[논문]Behaviors of Desorption Agents During Removal of Cs From Clay Minerals and Actual Soil

Park, Chan Woo; Kim, Ilgook; Yoon, In-Ho; Yang, Hee-Man; Seo, Bum-Kyung

doi:10.7733/jnfcwt.2021.19.1.39

Behaviors of Desorption Agents During Removal of Cs From Clay Minerals and Actual Soil 원문보기

Journal of nuclear fuel cycle and waste technology = 방사성폐기물학회지, v.19 no.1, 2021년, pp.39 - 49

Park, Chan Woo (Korea Atomic Energy Research Institute) , Kim, Ilgook (Korea Atomic Energy Research Institute) , Yoon, In-Ho (Korea Atomic Energy Research Institute) , Yang, Hee-Man (Korea Atomic Energy Research Institute) , Seo, Bum-Kyung (Korea Atomic Energy Research Institute)

Abstract ▼ AI-Helper

The behaviors of various desorption agents were investigated during the desorption of cesium (Cs) from samples of clay minerals and actual soil. Results showed that polymeric cation exchange agents (polyethyleneimine (PEI)) efficiently desorbed Cs from expandable montmorillonite, whereas acidic desorption solutions containing HCl or PEI removed considerable Cs from hydrobiotite. However, most desorption agents could desorb only 54% of Cs from illite because of Cs's specific adsorption to selective adsorption sites. Cs desorption from an actual soil sample containing Cs-selective clay mineral illite ( PEI > NH4+, and the highest Cs desorption amount achieved using HCl was 83%. Unlike other desorption agents with only cation exchange capabilities, HCl can attack minerals and induce dissolution of metallic elements. HCl's ability to both alter minerals and induce H+/Cs+ ion exchange is expected to promote Cs desorption from actual soil samples.

주제어

표/그림 (6)

$Fig. 1. XRD patterns of montmorillonite (MT), illite (IL), and hydrobiotite (HB); and the fraction of an actual soil sample (< 200 μm).$ 그림 Fig. 1. XRD patterns of montmorillonite (MT), illite (IL), and hydrobiotite (HB); and the fraction of an actual soil sample (< 200 μm).
표 Table 1. Elemental compositions of the clay minerals and the soil sample
표 Table 2. Amount of Cs adsorbed on the clay minerals and SF200¹, and percentage of adsorbed Cs ions to CEC of the samples
그림 Fig. 2. Cs-desorption efficiency of various desorption agents (20 mmol·g^-1) against (a) Cs-MT, (b) Cs-IL, (c) Cs-HB, and (d) Cs-SF200 (24 hr reaction).
그림 Fig. 3. Amount of radiocesium desorbed from ¹³⁷Cs-SF200 after reaction with various desorption agents (20 mmol·g^-1) at 20°C for 24 hr.
그림 Fig. 4. Cumulative amounts of radiocesium desorption by repeated treatment of ¹³⁷Cs-SF250 with desorption agents (20 or 50 mmol·g^-1) at 20°C (reaction time of each step: 24 hr).

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가설 설정

In the work reported in this paper, we investigated the behavior of various desorption agents (including polymeric cation exchange agents, single molecular cations, and acid) for desorption of Cs from clay minerals and actual soil sam- ples. The clay minerals investigated included expandable montmorillonite, non-expandable illite, and mixed-layer clay of expandable vermiculite and non-expandable biotite (hydrobiotite).

제안 방법

For analysis of the elemental contents in the samples, XRF measurements of the clay minerals and the SF200 were carried out (Table 1). As expected, the element contained in nearly all the samples was Si because it is a major component of phyllosilicate clay minerals and quartz.

대상 데이터

Cesium chloride, tetramethyl ammonium chloride (TMA), hydrochloric acid, poly(diallyldimethylammonium chloride) (PDDA, Mw < 100 kDa), hydrochloric acid, ammonium nitrate, and poly(ethyleneimine) with Mw = ~2 kDa (PEI_2k) and ~25 kDa (PEI_25k), were purchased from Sigma-Aldrich and used as received.
Montmorillonite (MT, SAz-1 from The Clay Minerals Society, USA) and illite (IL, 2, 500 mesh, Youngkoong Illite Co., Ltd.) were used as received. A hydrobiotite (HB, < 38 μm) sample was prepared by sequential treatment of vermiculite (Sigam-Aldrich) by mechanical milling (M 20 universal mill, IKA) and mechanical sieving using a standard test sieve (400 mesh) [16].
analyzed. Polymeric cations (PEI_2k, PEI_25k, and PDDA), single molecular cations (TMA and NH₄⁺), and strong acid (HCl) were tested as desorption agents. The PDDA and TMA contain permanently charged quaternary ammonium cations.
The clay minerals investigated included expandable montmorillonite, non-expandable illite, and mixed-layer clay of expandable vermiculite and non-expandable biotite (hydrobiotite). To investigate the behavior of Cs-desorption from actual soil samples containing various soil constitu- ents, soil samples were collected from near the Kori Nuclear Power Plant (NPP).
The soil samples were taken at depths of 0 to 15 cm from the soil surface within 2 km of the Kori NPP (35° 20′ 33″ N, 129° 17′ 33″ E). The soil fraction under 200 μm (SF200) was obtained by dry-sieving the soil using a vibratory sieve shaker (Retsch AS 200) with a standard sieve (Retsch, ISO 3310/1).
The clay minerals investigated included expandable montmorillonite, non-expandable illite, and mixed-layer clay of expandable vermiculite and non-expandable biotite (hydrobiotite). To investigate the behavior of Cs-desorption from actual soil samples containing various soil constitu- ents, soil samples were collected from near the Kori Nuclear Power Plant (NPP). In addition, the correlations between the mineral components and Cs-desorption behaviors were investigated.

이론/모형

For the XRF analysis, a double layer pellet (sample and boric acid) was prepared by pressing the clay or soil (200 mg) on an as-prepared boric acid pellet (6 g) using a hydraulic press at 20 t [20]. The cation exchange capacity (CEC) of clay minerals and soil samples were determined by following the SW-846 Test Method 9081 (U.S. Environmental Protection Agency).
The compositions of the clay minerals and SF200 were determined by X-ray diffraction (XRD) analysis using a Rigaku SmartLab diffractometer (Japan). The elemental contents in the samples were determined by energy dispersive X-ray fluorescence (XRF) spectrometry analysis using an S2 RANGER (Bruker).

성능/효과

Furthermore, the total amount of ¹³⁷Cs desorbed by two different concentrations of NH₄⁺ were almost identical (~32%). In these regards, it is concluded that NH₄⁺ is efficient for removing weakly bound Cs in actual soil in a single washing step, but that additional extraction of stably bound ¹³⁷Cs is inefficient.

후속연구

Unlike the other desorption agents, HCl is known to initiate disintegration of clay minerals [28, 35], and it was reported that Al and Fe elements can be partially dissolved from illite and kaolinite by an HCl solution [36]. It is predicted that the additional desorption of ¹³⁷Cs by repetitive HCl treatment is related to weakening of the structural integrity of the soil components; thus, more comprehensive study will be required.

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