Key Laboratory of Surficial Geochemistry, Ministry of Education, School of Earth Sciences and Engineering, Nanjing University, Nanjing 210023, China;
Division of Geological and Planetary Sciences, California Institute of Technology, Pasadena, CA 91125.
Proc Natl Acad Sci U S A. 2021 May 25;118(21). doi: 10.1073/pnas.1921544118.
Fly ash-the residuum of coal burning-contains a considerable amount of fossilized particulate organic carbon (FOC) that remains after high-temperature combustion. Fly ash leaks into natural environments and participates in the contemporary carbon cycle, but its reactivity and flux remained poorly understood. We characterized FOC in the Chang Jiang (Yangtze River) basin, China, and quantified the riverine FOC fluxes. Using Raman spectral analysis, ramped pyrolysis oxidation, and chemical oxidation, we found that FOC is highly recalcitrant and unreactive, whereas shale-derived FOC (FOC) was much more labile and easily oxidized. By combining mass balance calculations and other estimates of fly ash input to rivers, we estimated that the flux of FOC carried by the Chang Jiang was 0.21 to 0.42 Mt C⋅y in 2007 to 2008-an amount equivalent to 37 to 72% of the total riverine FOC export. We attributed such high flux to the combination of increasing coal combustion that enhances FOC production and the massive construction of dams in the basin that reduces the flux of FOC eroded from upstream mountainous areas. Using global ash data, a first-order estimate suggests that FOC makes up to 16% of the present-day global riverine FOC flux to the oceans. This reflects a substantial impact of anthropogenic activities on the fluxes and burial of fossil organic carbon that has been made less reactive than the rocks from which it was derived.
粉煤灰——煤燃烧的残余物——在高温燃烧后含有相当数量的已碳化的颗粒有机碳(FOC)。粉煤灰泄漏到自然环境中并参与当代碳循环,但它的反应性和通量仍知之甚少。我们对中国长江流域的 FOC 进行了特征描述,并量化了河流 FOC 通量。通过拉曼光谱分析、斜坡热解氧化和化学氧化,我们发现 FOC 具有高度的稳定性和不反应性,而页岩衍生的 FOC(FOC)则更不稳定,容易氧化。通过结合质量平衡计算和其他对输入河流的粉煤灰的估计,我们估计 2007 年至 2008 年,长江携带的 FOC 通量为 0.21 至 0.42 Mt C·y-这一数量相当于总河流 FOC 输出的 37%至 72%。我们将如此高的通量归因于以下两个因素的结合:煤炭燃烧的增加,这增加了 FOC 的产量;以及流域内大量大坝的建设,减少了从上游山区侵蚀的 FOC 通量。利用全球灰分数据,初步估计 FOC 占当今全球河流向海洋输送的 FOC 通量的 16%。这反映了人为活动对通量和埋藏化石有机碳的巨大影响,使其比其来源岩石的反应性降低。