6
WO 腊腓腖腎腕腘腝腅腁腂腇腚腡腛腞腙腈腤腣腃腄 腍腖腑腔腘腢腜腐腖腗腀腏腓腉腌腗腋腒腐腖腆腠腟 * 膻膘臥*臷膱臊 臝膡至膠至膠膑臍自膛膠膴膮膛 * 臝膡至膠膼膠膖膠腻腼膁膇膼膠膛 Preparation of Methylcellulose Microcapsules Containing L-Glutamine by Using Coalescence between Droplets in W/O Emulsion Masato Tanaka* , Yoshinari Taguchi* and Chieko Shima Department of Science and Technology, Graduate School, Niigata University, ,2*/* Ikarashi, Niigata-shi, Niigata 3/*,+2+ * Department of Chemical Engineering, Niigata University, ,2*/* Ikarashi, Niigata-shi, Niigata 3/*,+2+ ῌῌῌῌῌῌῌῌῌῌῌῌῌῌῌῌ It was investigated whether methylcellulose microcapsules containing l-glutamine were able to be prepared by using coalescence between two kinds of droplets in W/O emulsion or not. Methylcellulose as the shell material was dissolved in the one aqueous droplets and the tannic acid as the gelation agent for methylcellulose was dissolved in the other aqueous droplets. It was found that methylcellulose microcapsules were able to be prepared by coalescence between the two kinds of droplets. The mean microcapsule diameter and the content rate of l-glutamine were found to increase with the concentration of methylcellulose. Moreover, it was found that microcapsules were not destroyed in the water phase and l-glutamine was released through the ungelated part of the microcapsule shell. (Received May ,, ,**/ ; Accepted Jun. +0, ,**/) 膅腲腷膌腵膄腽膊腤臛腧腤膔腤臛腤臲膖腑膿腨腯臸腟腙腤膏腫臮至腖腞腌腯腎腦臛膥 腎腯腱膅腼腶膍腸腗腯臻膪臱腱膚腣腗腯臼臨臙膖膧膤腧臭腗腯腔腠腑腟腒腯腟腋腯腖腐 腖腢腑腭腪腧腟腒腯腓腝腖腦腏腢腡腑臣膷腕 腰腯腔腠腺腼膂膿腣腢腯腠腌腍腔腠腢腡腤致腤腛腪 腙腤腪腧腐腢腮膷腕腰腛腫腤腣腢腜腞腌腯 +腔腤腬腍腢腔腠腐腭膎膗腟臵臗腢膄膌腽腼腣膨腝腓臦臇腑膚腟腋腯膿膫膅腲腷膌腵膄腽膊腤臧臯膭臖 腱膞腗腯腔腠腥腢臝膬臛臫臅腤膞腣膩腗腯 腫腤腠膽腎腭腰腯腙腔腟膴膮腟腥臟臢臤腤臞腱臟臢臤腻腳膊臅腟腋腯膈膀膊腽膊膌腃腼腣腬腮膅腲腷膌 腵膄腽膊膖腗腯膭臖腱膞腗腯腔腠腱臌腩腛腔腤腛腪腣臬腱臰臬腠腖臢臬腱臆臬腠腖腛 WO 腴膅膊腻膉膍膲腣腏腌腞腻腳膊臅腠腢腯膈膀膊腽 膊膌腃腼腱膝腖腛膒膈膀膊腽膊膌腃腼腤腹膊膖臄 腟腋腯腾膍膃膍臈腱膝腖腛膒腠腱臀膐腕腘腯腔腠腣腬 膈膀膊腽膊膌腃腼膅腲腷膌腵膄腽膊腑臺臧腟腒腯腐腡 腍腐腱膳腖腛膈膀膊腽膊膌腃腼腤腾膍膃膍臈腣腬腯腹 膊膖腥Conn et al. 腭腣腬腮臚臃腣膴膮腑腢腕腰腞腌腯 ,腔腤腹膊膖膔腥臏膕腟腫臠膾腗腯腛腪腣膈膀膊腽膊 膌腃腼腱臫臅腠腖腛膅腲腷膌腵膄腽膊腤臺臧腣腪腧腕腰腞 腌腯 -.臑膶腟腥臟臢臤腤臞臐腠腖腞腤臦膢臤腱腗腯 L腸膊腾膆膍腱臂/腆腄2臓腠腖腞膈膀膊腽膊 膌腃腼腍腆L腸膊腾膆膍腤腱臶膟膖腕腘 腞膳腖腛+῏῍῎ῒ 臰臬腣臉腖腛腺腃膍膹臄腠腖腞臉腖腛至膋腻膀膍腥膺臗膼膯膣臎膜臒臧腤腫腤腱腨腛膅腲腷膌腵膄腽膊腻腳膊臅腠腢腯膈膀膊腽膊 膌腃腼 MC腥臜膓膖膠膣臎膜臒臧 腔腟 SM-.***臐腤 L腸膊腾膆膍 Gln腤臫膣臎膜臒臧腤 腫腤腱腙腰腚腰腌腛腙腖腞膈膀膊腽膊膌腃腼腤腹膊 膖臄腟腋腯腾膍膃膍臈 TA腥膦膖膠膣臎膜臒臧腤腫 * 3/*,+2+ 臝膡膵臝膡臋膸臕, 腤臹 2*/* 3/*,+2+ 臝膡膵臝膡臋膸臕, 腤臹 2*/* 腮腨臩腅Corresponding author[email protected] Nippon Shokuhin Kagaku Kogaku Kaishi Vol. /,, No. 3, .*0.++ (,**/) 腛腘406 22

