JP2015171757A - 表面ドーピング方法 - Google Patents
表面ドーピング方法 Download PDFInfo
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- JP2015171757A JP2015171757A JP2015085376A JP2015085376A JP2015171757A JP 2015171757 A JP2015171757 A JP 2015171757A JP 2015085376 A JP2015085376 A JP 2015085376A JP 2015085376 A JP2015085376 A JP 2015085376A JP 2015171757 A JP2015171757 A JP 2015171757A
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- Prior art keywords
- dopant
- metal
- growth factor
- titanium
- abrasive
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Abstract
Description
本出願は、その開示が参照により本明細書に組み込まれる2007年4月6日出願の米国仮出願60/910464の優先権を、米国特許法119条(e)に基づいて請求するものである。
金属表面を露出させるために、該金属基板の表面より金属酸化物を除去する工程と、
該基板の該表面にドーパントを浸透させるために、少なくとも1つの流動体ジェットからドーパントを含む粒子を該金属表面に供給する工程と、を含む。
1.表面の中及び表面の上の少なくとも何れかに、追加的な材料を供給するための、研磨性吹き付け工程。
2.不活性雰囲気において表面から酸化物層を除去する工程と、その表面が再び参加される前に行われる追加的な材料を表面の中又は表面の上に堆積する工程。
3.上記1.と2.の組合せ。
・形態/表面の形/形状/質感/粗度/微細構造(microstructure)
・表面の面積
・構造‐分子の組立の秩序/無秩序、包含、空き、及び編成
・結晶の結晶化度、サイズ、分布及び定位(orientation)
・化学
・科学的な組成
・元素組成
・元素の化学性
・分子組成
・官能基
・分子浸透層
・外因性の混入物及び不純物
・酸化物層の多孔性、厚さ、及び組成
・生化学
・生物的な性能
・表面エネルギー‐親油性/疎油性
・湿潤性‐親水性/疎水性
・吸着‐物理吸着及び化学吸着
・電気的性質‐表面電位及び表面電荷、絶対誘電率
・磁性
・光学的特性‐光学的反射/吸収
・表面の機械的な特性‐表面層の弾性/可塑性、表面における伸張力/圧縮力
・表面の動的性質‐原子及び分子の可動性。
・基板の素材及びその表面特性
・処理工程のパラメータ及び環境的な条件
・研磨剤及び、その物理的性質、化学的性質、サイズ、硬度、形態など
・ドーパントの素材及びその化学的性質、物理的性質、担体媒体であるか追加的な薬剤(例えば治療のため)であるか、活性か不活性か、合成物かコックテール混合物か。
・常温処理
・ドーパント素材の温度又は処理による劣化がない
・温度感性の薬物を破壊せずに表面に供給できる
・製造を容易にする一段階過程
・治療薬を運ぶために共形ポリマーフィルム(conformal polymer film)が必要でない
・ラミネート層が生じない‐欠けない、剥がれない
・特定の用途のためにインプラントに特殊処理を行うことに使われ得る
・医療用具の分野以外の産業部門においても用途がある(例えば航空宇宙産業、食品産業(チタンパイプの使用)、半導体産業などのチタンを使用する産業)。
例1
この例はHAをドーパント、アルミナビーズを研磨剤として用いて、チタニウムの基板を変性加工することを説明する。
この例はHAをドーパント、シリカビーズを研磨剤として用いて、チタニウムの基板を変性加工することを説明する。
この例はHA/ゲンタマイシンをドーパント、アルミナビーズを研磨剤として用いて、チタニウムの基板を変性加工することを説明する。
この例はHA/バンコマイシンをドーパント、アルミナビーズを研磨剤として用いて、チタニウムの基板を変性加工することを説明する。
この例はHA/トブラマイシンをドーパント、アルミナビーズを研磨剤として用いて、チタニウムの基板を変性加工することを説明する。
この例はHAのドーパント、そして異なるサイズ及び硬度の研磨剤を用いて、チタニウムの基板を変性加工することを説明する。
