JP6734317B2 - 放射性核種の除去方法 - Google Patents
放射性核種の除去方法 Download PDFInfo
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- 238000004132 cross linking Methods 0.000 claims description 23
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 21
- 125000002887 hydroxy group Chemical group [H]O* 0.000 claims description 19
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 claims description 13
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- FHVDTGUDJYJELY-UHFFFAOYSA-N 6-{[2-carboxy-4,5-dihydroxy-6-(phosphanyloxy)oxan-3-yl]oxy}-4,5-dihydroxy-3-phosphanyloxane-2-carboxylic acid Chemical compound O1C(C(O)=O)C(P)C(O)C(O)C1OC1C(C(O)=O)OC(OP)C(O)C1O FHVDTGUDJYJELY-UHFFFAOYSA-N 0.000 claims description 10
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- JMZFEHDNIAQMNB-UHFFFAOYSA-N m-aminophenylboronic acid Chemical compound NC1=CC=CC(B(O)O)=C1 JMZFEHDNIAQMNB-UHFFFAOYSA-N 0.000 description 3
- 229920002521 macromolecule Polymers 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 229910052712 strontium Inorganic materials 0.000 description 3
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- OZAIFHULBGXAKX-UHFFFAOYSA-N 2-(2-cyanopropan-2-yldiazenyl)-2-methylpropanenitrile Chemical compound N#CC(C)(C)N=NC(C)(C)C#N OZAIFHULBGXAKX-UHFFFAOYSA-N 0.000 description 2
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- 238000005481 NMR spectroscopy Methods 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 description 2
- 229910021536 Zeolite Inorganic materials 0.000 description 2
- 229910000019 calcium carbonate Inorganic materials 0.000 description 2
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- 229910017052 cobalt Inorganic materials 0.000 description 2
- 239000010941 cobalt Substances 0.000 description 2
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 2
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 2
- 238000001035 drying Methods 0.000 description 2
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- WBJZTOZJJYAKHQ-UHFFFAOYSA-K iron(3+) phosphate Chemical compound [Fe+3].[O-]P([O-])([O-])=O WBJZTOZJJYAKHQ-UHFFFAOYSA-K 0.000 description 2
- NCNCGGDMXMBVIA-UHFFFAOYSA-L iron(ii) hydroxide Chemical compound [OH-].[OH-].[Fe+2] NCNCGGDMXMBVIA-UHFFFAOYSA-L 0.000 description 2
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- YLGYACDQVQQZSW-UHFFFAOYSA-N n,n-dimethylprop-2-enamide Chemical compound CN(C)C(=O)C=C YLGYACDQVQQZSW-UHFFFAOYSA-N 0.000 description 2
- HXITXNWTGFUOAU-UHFFFAOYSA-N phenylboronic acid Chemical compound OB(O)C1=CC=CC=C1 HXITXNWTGFUOAU-UHFFFAOYSA-N 0.000 description 2
- 238000011084 recovery Methods 0.000 description 2
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- 239000010457 zeolite Substances 0.000 description 2
- QWMJEUJXWVZSAG-UHFFFAOYSA-N (4-ethenylphenyl)boronic acid Chemical compound OB(O)C1=CC=C(C=C)C=C1 QWMJEUJXWVZSAG-UHFFFAOYSA-N 0.000 description 1
- IXPNQXFRVYWDDI-UHFFFAOYSA-N 1-methyl-2,4-dioxo-1,3-diazinane-5-carboximidamide Chemical compound CN1CC(C(N)=N)C(=O)NC1=O IXPNQXFRVYWDDI-UHFFFAOYSA-N 0.000 description 1
