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1 w y wz 9«( 2y 00~00, 2006 J. of the Korean Society for Environmental Analysis q w p w q ½»x Á½ {*Á Á Áy Á * w y w, * w tœw Characterization of Malodor Release from Decaying Foods and Tactics for Odor Control through Microbial Treatment K.H. Kim, Y.H. Kim*, M.S. Im, S.Y. Park, Y.J. Hong, and B.S. Choi* Dept. of Earth & Environmental Sciences, Sejong University *Dept. of Food Science and Technology, Sejong University In this study, the concentrations of major odorous compounds were measured from decaying food samples made of meat and fish as a function of time. The experimental data were collected as part of two different experiment types; experiment type 1 was made using food samples decaying continuously, while experiment type 2 was made by applying microbial treatment to those decaying food samples. The results of meat samples have shown that the emission concentrations of most odorous compounds were distinctive enough; in the case of reduced sulfur compounds such as hydrogen sulfide and methane thieol, their concentrations commonly approached a few hundred ppm values. However, the observed concentrations from fish samples were substantially low due to the effect of the initial salt treatment. According to the microbial treatment experiment, its initial effect is dramatically effective enough to remove the dominant proportion of certain odorous species such as some reduced sulfur compounds and ammonia; however, such removal effects are found to fade away through time. The results of our preliminary study were successful to characterize odorous emissions from rotting food samples. However, more studies are needed to explain mechanistically the effect of microbial treatments under different experimental settings. Key words: food, decay, malodor compounds, reduced sulfur, hydrogen sulfide 1. y w j w wì y {» ƒ g. y d w ƒ, w sw ¾ w w wù û. 1,2 yy w w p w w q š. q yy ƒ w wù w. q x» w, ü ww x w. y ù sww»yw ³ w w w., yy ù ƒ. q p q w w w. w x p» w w w. 3 x w w» w w» w. 4,5 To whom correspondence should be addressed. khkim@sejong.ac.kr

2 q w p w q 75 w q l w p q wš w. w x qy p w w. w mw, q p w w w. m q w ù»» q w y wš w. w w w z» wš w q z sƒ w x y l 40», x q jš q l w.» w w 12ƒ s sww 5 32 Table 1. A list of chemicals investigated for malodor released by decaying food samples in this study. Full name Modified Name Structural formula Ref Treshold concentration Formaldehyde Form-A HCHO Acetaldehyde Acet-A CH 3 CHO * Acrolein Acrolein CH 3 =CHCHO A. Carbonyl compounds B. Reduced S compounds C. N compounds Acetone Acetone CH 3 COCH 3 Propionaldehyde Propion-A CH 3 CH 2 CHO * crotonaldehyde Croton-A CH 3 CH=CHCHO Butyraldehyde Butyr-A CH 3 CH 2 CH 2 CHO * Benzaldehyde Benz-A C 6 CHO Iso-valerldehyde Isovaler-A (CH 3 2 CHCH 2 CHO * valeraldehyde Vale-A (CH 2 3 CHO * o-tolualdehyde o-tolu-a CH 3 C 6 H 4 CHO m-tolualdehyde m-tolu-a CH 3 C 6 H 4 CHO p-tolualdehyde p-tolu-a CH 3 C 6 H 4 CHO ¾ Hydrogen sulfide H2S H 2 S* * Methyl mercaptan CH3SH CH 3 SH* * Dimethyl sulfide DMS (CH 3 2S* * Carbon disulfide CS2 CS 2 * 0.21 Dimethyldisulfide DMDS (CH 3 2 S 2 * * Ammonia NH3 NH 3 * 0.1 Trimethyl amine TMA (CH 3 3 N * Total VOC TVOC C ¾ Benzene B C 6 H Toluene T C 6 CH 3 Ethylbenzene E C 6 C 2 D. Total and individual VOC m,p-xylene MPX (CH 3 2 C 6 H 2 o-xylene OX (CH 3 2 C 6 H4 Styrene STY C 6 CH=CH 2 * 0.03 Bromobenzene BB C 6 Br 1,3,5-Trimethylbenzene 1,3,5-TMB (CH 3 3 C 6 H 6 1,2,4-Trimethylbenzene 1,2,4-TMB (CH 3 3 C 6 H7 p-isopropyltoluene p-ipt C 10 H 14 n-bultylbenzene n-bb C 10 H 14 ¾ ¾ *A list of chemicals designated as malodor compounds by the Korean Ministry of Environment (Since Feb., 2005

