利用不同环境和实验中FT-ICR MS数据的综合,推进有机物化学稳定性评估

IF 2.6 3区 地球科学 Q2 GEOCHEMISTRY & GEOPHYSICS Organic Geochemistry Pub Date : 2023-10-01 DOI:10.1016/j.orggeochem.2023.104667
Juliana D'Andrilli , Carlos M. Romero , Phoebe Zito , David C. Podgorski , Robert A. Payn , Stephen D. Sebestyen , Andrew R. Zimmerman , Fernando L. Rosario-Ortiz
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引用次数: 1

摘要

傅里叶变换离子回旋共振质谱(FT-ICR MS)数据中的模式提供了有机物质(OM)特征如何由自然过程形成的视角。在这里,我们重新评估和更新了分子不稳定性边界(MLB)方法,利用FT-ICR质谱数据的合成来评估OM的不稳定性。现在包括美国各地淡水、植物凋落物和生物炭渗滤液、土壤和油的MLBL(生物性)指数(即氢碳比≥1.5的OM比例)、OM和溶解OM (DOM)不稳定性的趋势,这些趋势来自实验室实验,研究分离的微生物、光化学和热降解,以及受人类活动(例如肥料添加和农业管理)影响的生态系统的生物性模式的生物地球化学解释。光处理提高了OM的氢饱和度,描述了更高的生物活性(>MLBL值)。DOM MLBL值在微生物和热降解过程中下降。分离处理的实验室实验显示,MLBL的变化比人类管理系统的现场样本所显示的更大。我们将MLB上方含N和/或s的DOM的变化解释为异质生物相容性材料的生产或使用。我们解释了异质性不稳定DOM组成,以表明在河流和土壤样品中的本地生产,生物量增长,养分积累或生物降解。我们合成的最新数据表明,MLB方法应该重新构建,以提供生物、热和光化学过程的不稳定性指标。对稳定性的更广泛的看法提供了一种有用的工具,可以将大型、复杂和流程驱动的DOM数据分解为更简单、信息更丰富的生态系统形式和功能趋势指示器。
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Advancing chemical lability assessments of organic matter using a synthesis of FT-ICR MS data across diverse environments and experiments

Patterns in Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) data provide perspective on how organic matter (OM) character is shaped by natural processes. Here, we reevaluate and update the molecular lability boundary (MLB) approach to assess OM lability using a synthesis of FT-ICR MS data. Now included are MLBL (biolability) indices (i.e., the OM proportion of hydrogen-to-carbon ratios ≥ 1.5) of freshwaters, plant litter and biochar leachates, soils, and oils across the US, trends in OM and dissolved OM (DOM) lability from laboratory experiments examining isolated microbial, photochemical, and thermal degradation, and biogeochemical interpretations of biolability patterns across ecosystems influenced by human activity (e.g., fertilizer addition and agricultural management). Photo-processing increased the hydrogen saturation of OM, describing products of higher biolability (>MLBL values). DOM MLBL values decreased during microbial and thermal degradation processes. Laboratory experiments with isolated treatments showed larger changes in MLBL than exhibited by field samples from systems managed by humans. We interpret changes in N- and/or S-containing DOM above the MLB as the production or use of heterogeneously biolabile material. We interpret heterogeneously labile DOM composition to indicate autochthonous production, biomass growth, nutrient accumulation, or biological degradation in stream and soil samples. The most recent data in our synthesis suggest that the MLB approach should be reframed to provide lability indices for biotic, thermal, and photochemical processes. A broader perspective on lability provides a useful tool to decompose large, complex, and process-driven DOM data into more simple and informative indicators of trends in ecosystem form and function.

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来源期刊
Organic Geochemistry
Organic Geochemistry 地学-地球化学与地球物理
CiteScore
5.50
自引率
6.70%
发文量
100
审稿时长
61 days
期刊介绍: Organic Geochemistry serves as the only dedicated medium for the publication of peer-reviewed research on all phases of geochemistry in which organic compounds play a major role. The Editors welcome contributions covering a wide spectrum of subjects in the geosciences broadly based on organic chemistry (including molecular and isotopic geochemistry), and involving geology, biogeochemistry, environmental geochemistry, chemical oceanography and hydrology. The scope of the journal includes research involving petroleum (including natural gas), coal, organic matter in the aqueous environment and recent sediments, organic-rich rocks and soils and the role of organics in the geochemical cycling of the elements. Sedimentological, paleontological and organic petrographic studies will also be considered for publication, provided that they are geochemically oriented. Papers cover the full range of research activities in organic geochemistry, and include comprehensive review articles, technical communications, discussion/reply correspondence and short technical notes. Peer-reviews organised through three Chief Editors and a staff of Associate Editors, are conducted by well known, respected scientists from academia, government and industry. The journal also publishes reviews of books, announcements of important conferences and meetings and other matters of direct interest to the organic geochemical community.
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