- WUKANDNCRFGEHC-UHFFFAOYSA-N 3-(dimethylamino)propyl-(ethyliminomethylidene)azanium;chloride;hydrochloride Chemical compound Cl.Cl.CCN=C=NCCCN(C)C WUKANDNCRFGEHC-UHFFFAOYSA-N 0.000 description 1
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 1
- BHPQYMZQTOCNFJ-UHFFFAOYSA-N Calcium cation Chemical compound [Ca+2] BHPQYMZQTOCNFJ-UHFFFAOYSA-N 0.000 description 1
- 229910052684 Cerium Inorganic materials 0.000 description 1
- 241000870659 Crassula perfoliata var. minor Species 0.000 description 1
- CKLJMWTZIZZHCS-UHFFFAOYSA-N D-OH-Asp Natural products OC(=O)C(N)CC(O)=O CKLJMWTZIZZHCS-UHFFFAOYSA-N 0.000 description 1
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- CKLJMWTZIZZHCS-REOHCLBHSA-N L-aspartic acid Chemical compound OC(=O)[C@@H](N)CC(O)=O CKLJMWTZIZZHCS-REOHCLBHSA-N 0.000 description 1
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 230000000996 additive effect Effects 0.000 description 1
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 1
- YVBOZGOAVJZITM-UHFFFAOYSA-P ammonium phosphomolybdate Chemical compound [NH4+].[NH4+].[NH4+].[NH4+].[O-]P([O-])=O.[O-][Mo]([O-])(=O)=O YVBOZGOAVJZITM-UHFFFAOYSA-P 0.000 description 1
- 150000003863 ammonium salts Chemical class 0.000 description 1
- 150000001450 anions Chemical group 0.000 description 1
- 229910052787 antimony Inorganic materials 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 229960005261 aspartic acid Drugs 0.000 description 1
- 229910001424 calcium ion Inorganic materials 0.000 description 1
- YCIMNLLNPGFGHC-UHFFFAOYSA-N catechol Chemical group OC1=CC=CC=C1O YCIMNLLNPGFGHC-UHFFFAOYSA-N 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
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- 150000001875 compounds Chemical class 0.000 description 1
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- 229910001873 dinitrogen Inorganic materials 0.000 description 1
- 150000002009 diols Chemical group 0.000 description 1
- 239000006185 dispersion Substances 0.000 description 1
- 238000004090 dissolution Methods 0.000 description 1
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- 239000006260 foam Substances 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 239000000499 gel Substances 0.000 description 1
- 229910052588 hydroxylapatite Inorganic materials 0.000 description 1
- 235000014413 iron hydroxide Nutrition 0.000 description 1
- 229910021506 iron(II) hydroxide Inorganic materials 0.000 description 1
- 230000005415 magnetization Effects 0.000 description 1
- 229940099596 manganese sulfate Drugs 0.000 description 1
- 239000011702 manganese sulphate Substances 0.000 description 1
- 235000007079 manganese sulphate Nutrition 0.000 description 1
- SQQMAOCOWKFBNP-UHFFFAOYSA-L manganese(II) sulfate Chemical compound [Mn+2].[O-]S([O-])(=O)=O SQQMAOCOWKFBNP-UHFFFAOYSA-L 0.000 description 1
- 230000007935 neutral effect Effects 0.000 description 1
- 229910052758 niobium Inorganic materials 0.000 description 1
