Nonequilibrium sorption of organic chemicals: elucidation of rate-limiting processes

Brusseau, Mark L.; Jessup, R. E.; Rao, P. Suresh C.

doi:10.1021/es00013a015

Cited by 428 publications

(281 citation statements)

References 32 publications

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“…We hypothesized that some of the retardation could have resulted from steric effects. Brusseau et al claimed the size of the ''pores'' associated with organic matter is similar to the geometrical parameters of the sorbate molecules [35]. The lower desorption reversibility of chrysene than phenanthrene in DHS may also serve as the evidence to support our suspicion of steric hindrance influence on desorption.…”

Section: Effects Of Aging and Chemical Property On Desorptionsupporting

confidence: 59%

“…As the sorbate becomes diluted, segmental flexibility of solid decreases. These processes are only partly reversible and sorbate molecules are entrapped in the sorbent consequently [12,35]. It was found that physical reorientation of sorption domains can produce contacttime-dependent changes in the phase-distribution behaviors of organic solutes in soil organic matter [3].…”

Section: Possible Mechanisms Contributing To Desorption Resistancementioning

confidence: 99%

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Aging effects on sorption–desorption behaviors of PAHs in different natural organic matters

Wang

Chen

et al. 2012

Journal of Colloid and Interface Science

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a b s t r a c tThe aging effects of sorption-desorption of two polycyclic aromatic hydrocarbons (PAHs), that is, phenanthrene and chrysene on different natural organic matters (NOMs), that is, humic acid, fulvic acid, and humins of different sources were studied. Both organic carbon-normalized distribution coefficients (K oc ) and the reversible desorption fractions (f rd ) were evaluated. Results showed that aging effects were both sorbent and sorbate specific. With increasing aging duration, K oc s of phenanthrene on humins increased, whereas K oc s of chrysene did not change significantly. Significant f rd declinations over aging times were observed for all the NOMs, which demonstrated the effects of aging on availability of PAHs. Furthermore, the f rd was not only positively correlated with the atomic O/C ratio of NOMs, which represent the geological maturity of NOMs, but also varied with the property of sorbates. We conclude that aging effects of HOCs on NOMs should be a case-specific process and the desorption reversibility depends on the structure and characteristics of both NOMs and sorbates.

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Section: Effects Of Aging and Chemical Property On Desorptionsupporting

confidence: 59%

Section: Possible Mechanisms Contributing To Desorption Resistancementioning

confidence: 99%

Aging effects on sorption–desorption behaviors of PAHs in different natural organic matters

Wang

Chen

et al. 2012

Journal of Colloid and Interface Science

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“…Diversos trabalhos revelaram que algumas reações são tempodependentes (Karickhoff, 1980;Karickhoff & Morris, 1985;Pignatello, 1989), e a ausência de equilíbrio seria causada por diferentes processos de adsorção e difusão da molécula com a fase sólida do solo. O processo de difusão tem sido classificado como: filme difusão, retardamento por difusão intrapartícula e difusão intraorgânica (Brusseau et al, 1991). Estudando a adsorção de simazina em colunas de solo saturado, Fortin et al (1997) observaram que o decaimento na curva BTC após interrupção da lixiviação foi atribuído à difusão intraorgânica.…”

Section: Resultsunclassified

Avaliação do transporte de atrazina em solos sob diferentes condições de manejo agrícola

Correia

Langenbach

Campos

2010

Rev. Bras. Ciênc. Solo

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RESUMOA pouca informação sobre o movimento de pesticidas em solos brasileiros com manejo de plantio direto torna o conhecimento desse assunto de grande relevância na avaliação de risco de contaminação do solo e de lençóis de água. Os experimentos simularam chuvas intensas com fluxo contínuo por meio de uma nova técnica para a determinação simultânea das propriedades de advecção, difusão e sorção, representando o transporte de contaminantes ao longo do perfil de solo estudado. Os resultados mostraram que as propriedades físico-químicas não se correlacionam com a permeabilidade do solo e a lixiviação da atrazina. A condutividade 10 vezes maior no plantio direto (PD) e sistema natural (SN) do que no sistema convencional (SC) e solo subsuperficial (SUB) sugere que o processo de advecção ocorre predominantemente através dos macroporos por fluxo preferencial, que são destruídos na aração do SC. Dessa forma, a condição de fluxo contínuo, representando fortes chuvas, faz com que a lixiviação em PD seja maior que em SC, contrariando dados da literatura em experimentos de campo com chuvas intermitentes, os quais mostraram menor lixiviação em PD comparado ao SC. Os riscos de contaminação dos lençóis de água não são determinados apenas pelo manejo do solo, mas também pelas condições pluviométricas intensas nos trópicos, com perspectivas de ainda serem maiores nos cenários de mudanças climáticas.Termos de indexação: pesticidas, contaminação, plantio direto.(1) Recebido para publicação em janeiro de 2009 e aprovado em dezembro de 2009.

