期刊名称：Proceedings of the National Academy of Sciences
印刷版ISSN：0027-8424
电子版ISSN：1091-6490
出版年度：2015
卷号：112
期号：11
页码：3247-3252
DOI：10.1073/pnas.1424728112
语种：English
出版社：The National Academy of Sciences of the United States of America
摘要：SignificanceHuman activities affect the water cycle in many ways, some of which remain difficult to measure. One such process is emission of water vapor through combustion of fossil fuels, which may be a significant part of the atmospheric water budget in urban centers. It has not previously been possible to uniquely identify combustion-derived water vapor with atmospheric measurements. We introduce a method for the measurement of combustion-derived vapor, and show that this source contributes as much as 13% of surface-level vapor in the atmosphere of one city. The new approach may help researchers monitor sources of greenhouse gas emissions from cities and study the impact of water of combustion on urban weather, quality of life, and atmospheric chemistry. Anthropogenic modification of the water cycle involves a diversity of processes, many of which have been studied intensively using models and observations. Effective tools for measuring the contribution and fate of combustion-derived water vapor in the atmosphere are lacking, however, and this flux has received relatively little attention. We provide theoretical estimates and a first set of measurements demonstrating that water of combustion is characterized by a distinctive combination of H and O isotope ratios. We show that during periods of relatively low humidity and/or atmospheric stagnation, this isotopic signature can be used to quantify the concentration of water of combustion in the atmospheric boundary layer over Salt Lake City. Combustion-derived vapor concentrations vary between periods of atmospheric stratification and mixing, both on multiday and diurnal timescales, and respond over periods of hours to variations in surface emissions. Our estimates suggest that up to 13% of the boundary layer vapor during the period of study was derived from combustion sources, and both the temporal pattern and magnitude of this contribution were closely reproduced by an independent atmospheric model forced with a fossil fuel emissions data product. Our findings suggest potential for water vapor isotope ratio measurements to be used in conjunction with other tracers to refine the apportionment of urban emissions, and imply that water vapor emissions associated with combustion may be a significant component of the water budget of the urban boundary layer, with potential implications for urban climate, ecohydrology, and photochemistry.