3 76 ½»xÁ½ {Á Á Áy Á ƒ ww l w w (Table 1: (1 p w w e 13ƒ, (2 yy w y y 5ƒ, (3 TVOC VOC sww 12ƒ, (4 p p ( w TMA. wì œ x» d w. q w» w ƒ kw. [1] v [2] ƒw ( e 470, 140 g ƒƒ w. 2ƒ 2.5 L n x» 2 4 q x y w.» š, 1/4 e l v 10 cm ¼ w. mw, y» w r w. w Table 2 w, j 4ƒ w : M1, M2, F1, F2.» M F (meat (fish š 1 2 w q w q z ƒw w» w y w w w mw w. š w w» w» ƒ w w w» w w., y y, VOC, TMA,» w œx v (lung sampler w w. l w œx v w œ k x w q ¼»ü œ» ü g. w» 5 L w. l w p yw wwš w w. w yw» w w v lv w. 5 w w k z,»k y w. p w w e DNPH e p (Supelco, USA w w. rv ( q k yw» w, ep KI j DNPH ep w w. œ x 7» v w. w, v» m g w. w ƒƒ w y y y y ƒ l ww w. 6 Peltier cooling Table 2. A scheme for decay experiment with and without microbial treatment as a function of time (number of days.* Exp Type** Exp No. ¾ ¾ ¾ ¾ ¾ ¾ Ref (sample ¾ ¾ [1] Exp type 1: Decaying only M1(F hr Decay [2] Exp type 2: Decaying with microbial treatment M2(F2 0 8 Decay 1 hr Treatment *Samples are prepared as replicates and analyzed separately for two different experiment types. **Capital letters of M and F denote meat and fish, respectively, while numbers of 1 and 2 denote experiments with decay only and decay plus microbial treament, respectively.

4 q w p w q 77 (PC/Thermal desorber (TD (Unity & Air server: Markes, Ltd., UK w, k w cold trap yyw (1, (2 š, (3 GC g w. š y ƒ PFPD (Pulsed Flame Photometric Detector: O.I Co., Model 5380, USA w GC (Donam instrument, Model: DS 6200, Korea w. w» FPD w w, k, x, w j k l, pg y y w w. 8 Nafion dryer ew, w GC ƒ yw. š w cold trap Carbopack B Silica Gel w. e BP-1 (Length: 60 m, ID: 0.32 mm, Film thickness: 5.0 µm, SGE w {»yw {»yw (VOC y y w w PC/TD l FID (Frame Ionization Detector GC (Donam instrument, Model: DS 6200, Korea w w. VOC v 9 Nafion dryer w PC/TD w yw. VOC w cold trap Carbopack B Carbopack C 1:1 w w. e DB-VRX (Length: 60 m, ID: 0.32 mm, Film thickness: 1.8 µm, J&W w. w l v (400 ml», benzene 0.14 ppb, toluene 0.11 ppb, ethylbenzene 0.11 ppb, m,p-xylene 0.04 ppb, styrene 0.12 ppb w ùkü. w t (RSE w w, 5% ü ùkû p p (TMA p p (TMA, l w SPME (polydimethylsiloxane/ dicinylbenzene, 65 µm film w - w w. w TMA SPME w k z, GC (Donam instrument, Model: DS 6200, Kor injector 210 C o 3 k w. TMA GC ü w» w e CP-Wax52CB (Length: 50 m, ID: 0.32 mm, Film thickness: 1.2 µm, Chrompack w. TMA VOC y w GC/FID w l w. w x œ x 10 ƒ. w, l w TMA w». ù rw, w w mw w. 11 ƒ w, TMA w e p w w e w» w, HPLC w. DNPH ep 5 ml acetonitrile w z, 20 µl j HPLC w e w. e Hichrom 5 C18 (Length: 25 cm, ID: 4.6 mm, : reversed phase w. e 13ƒ ƒ z, 65% acetonitrile (acetonnitrile:water=6.5:3.5 w. w w 2,4-DNPH w ƒ ƒ ù 360 nm q (UV ƒƒ w w.» mw 7 yw y w ƒ,» ü dw, d (9.2 l w 0.48~0.58 ppb w w ùkû. w, 0.61~1.90% ùkû UV/VIS Ÿ d» (Model Genesys TM 10 series, Thermo electron Corp. w. m g (10 ml r p t (5 ml k z, ùp (5 ml w g ( 20 ml. w e, r w. yw