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“…All but one of these models requires at least two (mathematical) compartments to fit the experimental data. These compartments can then define a combination of an instantaneous compartment where no mass transfer limitation is assumed with a dynamic compartment where mass transfer is limited (Ball and Roberts 1991;Sabbah et al 2005), two dynamic compartments (Brusseau et al 1991;Weber et al 1992;Xing and Pignatello 1996;Cornelissen et al 1998;Ghosh et al 2000;Shor et al 2003;Gamst et al 2004) or a continuum of compartments with various parameters (Culver et al 1997;Werth et al 2000;Werth and Hansen 2002). Although sometimes excellent fits of experimental and modeled data were demonstrated in the different papers, the physical explanation of the desorption process and its limitations is only briefly elaborated and do not include the effect of particle-size distribution.…”

Section: Introductionmentioning

confidence: 99%

“…For example, Freundlich sorption isotherms (Miller and Pedit 1992;Lin et al 1994;Rugner et al 1999;Braida et al 2001;Gamst et al 2004) or linear sorption isotherm (Wu and Gschwend 1986;Steinberg et al 1987;Rijnaarts et al 1990;Ball and Roberts 1991;Brusseau et al 1991;Pignatello et al 1993;Pedit and Miller 1994;Li and Werth 2004) were used to model desorption kinetics. In radial diffusion models, particle-size effects are generally lumped into a single-fit-parameter D a /R 2 , where D a is a diffusion coefficient and R the radius of the spheres.…”

Section: Introductionmentioning

confidence: 99%

Modeling desorption kinetics of a persistent organic pollutant from field aged sediment using a bi-disperse particle size distribution

et al. 2009

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Purpose With the predicted climate change, it is expected that the chances of river flooding increase. During flood events, sediments will resuspend and when sediments are polluted, contaminants can be transferred to the surrounding water. In this paper we discuss a numerical intraparticle diffusion model that simulates desorption of dieldrin from a suspension of contaminated porous sediment particles with a well-characterized particle size distribution. The objective of this study was to understand the desorption rate (flux) of dieldrin from a suspension of field-aged sediment at different hydraulic retention times (HRT) of the aqueous phase and to elaborate the effect of particle-size distribution on mass transfer. Materials and methods Desorption kinetics of dieldrin, a persistent organic pollutant (POP), were experimentally measured and described in a separate paper using fieldcontaminated sediment. A radial diffusion model, accommodating intraparticle reversible sorption kinetics, aqueous phase pore diffusion, and a sink term for bulk aqueous phase refreshment was used to describe the experimental data. Results and discussion We observed rapid equilibrium of contaminants between small particles (10 μm) and the surrounding water even though the sorption affinity of dieldrin towards organic matter was high. On the contrary, for the larger particles (84 μm), calculations show that desorption was limited by intraparticle diffusion. Combining small and larger particles in our radial diffusion model resulted in the biphasic desorption behavior often observed even when using a linear isotherm. Conclusions Flood events will result in an increase of desorption rate of POPs from sediments to the surrounding water. HRT and the particle-size distribution determine the desorption rate. We conclude that nonstationary diffusion within organic matter is the main process of mass transfer. Particle size distributions are very valuable to understand the phenomenology related to mass transfer limitations often described as limited bioavailability and can be used as basis to develop engineering options to limit contaminant mass fluxes into the environment.

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Nonequilibrium sorption of organic chemicals: elucidation of rate-limiting processes

Cited by 428 publications

References 32 publications

Aging effects on sorption–desorption behaviors of PAHs in different natural organic matters

Aging effects on sorption–desorption behaviors of PAHs in different natural organic matters

Avaliação do transporte de atrazina em solos sob diferentes condições de manejo agrícola

Modeling desorption kinetics of a persistent organic pollutant from field aged sediment using a bi-disperse particle size distribution

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