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Page 1: W O - jstage.jst.go.jp

W�O���������� ���������������������� �!"��#$%

����*�� ����*� ���� � ���������

*�� �������������

Preparation of Methylcellulose Microcapsules Containing L-Glutamine

by Using Coalescence between Droplets in W/O Emulsion

Masato Tanaka*�, Yoshinari Taguchi* and Chieko Shima

Department of Science and Technology, Graduate School, Niigata University,

,�2*/* Ikarashi, Niigata-shi, Niigata 3/*�,+2+

* Department of Chemical Engineering, Niigata University,

,�2*/* Ikarashi, Niigata-shi, Niigata 3/*�,+2+

����������������

It was investigated whether methylcellulose microcapsules containing l-glutamine were able to be

prepared by using coalescence between two kinds of droplets in W/O emulsion or not. Methylcellulose as the shell

material was dissolved in the one aqueous droplets and the tannic acid as the gelation agent for methylcellulose

was dissolved in the other aqueous droplets. It was found that methylcellulose microcapsules were able to be

prepared by coalescence between the two kinds of droplets. The mean microcapsule diameter and the content rate

of l-glutamine were found to increase with the concentration of methylcellulose. Moreover, it was found that

microcapsules were not destroyed in the water phase and l-glutamine was released through the ungelated part of

the microcapsule shell. (Received May ,, ,**/ ; Accepted Jun. +0, ,**/)

����� !"#$�%#&�'� (�#$�#)��*+,-�.� /#012 345-6 78� $9:�7-�;�:��<=>?-�@A B:C�D?-�EF� G�HI%�J?-KL*.M-� �.N-6 3O3P*Q� $�D��.M-���R� ��PS*TUVW-KL� X�Y+DP-L5ZKL� PS#�[#\]D� /#��'� OP^U�VW\1#DP_45-+`6K#aZPKLOQ� bc.deP �!�Dfgh� �ij*C�.N-+k������ !"#lmno:p�?-KL'� )�P�q$�rs#p�Dt�?-1#Lu7QW-6 /K.� ���.'� vwx#y�R:vwx�z"s.N-{|"!"�}�Da^����� !"�?-no:p�?-KL:~�\6K#\]D� ��:���L3� w�:���L3\

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� � � �

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*�

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�/º ®Corresponding author`� [email protected]

Nippon Shokuhin Kagaku Kogaku Kaishi Vol. /,, No. 3, .*0 .++ (,**/) »01¼406 ® 22 `

Page 2: W O - jstage.jst.go.jp

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wt����������� . *** mPas� �!"�#$�,� ����%&'(� Fig. +�#$� )*+�,- 2./.+*/, m, %01 /.*.+*/. m-� 234�53�6� �� )*7�7- /.*.+*/, m� 089:;<�=>�?@� A �B� +�-�C(�D(E�� 234�53�6�,F�GH 3.+*/, m, I +.+*/, m�J�KLMNOPQR� .8SAT���

-� ����� ���Fig. ,�UV=�WX ��YO5��Z�[�#$�\] ^_`� Gln�^_`abc� �dZ�@�efE gHh�ijklmn)*�iAop���iq�rsHt S�O �solid-in-oil� rsu�YOE�� MC���� MCvw�xA"A Uyz�{=�>�3��|} �1*�� )* �,./ s/+� Ek��~��������|E � -��)*E�� ���� -��)*EkYOE�� !�MC������YOE� S�O �solid-in-oil� rsu�efEUyz�{=�>�3��)* �,./ s/+� Ek �S�O��Wrsu�YOE�� p� ���� �6�@�����������c���dZ�@���Htk)*+��fEk /*����E�� !����� ��YOE� �S�O� �Wrsu�efE��� 1./s/+�)*$�!"�iA ��S�O� �W� �Orsu�YOE�� ,��

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.� ����®%&�¯�E�%&°±� Table +�#$�

Fig. + Schematic diagram of experimental apparatus

Fig. , Flow sheet of experiment

Table + Experimental conditions

²Experimental Conditions³volume of continuous phase

volume of dispersed phase

amount of lecithin

volume of gelation agent solution

concentration of gelation agent

impeller speed

reaction temperature

reaction time

+42.+*o. m-

*4,.+*o. m-

/4*.+*o- kg

*40.+*o. m-

+* wt�14/ so+

/*�, hr

²Operation conditions³concentration of MC

amount of Gln

+4,/, +4/, +41/,

,4*, ,4,/, ,4/ wt�,4/, /4*.+*o- kg

´�µ : �¥�¦p�¶�E�y�>K@·¸ ����UV=�WX ��YO 407� 23 �

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/� ���������� ��������������� �������������������� � !"# ��� +$%� &S�O�' ()*���+,����-.%� &MC%�' /0�12�34546�7*%� &TA�' /�89��:# ��;8 <(=>?@�AB�� ������(C�?@�� D��� +�5EF����� �����1�.F-E��G?H�I��# )J��K�LM�N-������O*�%�P89���?H�D/(������ +,����-./34546/� <�# Fischer�L.Q�1��:# TA���RST�U�VOH/ TAW�MC�VOH &X*# RYVH�Z' ���/(�[/*���*# \;8?@�G]^�/_`a@�� D����# TA�\8/MC/�bc <(�Z��G*�d1��3'e+,'�

0� ����� �� ������fg��*�� �������fg�# ��h�i��j?@� +**k��� ������� lj*# D�!�:mI� �# "n���� �����g�# &#go$g'�,/*�mI� DD�# �fg�# p��%W��&�f�g Dp &Sautarg' /*�qr*�

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��*�� ������'�!�# ��h�i &{x4|.}p~��-BH-,' ��:uv*�W# �� ������C�# ()�*# ���+�,��-[h�i &SEM JSM-/2**# .�-[}p~��' ��:uv*� �� ���������+�# ������ /0*�1a@/0)�auv*�� 23���45�� �������45�# ������*�mI

� W�# �� ������+��67��:�:��*# 9%8 &/*�+*V0 kg' �8:�:# +*�+*V0 m-��9���:*����#;�<� ,*P��*��a�%��=% ���y��� &HPLC' �>?*� Gln@A�B%*� �# ��F� GLw�L4.���Inertsil ODS--, ..0f�+/* mm�C�# ��F�A�.*�# UV�r��<$� ,+* nm, �DE� ,* mMx46��% &x46F�� �x�F ,..�+*V- kg��9�� +�+*V- m-�+.¡¢�*# x46�O`� pH ,./���'# G= *.1 mL�min�B%*� B%*H�p���£�qr*# �45/*�

&�� ������I¤�8J:�Fs�tY ������r*Gln�\8'

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&�� ������I¤�8J:�Rs�tY 9%ZPQ��r*Gln�\8'

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�# B%� ,¬�­*# D@a�H��fH��C*�� �� ������R®A�� �������9��MN?HOP*� �*

�# 9%ZPQ��� ������w4�x4y*��h�i��£�� lj*� �*�p��:�fg Dp

�qr*# MNS��fg DpO/�T &Dp�DpO' �mI�R®A/*�

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+� ���������� !"#$MC%&�'(Fig. -�MC@A &CMC' (�� ������fg�¯°�j±�²�� �# U��# V§W³^�Z�²*� W# Fig. -��# �� ������X´?�j±

Fig. - E#ect of MC concentration on mean particle

diameter of microcapsules and viscosity of MC

aqueous solution

.�µY¶·¸·~¹ Z /, º Z 3 » ,**/ [ 3 ¼408 & 24 '

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����MC������� ��� ��������������� ��� MC!�""�� # +* mm

$% /** mm&"'()*+��,-"� -�.� �+.1/ wt�/0�!�123�*+��,-"45$,�-� � MC������4� MC6�$%78��9,":5�,� +.1/ wt�;<$%�=>*.��9?� @S�OA�W�B�CD��E��F�,�G�HI4.��,-"�JK�,�"LM%�,�

,� ���������Fig. .�� NOP�,Q� @S�OA�W�B"� NOP4R���S�TUVWXYZO�[\2]^�9,_`ab� ���Bcd1 ����1e, @S�OA B4MC���f�Eg���,cd4hi1(,� j�� TUVWXYZO�k\l$%TUVWXYZO mn1e,-"� Gln�Egop�qrst4MCu�9?�v�wxo���,-"4hio�,�

Fig. /�TUVWXYZOy�� SEM_`�ab� �� MC!�4z�{|1}~o��TUVWXYZO�y�� ���4e?�$���#�]�4�����,-"45$,� -��F��� MC!�4��{|1}~o��TUVWXYZO�y� �����%$1�$��]� _`o�*)*+��,� -� � MC!�4��"�

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-� �����TUVWXYZO������� � ��*TUVWXYZO��G1e,-"$%� �����������"LM%�,MC!�&���G�}�� Fig. 0���ab� ��� �� � !�""�=>�.����,� ��� MC!� ,./ wt�1 � ��7��<���"*+��,� -� � !��.������ MC�����"�B�4'()*? ¡�Eg���, @S�OA B�Eg¢£G4.��,""�� @S�OA B�MC�B$%� ¤4�¥o�,-"�JK���,"LM%�,�j�� ������7�4���������� MC!� ,.,/ wt��{|1TUVWXYZO�}~��¦§��� -�9?� ��7�4 ,./ g" /.* g�¨81��©�+-�� ,0�"*?� ��7�""�ª��4.����

.� �����}~o��TUVWXYZO�����«¬­��¦§�,���� ®O¯°t��±&�²³��´�µP�¶

Fig. . Photographs of microcapsule

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Fig. 0 E#ect of quantity of core material on content rate

·�¸ : �B¹8º�����®O¯°tª�ZOW»¼TUVWXYZO�}~ 409@ 25 A

Page 5: W O - jstage.jst.go.jp

��� ����� Fig. 1�� � ��MC��������� ������������� ��MC���� �� Gln�!"� #$%&�'()*+,-�./#$0� �1���2� ,*3456� �� ,*��7�8�9:#$ �%;&��1%� <0� 7�8�=>��?@A� �� ��$�BC D,./ g& /.* gE �� ��� -*��()*+,-�F;%;&� =>��GH�%&� ��I>�%;&� ,*3456� �� +/J-*��7�8�9:#$ �%;&� ���K1%�

/� �������Fig. 2LM#$0NOPQRSTU�VWX����Y�%0Z� NOPQRSTU�VW��[\]^�NOPQRSTU_� DDp�DpOE ��� MC���`�abcd�e�%fg�./#$%���� 7�8=>�&MC����h#i �NOPQRSTU��j�./#$��� ;�;&�� LM#$0NOPQRSTU�MCklU�� mnop#$ �%0Z� Veq%�j� r#$0��&st2$%� �1���2� Fig. 1���12K1%q'� �op��MC��u�%;&qv� 9:#$07�8� Gln�� #$%��&st2$%�

7�8�9:�0klUw�xyUTUQ+,Vz&{Uh|�}%~����Vz&�b��� W�O������#i%;&qv� ���%�V�b������ NOPQRSTU�LM�%;&���0� �� � ���q'�����0�� W�O�������0�4b�qv� �U~�

��9:�0xyUTUQ+,RSTU�LM�%;&����}�0�� xyUTUQ+,���&&�� NOPQRSTU_���H�%&&�� ����I>�0�� ��$�BC�LM�0NOPQRSTU�� -*�]^�()*+,-��0;&12� #2�%LMBC���h����}%�� NOPQRSTU�VW��e�j�./#$�1�0�� �U~���� �� �op��xyUTUQ+,��u&��^��U~����uq%��&�/#$0�

+E �� �� ���NOPQRSTU�� D ¡ �E� D+322E�,E Conn. E., P. Stumpb, G. Bruening and R. Doi, ; Outlines

of Biochemistry, /th ed., John Wiley & Sons, California,

USA D+321E�-E ¢£¤¥� £¦§¨� £W�© ; ª«¬­�N-®¯P,&�%��u�RSTU�LM� h°±°��²� ,/ D/E�0,3�0-/ D,**+E�

.E Taguchi, T., Yamada, Y., Ishikura Y. and Tanaka, M.,

Preparation of Biodegradable Capsules Composed of

Paper Fiber by Utilizing Liquid-Liquid Dispersion, J.

Fig. 1 E#ect of soaking time of microcapsules into

distilled water on release rate

Fig. 2 E#ect of soaking time of microcapsules into

distilled water on mean particle diameter of

microcapsules

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