- 239000012299 nitrogen atmosphere Substances 0.000 description 1
- XYJRXVWERLGGKC-UHFFFAOYSA-D pentacalcium;hydroxide;triphosphate Chemical compound [OH-].[Ca+2].[Ca+2].[Ca+2].[Ca+2].[Ca+2].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O XYJRXVWERLGGKC-UHFFFAOYSA-D 0.000 description 1
- 229910001414 potassium ion Inorganic materials 0.000 description 1
- 230000001376 precipitating effect Effects 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 238000010926 purge Methods 0.000 description 1
- 230000002441 reversible effect Effects 0.000 description 1
- 229910001419 rubidium ion Inorganic materials 0.000 description 1
- 229910052707 ruthenium Inorganic materials 0.000 description 1
- HBROZNQEVUILML-UHFFFAOYSA-N salicylhydroxamic acid Chemical group ONC(=O)C1=CC=CC=C1O HBROZNQEVUILML-UHFFFAOYSA-N 0.000 description 1
- 235000010413 sodium alginate Nutrition 0.000 description 1
- 239000000661 sodium alginate Substances 0.000 description 1
- 229940005550 sodium alginate Drugs 0.000 description 1
- 229910001415 sodium ion Inorganic materials 0.000 description 1
- 239000007921 spray Substances 0.000 description 1
- CADICXFYUNYKGD-UHFFFAOYSA-N sulfanylidenemanganese Chemical compound [Mn]=S CADICXFYUNYKGD-UHFFFAOYSA-N 0.000 description 1
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical compound O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/22—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising organic material
- B01J20/26—Synthetic macromolecular compounds
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
- B01J20/28—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof characterised by their form or physical properties
- B01J20/28014—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof characterised by their form or physical properties characterised by their form
- B01J20/28047—Gels
-
- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J3/00—Processes of treating or compounding macromolecular substances
- C08J3/24—Crosslinking, e.g. vulcanising, of macromolecules
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L101/00—Compositions of unspecified macromolecular compounds
- C08L101/02—Compositions of unspecified macromolecular compounds characterised by the presence of specified groups, e.g. terminal or pendant functional groups
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- G—PHYSICS
- G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
- G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
- G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
- G21F9/001—Decontamination of contaminated objects, apparatus, clothes, food; Preventing contamination thereof
- G21F9/002—Decontamination of the surface of objects with chemical or electrochemical processes
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- Organic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- Analytical Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Polymers & Plastics (AREA)
- Medicinal Chemistry (AREA)