この例はツインノズル(twin nozzle)を用い、HAをドーパントとして1つの粒子ストリームで供給し、アルミナビーズを研磨剤として別の粒子ストリームで供給すると同時に、ブラスト加工のパラメータ及び研磨剤とドーパントに比率を調整しながらチタニウムの基板を変性加工することを説明する。
この例はHAをドーパント、アルミナビーズを研磨剤として用いて、ステンレス鋼の基板及びグレード2チタンの基板を変性加工することを説明する。
この例はナノ多孔性シリカをドーパント、アルミナビーズを研磨剤として用いて、チタ二ウムの基板を変性加工することを説明する。ナノ多孔性シリカは適切な薬物溶離担体として知られている。
この例は、ナノ多孔性HA(薬物溶離担体)をドーパント、アルミナビーズを研磨剤としてアルミニウム及びニチノールを変性加工することを説明する。
Claims (70)
- 金属基板を処理する方法であって、
金属表面を露出させるために、前記金属基板の表面より金属酸化物を除去する工程と、
前記基板の前記表面にドーパントを浸透させるために、少なくとも1つの流動体ジェットから前記ドーパントを含む粒子を前記金属表面に供給する工程と
を含むことを特徴とする方法。 - 前記除去工程は、不活性雰囲気において行われることを特徴とする請求項1に記載の方法。
- 前記除去工程は、前記供給工程と実質的に同時に行われ、その結果前記金属表面は前記供給工程以前には実質的に酸化されていないことを特徴とする請求項1に記載の方法。
- 前記除去工程は前記金属酸化物表面に研磨ブラスト加工を行う工程を含むことを特徴とする、請求項1記載の方法。
- 前記研磨ブラスト加工工程は、グリットブラスト加工、マイクロブラスト加工、ウォータージェットブラスト加工、及びショットピーニングから選ばれることを特徴とする請求項2に記載の方法。
- 前記研磨ブラスト加工工程は、前記ドーパントを含む粒子を供給する工程と同時に行われることを特徴とする請求項2に記載の方法。
- 前記除去工程は、ドリル加工、切断、成形、フライス加工、マイクロマシニング、スクラッチング、研削、磨き、及び研磨の少なくとも1つの工程から選ばれることを特徴とする請求項1に記載の方法。
- 前記除去工程は、酸エッチング、アルカリエッチング、及び過酸化水素処理の少なくとも1つの工程から選ばれることを特徴とする請求項1に記載の方法。
- 前記除去工程は、切除、マーキング/エッチング、溶接、切断、被覆から選ばれたレーザー処理を含むことを特徴とする請求項1に記載の方法。
- 前記除去工程は、エッチングと洗浄とから選ばれたプラズマ処理工程を含むことを特徴とする請求項1に記載の方法。
- 前記基板は、チタニウム、ステンレス鋼、アルミニウム、及びニチノールから選ばれることを特徴とする請求項1に記載の方法。
- 物体の表面を処理する方法であって、
前記物体の表面に前記ドーパントを浸透させるために、前記ドーパントを含む第1粒子セットと、研磨剤を含む第2粒子セットとを少なくとも1つの流動体ジェットから前記物体の表面に実質的に同時に供給する工程を含むことを特徴とする方法。 - 前記少なくとも1つの流動体ジェットは、湿式ブラスト加工装置、研磨のウォーター・ジェットピーニング装置、湿式ショットピーニング装置から選ばれることを特徴とする請求項1乃至12の何れかに記載の方法。
- 前記少なくとも1つの流動体ジェットは、乾式ショットピーニング装置、乾式ブラスト加工装置、輪形摩擦試験機、グリットブラスト加工装置、サンドブラスト加工装置、及びマイクロブラスト加工装置から選ばれることを特徴とする請求項1乃至13の何れかに記載の方法。
- 前記少なくとも1つの流動体ジェットは0.5〜100バールの圧力において作動することを特徴とする請求項1乃至14の何れかに記載の方法。
- 前記少なくとも1つの流動体ジェットは1〜30バールの圧力において作動することを特徴とする請求項1乃至15の何れかに記載の方法。
- 前記少なくとも1つの流動体ジェットは1〜10バールの圧力において作動することを特徴とする請求項1乃至16の何れかに記載の方法。
- 前記少なくとも1つの流動体ジェットは0.5〜100バールの圧力において作動することを特徴とする請求項1乃至17の何れかに記載の方法。
- 前記少なくとも1つの流動体ジェットは1〜30バールの圧力において作動することを特徴とする請求項1乃至18の何れかに記載の方法。
- 前記少なくとも1つの流動体ジェットは3〜10バールの圧力において作動することを特徴とする請求項1乃至19の何れかに記載の方法。
- 前記物体は金属であることを特徴とする請求項12乃至20の何れかに記載の方法。