5 78 ½»xÁ½ {Á Á Áy Á 1 e z, Ÿ w. w»» w» ùkü q z w» w w. l t SJP glucose 30[g/L] * Bacto peptone 10[g/L] * Malt extract[g/l] * Yeast extract 3 [g/l] w. š 100 ml-ymp media 1ml w z, 28 o C, 200 RPM 24 shaking incubator w. qƒ 8 ww M2 F2» w SJP 1 ml ƒƒ w. SJP n w» w w ph 4.54, ³ [FU/ml] k w. 3. m 3.1. q x» Table 2 w x w w. M1 F1 w x qƒ w (t=0 day l 40 ¾ x ww. š» 6, Tedlar bag w» ü wš w. Table 2 w š» w q x w w,. x t ƒ x x ww. x 1x w q w w š x 2x qƒ ww ƒw / q wš w. w e x 1x q x w» ƒƒ 6 wš w 6 x ww (Table 2 x 1, 2, 3, 4, 5, 6. qƒ» wš, z ƒ 5 w : x 2 6 ƒƒ 8, 8 1, 9, 15, 40 w w. qƒ w w x 2» 8 w ƒ w qƒ š w. ww» w» w. 8 z w w q ww y z w w ƒ x w» w. x 2x x 1 w w 6 w w» l 6 xw ww. ù x, x 1 2 x 1x w w. x 3, 4, 5, 6 ƒw 1,, w z w» w ww x w. x 1x ù 2x w 6 x ww, w w w ƒ w v ƒ w w w w ƒ» w. (1 w q w sƒw» w x 1x w w, (2 p w x 2x sƒ, (3 z sƒ w» w x 1, 2 x 3ƒ sƒwš w. w ƒ» q w» w, w y ƒ w» w. ƒ x 1x w w w. x 1 6¾ x 3 4 w q w q wš w. 6 x w 2.5 l» 5 l w, x 3 4 z w ƒ w» w y. š» w x 1x w Table 3, 4, 6 x x 3, 4 ƒ w û w y w. q 1A w x 1, 2, 5, 6 w. z» w