- Life Sciences & Earth Sciences (AREA)
- High Energy & Nuclear Physics (AREA)
- General Engineering & Computer Science (AREA)
- Physics & Mathematics (AREA)
- Food Science & Technology (AREA)
- General Chemical & Material Sciences (AREA)
- Dispersion Chemistry (AREA)
- Electrochemistry (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
Description
本発明は、ヒドロキシ基を含む第1高分子と、ボロン酸基が官能基として導入された第2高分子と、放射性核種除去用吸着剤とを含む放射性核種除去用組成物を提供する。
本発明は、(a)ヒドロキシ基を含む第1高分子を含有する第1溶液を準備する段階と、(b)ボロン酸基が官能基として導入された第2高分子を含有する第2溶液を準備する段階と、(c)放射性核種による汚染表面上に前記第1溶液および前記第2溶液をそれぞれ噴射または塗布した後、前記第1高分子および前記第2高分子を互いに架橋結合させて、放射性核種が吸着されたハイドロゲルを形成させる段階とを含み、前記第1溶液または前記第2溶液に放射性核種除去用吸着剤をさらに含有することを特徴とする放射性核種の除去方法を提供する。
実施例1
第1高分子としてポリビニルアルコール8重量%および放射性セシウム除去用吸着剤としてプルシアンブルーがコートされた磁性吸着剤(図2を参照)0.5重量%を含む水溶液(第1溶液)を準備した。
まず、ポリスクシンイミドを下記のような方法で合成した:L−アスパラギン酸40gをスルホラン200mLに溶かした後、これにリン酸15mmolを添加した後、N2雰囲気下に170℃で10時間撹拌した。撹拌する中に生成される水は、ディーン・スターク・トラップ(Dean−stark trap)を利用して除去した。次に、過量のメタノールに沈殿させて合成物を回収し、水に分散させて、水溶液のpHが中性になるまで沈殿および分散を繰り返した後、乾燥させて、ポリスクシンイミドを最終的に合成した。
ポリメチルビニルエーテル−alt−マレイン酸無水物(Sigma Aldrich社、製品番号416320)(Mw=1,080,000)1gおよび3−アミノフェニルボロン酸0.3gを水100mLに溶かした後、24時間反応させた。以後、透析を通じて未反応物を除去して、第2高分子を製造した(図8を参照)。これを2重量%で含む水溶液(第2溶液)(pH8.5)を準備したことを除いて、実施例1と同じ方法で放射性セシウムを除去した。
アクリルアミド614mg、4−ビニルフェニルボロン酸142mgおよび2、2’−アゾビスイソブチロニトリル10mgをN、N’−ジメチルホルムアミド6mLに溶かした。以後、アルゴンガスまたは窒素ガスに1時間以上パージングした後、70℃で12時間以上撹拌した。以後、透析を通じて未反応物を除去して、第2高分子を製造した(図9を参照)。これを2重量%で含む水溶液(第2溶液)(pH10)を準備したことを除いて、実施例1と同じ方法で放射性セシウムを除去した。
アクリルアミドの代わりに、N、N−ジメチルアクリルアミドを使用し、第2溶液のpHを7.5で準備したことを除いて、実施例4と同じ方法で放射性セシウムを除去した。
放射性セシウムによる汚染表面(ペイント、アルミニウム、ステンレススチールおよびセメント)上にスプレーを利用して水を噴射して、放射性セシウムを除去した。
放射性セシウムによる汚染表面(ペイント、アルミニウム、ステンレススチールおよびセメント)上にスプレーを利用して0.1MのNH4Clを噴射して、放射性セシウムを除去した。
第1溶液において放射性セシウム除去用吸着剤として、韓国特許登録第10−1658475号の実施例1によって製造されたプルシアンブルーがコートされた磁性吸着剤0.5重量%を排除したことを除いて、実施例1と同じ方法で行った。
第1溶液において放射性セシウム除去用吸着剤として、韓国特許登録第10−1658475号の実施例1によって製造されたプルシアンブルーがコートされた磁性吸着剤0.5重量%の代わりに、0.1MのNH4Clを使用したことを除いて、実施例1と同じ方法で行った。
放射性セシウムによる汚染表面(ペイント、アルミニウム、ステンレススチールおよびセメント)上に市販のストリッパブルコート剤として、ディコンジェル(DeconGel)1101を処理して、放射性セシウムを除去した。
*DF=A0/Af
(Ao=放射性セシウム除去前の模擬汚染表面の放射性セシウム濃度、Af=放射性セシウム除去後の模擬汚染表面の放射性セシウム濃度)
Claims (6)
- (a)ヒドロキシ基を含む第1高分子を含有する第1溶液を準備する段階と、
(b)ボロン酸基が官能基として導入された第2高分子を含有する第2溶液を準備する段階と、
(c)放射性核種による汚染表面上に前記第1溶液および前記第2溶液をそれぞれ噴射または塗布した後、pH5〜12条件で脱水縮合反応を通じて前記第1高分子および前記第2高分子を互いに架橋結合させて、放射性核種が吸着されたハイドロゲルを形成させる段階とを含み、
(d)前記放射性核種が吸着されたハイドロゲルを水に沈漬させた後、ハイドロゲルのみを選択的に溶解させるか、または前記放射性核種が吸着されたハイドロゲルのpHを4以下に調節した後、ハイドロゲルのみを選択的に溶解させ、
前記第1溶液または前記第2溶液に放射性核種除去用吸着剤をさらに含有することを特徴とする、放射性核種の除去方法。 - 前記(a)段階で前記第1高分子は、 ポリビニルアルコール、アラビアガム、グアーガム、ローカストビーンガムおよびこれらの誘導体よりなる群から選択された一つ以上である、請求項1に記載の放射性核種の除去方法。
- 前記(b)段階で前記第2高分子は、カルボキシル基またはカルボニル基を含む骨格を含む、請求項1に記載の放射性核種の除去方法。
- 前記骨格は、アルギネート、ポリスクシンイミド、ポリメチルビニルエーテル−alt−マレイン酸無水物、ポリアクリル酸、ポリアクリルアミド、ポリ(N、N−ジメチルアクリルアミド)およびポリビニルピロリドンよりなる群から選択された一つ以上である、請求項3に記載の放射性核種の除去方法。
- 前記第1溶液または前記第2溶液に放射性核種とイオン交換可能なイオン交換体をさらに含む、請求項1に記載の放射性核種の除去方法。
- 前記(c)段階で放射性核種が吸着されたハイドロゲルの形成後、前記第2高分子と追加架橋結合するための1価、2価または3価イオン溶液をさらに噴射する、請求項1に記載の放射性核種の除去方法。
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