakes. Three-dimensional fluorescence and Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) were used to detect the change in the forms and molecular structure of soluble OC (SOC). Remarkably increasing TOC and total nitrogen (TN) concentrations along with the decreasing TOC/TN (C/N) values upwards occurred in the sediment columns indicated the weakened terrigenous OC and N inputs from about the 1980s. The OC mineralization contributed to the decrease of C burial in deeper sedimentary layers. However, higher SOC concentrations was found in deeper depths, suggesting that SOC facilitated the OC accumulation and fixation in the sediments and triggered the higher OCBR values over time. Additionally, obvious fluorescence intensity existence throughout the the whole sediment cores suggested the synchronous accumulation of both humic acid-like and fulvic acid-like materials over time as dominant SOC fractions. Higher fluorescence intensity at upper sediment layers indicated the SOC burial as humic acid-like materials with stronger sequestration potential. The persistence of fluorescence signal suggested that fulvic acid-like materials dominated the SOC immobilization and resistance to mineralization in the sediments. Finally, FT-ICR-MS analysis showed that remarkable accumulation of lipids with abundances from 31 to 44 % of organics was attributed to the decomposition of lignins and dominated CHO and CHON formulas and OC compounds. Lipids and lignins with higher abundances dominated the SOC burial and fixation over time even though mineralization occurred. Our work testified that lipids and lignins contributed to the majority of humic acid-like materials and subsequent OC retention in the lacustrine sediments at the geological time scale.
稳定有机碳(OC)埋藏于湖相沉积物中是大气碳减排的重要碳固定途径。然而,在埋藏期间,沉积物中OC的保留效应和稳定性机制在分子尺度上仍不清楚。对两个淡水湖的沉积物进行了年代测定和OC组分分析。利用三维荧光和傅里叶变换离子回旋共振质谱(FT-ICR-MS)检测可溶性OC(SOC)的形态和分子结构变化。沉积物柱中TOC和总氮(TN)浓度显著增加,同时TOC/TN(C/N)值向上降低,表明自20世纪80年代左右以来陆源OC和N输入减弱。OC矿化导致深层沉积层中碳埋藏量减少。然而,在更深的深度发现了更高的SOC浓度,这表明SOC促进了沉积物中OC的积累和固定,并随着时间的推移引发了更高的OCBR值。此外,整个沉积物岩芯中都存在明显的荧光强度,这表明随着时间的推移,腐殖酸类和富里酸类物质作为主要的SOC组分同步积累。上部沉积层较高的荧光强度表明SOC以具有更强固存潜力的腐殖酸类物质形式埋藏。荧光信号的持续存在表明富里酸类物质主导了沉积物中SOC的固定和抗矿化作用。最后,FT-ICR-MS分析表明,脂质的显著积累(占有机物的31%至44%)归因于木质素的分解,且主要为CHO和CHON分子式及OC化合物。随着时间的推移,即使发生了矿化作用,较高丰度的脂质和木质素仍主导着SOC的埋藏和固定。我们的研究证明,在地质时间尺度上,脂质和木质素是湖相沉积物中大部分腐殖酸类物质及随后OC保留的主要贡献者。