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在无水条件下,纯 N2O 对生物炭和其他有机及无机材料的吸附。

Sorption of pure N2O to biochars and other organic and inorganic materials under anhydrous conditions.

机构信息

U.S. Geological Survey , Denver, Colorado 80225, USA.

出版信息

Environ Sci Technol. 2013 Jul 16;47(14):7704-12. doi: 10.1021/es400676q. Epub 2013 Jun 28.

Abstract

Suppression of nitrous oxide (N2O) emissions from soil is commonly observed after amendment with biochar. The mechanisms accounting for this suppression are not yet understood. One possible contributing mechanism is N2O sorption to biochar. The sorption of N2O and carbon dioxide (CO2) to four biochars was measured in an anhydrous system with pure N2O. The biochar data were compared to those for two activated carbons and other components potentially present in soils-uncharred pine wood and peat-and five inorganic metal oxides with variable surface areas. Langmuir maximum sorption capacities (Qmax) for N2O on the pine wood biochars (generated between 250 and 500 °C) and activated carbons were 17-73 cm(3) g(-1) at 20 °C (median 51 cm(3) g(-1)), with Langmuir affinities (b) of 2-5 atm(-1) (median 3.4 atm(-1)). Both Qmax and b of the charred materials were substantially higher than those for peat, uncharred wood, and metal oxides [Qmax 1-34 cm(3) g(-1) (median 7 cm(3) g(-1)); b 0.4-1.7 atm(-1) (median 0.7 atm(-1))]. This indicates that biochar can bind N2O more strongly than both mineral and organic soil materials. Qmax and b for CO2 were comparable to those for N2O. Modeled sorption coefficients obtained with an independent polyparameter-linear free-energy relationship matched measured data within a factor 2 for mineral surfaces but underestimated by a factor of 5-24 for biochar and carbonaceous surfaces. Isosteric enthalpies of sorption of N2O were mostly between -20 and -30 kJ mol(-1), slightly more exothermic than enthalpies of condensation (-16.1 kJ mol(-1)). Qmax of N2O on biochar (50000-130000 μg g(-1) biochar at 20 °C) exceeded the N2O emission suppressions observed in the literature (range 0.5-960 μg g(-1) biochar; median 16 μg g(-1)) by several orders of magnitude. Thus, the hypothesis could not be falsified that sorption of N2O to biochar is a mechanism of N2O emission suppression.

摘要

土壤中添加生物炭通常会抑制一氧化二氮(N2O)的排放。但目前还不清楚这种抑制作用的机制。一种可能的作用机制是 N2O 被生物炭吸附。本研究采用无水体系和纯 N2O 测量了 4 种生物炭对 N2O 和二氧化碳(CO2)的吸附。将生物炭数据与 2 种活性炭和其他可能存在于土壤中的成分(未碳化的松木和泥炭)以及 5 种表面积不同的无机金属氧化物进行了比较。20°C 时,来源于 250-500°C 的木屑生物炭和活性炭对 N2O 的朗缪尔最大吸附容量(Qmax)分别为 17-73cm3g-1(中位数 51cm3g-1),朗缪尔亲和力(b)分别为 2-5atm-1(中位数 3.4atm-1)。碳化材料的 Qmax 和 b 均明显高于泥炭、未碳化木材和金属氧化物[Qmax 为 1-34cm3g-1(中位数 7cm3g-1);b 为 0.4-1.7atm-1(中位数 0.7atm-1)]。这表明生物炭对 N2O 的吸附能力强于矿物质和有机土壤物质。CO2 的 Qmax 和 b 与 N2O 相当。利用独立的多参数线性自由能关系模型获得的吸附系数与矿物表面的实测数据相差 2 倍以内,但与生物炭和含碳表面的实测数据相差 5-24 倍。N2O 的等吸附焓主要在-20 到-30kJmol-1之间,比冷凝焓(-16.1kJmol-1)略为放热。20°C 时,生物炭对 N2O 的 Qmax(50000-130000μg g-1 生物炭)比文献中观察到的 N2O 排放抑制(0.5-960μg g-1 生物炭;中位数 16μg g-1)高出几个数量级。因此,不能否定 N2O 被生物炭吸附是 N2O 排放抑制的机制这一假说。

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