6 음식물의 부패에 의한 악취발생 특성 및 미생물을 이용한 부패악취저감 연구 언급한 바와 같이 실험 3, 4, 5, 6의 자료만을 활용하였 다. 결과적으로 실험 2의 단계를 통해, 8일까지 부패조 건이 유지된 시료에 미생물을 가한 후 1시간, 1일, 7일, 32일의 경과시점에 채취 및 분석을 하였다고 볼 수 있 다. 그리고 미생물처리에 따른 악취물질의 배출경감 효 과를 평가하기 위한 비값의 산출은 실험 3, 4, 5, 6의 결과로부터 도출하였다 (Table 5 참조. 이러한 비교에 활용한 실험 3, 4의 결과는 앞서 언급한 바와 같이 시 료채취 간격의 문제로 인해 절대 농도의 크기가 현저하 게 줄어들지만, 실험 1, 2형 모두 비교 대상구가 형성되 었다는 점에서 양 실험 유형의 결과를 이용한 비값을 Table 산출하는 데에는 별다른 문제가 없을 것으로 사료된다. 부패의 진행과 악취물질의 배출 특성 Table 3, 4에는 고기와 생선의 부패로부터 발생하는 악취성분들의 배출경향을 시간의 함수로 각각 제시하 였다. 양 쪽 표에는 일단 6차례의 실험결과를 가감없이 모두 제시하였지만, 앞서 설명과 같이 이들 결과 중 실 험 3, 4에 대한 절대치의 변화경향에 대한 해석에는 주 의가 필요하다. 그림 1A에는 실험 3, 4의 결과를 제외 한 황성분들의 악취발생 경향을 시간의 함수로 제시하 였다. 그리고 Table 3에는 모든 실험결과를 단순한 농 3.3. Results of meat corruption experiment as a function of decaying inverval (ppm unit.

7 80 Table 4. 김기현 김용휘 임문순 박신영 홍윤정 최병선 Results of fish corruption experiment as a function of decaying interval (ppm unit. 도의 크기만 제시하는 대신, 그 농도에 상응하는 악취 도 (로마숫자의 형태로도 동시에 제시하였다. 각 성분 의 농도에 상응하는 1에서 5도까지의 악취도로의 환산 은 기존에 발표된 환산식을 이용하였다. Table 3의 고기시료에 대한 결과를 보면, 부패가 진행하면서 악취 물질의 배출이 꾸준하게 이루어진 것을 알 수 있다. 특 히, 황화수소를 위시한 황계열 화합물들은 수 백 ppm 에 달하는 고농도의 배출이 이루어지면서, 악취도도 5 도의 수준을 보일 정도로 높게 나타났다. 이러한 경향 은 암모니아도 5도 수준을 유지할 정도로 수 백 ppm 6,12 수준의 고농도가 상당 수준 지속된 것을 볼 수 있다. 작은 양 (10 g의 고기, 생선, 부패음식 등의 악취물질 을 조사한 윤순일 의 선행연구에서도 이와 같이 황계 열 화합물의 고농도 배출현상을 확인한 바 있다. 14일 정도를 부패시킨 상태의 고기시료에서 황화수소 11 ppm, 메틸치온 9 ppm 등의 농도를 확인한 바 있다. 이들 성분에 비해 상대적으로 약하지만, 악취의 배출이 지속되는 경향은 카보닐, VOC, TMA 성분들에서도 확 인할 수 있다. 희석배수도 8일이 경과한 시점에 4백만 배 이상의 값을 보이며 가장 높게 나타났고, 실험 5, 6 13

8 음식물의 부패에 의한 악취발생 특성 및 미생물을 이용한 부패악취저감 연구 Table The effect of microbial treatment on meat samples is compared by applying microbial treatments on samples for 8 days under rotting conditions. As the time peirod of these experiments is counted upon the time of microbial treatment, addition of 8 days will match the time scale introduced in the experimental scheme of Table 2. 에서도 조금 감소하였지만 높은 수준의 결과를 보였다. 비교 대상으로 활용한 생선시료의 악취성분에 대한 발생경향을 비교해 보면, 모든 악취 성분들의 농도가 현저하게 떨어져 있다는 것을 확인할 수 있다 (Table 4. 이러한 경향은 가장 민감한 악취성분에 해당하는 황 계열 성분만의 결과를 분리해서 제시한 Fig. 2에서도 뚜렷하게 확인할 수 있다. 생선의 부패과정에서 발견한 배출농도는 선행연구들에 비해 현저하게 낮은 수준이 다. 윤순일(2003의 연구결과에 의하면, 생선시료의 경 우 고기시료에 비해 황화합물의 배출농도가 대략 3~6 배 정도 높은 수준을 유지하는 것으로 제시한 바 있다. 이는 실험에 사용한 생선시료 (꽁치가 미리 소금에 절 어둔 상태로 준비한 데 따른 효과로 볼 수 있을 듯 하 다. 비록 성분에 따라 큰 차이는 있지만, 소금으로 처 리한 생선시료의 결과를 보면, 고기 시료에 비해 대략 1,000 배 가까이 낮은 수준의 농도를 띄는 것으로 나타 났다. 이러한 경향은 거의 모든 악취성분들에서 일관적 으로 나타난다. 결과적으로 소금처리는 악취발생의 경 향에 현저한 영향을 미친다는 것을 알 수 있다. 따라서 악취저감에 대한 해석은 생선시료에 대한 분석결과 대 신, 고기시료에 대한 결과를 중심으로 시도하였다. 미생물 처리를 통한 악취저감 효과의 비교 미생물처리의 효과를 평가하기 위한 결과를 간략하 게 파악하기 위해, Table 5에는 고기를 이용한 실험 결과 중 1, 2 유형의 실험 중 실험 3, 4, 5, 6의 결 과만을 동시에 비교할 수 있게 제시하였다. 그리고 이 들 양 쪽 유형의 농도치를 이용한 비값을 산출하였다. 실험 1/실험 2의 비값을 산출하면, 미생물 처리의 효과 에 대한 특성을 단순하게 평가하는 것이 가능하다. 단 미생물의 처리에 따라 일부 성분들은 갑자기 검출한계 이하로 떨어지는 경향을 보이기도 한다. 따라서 비값의 3.4.

9 82 ½»xÁ½ {Á Á Áy Á Fig. 1. Comparison of release patterns for odorous sulfur compounds from decaying meat samples is made as a function of time (number of days. w w w e ew w. Table 5, z ƒ y ƒ w ùkù. p yy, 1 1 z ƒ¾ z ƒ ùkù. š ú z w, 7 z 7 š w w ƒ ù. w z 1 w q w q y w w, ƒ x w w. w, SJP w y q y qx w, ƒ ƒw z w. w y z» Fig. 2. Comparison of release patterns for odorous sulfur compounds from decaying fish samples is made as a function of time (number of days. w w, ù k z w. w yw, TMAù w w y w. w, VOC, w z ƒ w w ù w. 4. š» ew p w. š ƒ qw 8 ƒwš, z w., w w w w,

10 q w p w q 83 y yw ppm w š x y w. p w ¼ w, w w y w. ƒw x w, w z y w z ƒ w y w. p x» y w ¾ ƒ, ƒ ƒw p w v ƒ. p» w ƒ ü w, w f w ƒeƒ. mw, ù p w l w v y w. ö l»y. š x 1. Steinmann, A., Environmental Impact Assessment Review, 2004, 24, Rappert, S. and Muller, R., Waste Management, 2005, in press. 3. Liang, Y.-X, Su, Z.Z., Wu, W.-A, Lu, B.-Q, Fu, W.-Z, Yang, L. and Gu, J.-Y., Regulatory Toxicology and Pharmacology, 2003, 38, Kim, K.H., Environ. Sci. & Technol, 2005, 39(17, Kim, K.H., Choi, G.H., Choi, Y.J., Song, H.N., Yang, H.S., and Oh, J.M., Talanta, 2006, 68, ½»x,, y, y, y,,,, w»y wz, 2005, 21(2, y, ½»x, w wz, 2005, 18(1, ,, ½»x, w»y wz, 2005, 21(5, Kim, K.H., Oh, S.I., and Choi, Y.J., Talanta, (2, , ½»x,,, w»y wz, 2006, nš. 11. ½»x, x x,, w wz, 2006, 19(1, Nagata, Y. and Takeuchi N., Bulletin of Japan Environmental Sanitation Center, 1980, 7, Yun, S-I, Kor. J. Microbiol. Biotechnol., 2003, 31(4,

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