- 前記金属は、純金属、金属合金、1つ又は複数の相を含む金属間物、非晶相を含む金属間物、単独の結晶相を含む金属間物、多結晶相を含む金属間物から選ばれることを特徴とする請求項21に記載の方法。
- 前記金属は、チタニウム、チタン合金、鉄合金、ステンレス鋼、ステンレス鋼合金、炭素鋼、炭素鋼合金、アルミニウム、アルミ合金、ニッケル、ニッケル合金、ニッケルチタン合金、タンタラム、タンタル合金、ニオビウム、ニオブ合金、クロミウム、クロム合金、コバルト、コバルト合金、貴金属、及び貴金属合金から選ばれることを特徴とする請求項21又は22に記載の方法。
- 前記金属は、チタニウム、アルミニウム、ステンレス鋼、及びニチノールから選ばれることを特徴とする請求項12乃至23の何れかに記載の方法。
- 前記物体は移植できる医療用具であることを特徴とする請求項1乃至24の何れかに記載の方法。
- 前記物体は、病的な石灰化を除去するために使用される、カテーテル、ガイドワイヤ、バスケットから選ばれることを特徴とする請求項1乃至25の何れかに記載の方法。
- 前記粒子は気体の担体流動体に含まれて供給されることを特徴とする請求項1乃至26の何れかに記載の方法。
- 前記担体流動体は、窒素、水素、アルゴン、ヘリウム、空気、エチレンオキシド、及びそれらの組合せから選ばれることを特徴とする請求項27に記載の方法。
- 前記粒子は液体の担体流動体に含まれて供給されることを特徴とする請求項1乃至28の何れかに記載の方法。
- 前記液体はエッチング液体でもあることを特徴とする請求項29に記載の方法。
- 前記エッチング液体は塩基性であることを特徴とする請求項30に記載の方法。
- 前記エッチング液体は酸性であることを特徴とする請求項30に記載の方法。
- 前記供給工程は不活性環境において行われることを特徴とする請求項12乃至32の何れかに記載の方法。
- 前記研磨剤は、シリカ、アルミナ、ジルコニア、チタン酸バリウム、チタン酸カルシウム、チタン酸ナトリウム、酸化チタン、ガラス、生体適合性ガラス、ダイヤモンド、炭化ケイ素、リン酸カルシウム、炭酸カルシウム、金属粉、金属線、炭素繊維複合材、ポリマー、ポリマー複合材、チタニウム、ステンレス鋼、硬化鋼、及びクロム合金から選ばれることを特徴とする請求項4乃至6及び請求項12乃至33の何れかに記載の方法。
- 前記研磨剤は、モース硬度が0.1〜10であることを特徴とする請求項4乃至6及び請求項12乃至34の何れかに記載の方法。
- 前記研磨剤は、モース硬度が1〜10であることを特徴とする請求項4乃至6及び請求項12乃至34の何れかに記載の方法。
- 前記研磨剤は、モース硬度が5〜10であることを特徴とする請求項4乃至6及び請求項12乃至34の何れかに記載の方法。
- 前記研磨剤は、その粒径が0.1〜10000μmであることを特徴とする請求項4乃至6及び請求項12乃至37の何れかに記載の方法。
- 前記研磨剤は、その粒径が1〜5000μmであることを特徴とする請求項4乃至6及び請求項12乃至37の何れかに記載の方法。
- 前記研磨剤は、その粒径が10〜1000μmであることを特徴とする請求項4乃至6及び請求項12乃至37の何れかに記載の方法。
- 前記ドーパントは、ポリマー、金属、セラミック、及びそれらの組合せから選ばれることを特徴とする請求項1乃至40の何れかに記載の方法。
- 前記ドーパントは、2つ以上の異なる材料を含むことを特徴とする請求項1乃至41の何れかに記載の方法。
- 前記ドーパントは金属酸化物であることを特徴とする請求項1乃至42の何れかに記載の方法。
- 前記ドーパントは、チタン酸バリウム、チタン酸カルシウム、チタン酸ナトリウム、ゼオライト、ケイ質のゼオライト、リンを含むゼオライト、シリカ、アルミナ、ジルコニア、炭酸カルシウム、生体適合性ガラス、リン酸カルシウムガラス、及び二酸化チタンから選ばれることを特徴とする請求項1乃至43の何れかに記載の方法。
- 前記ドーパントは骨伝導性物質又は骨統合性物質であることを特徴とする請求項1乃至44の何れかに記載の方法。
- 前記骨伝導性物質又は骨統合性物質は変性されたリン酸カルシウムであることを特徴とする請求項45に記載の方法。
- 前記骨伝導性物質又は骨統合性物質はCa5(PO4)3OH、CaHPO4・2H2O、CaHPO4、Ca8H2(PO4)6・5H2O、α‐Ca3(PO4)2、β‐Ca3(PO4)2、及びそれらの組合せから選ばれることを特徴とする請求項45又は46に記載の方法。
- 前記変性されたリン酸カルシウムは、炭酸アニオン、塩素アニオン、フッ素アニオン、ケイ酸アニオン、及びアルミン酸アニオンから選ばれる少なくとも1つのアニオンを含むことを特徴とする請求項46又は47に記載の方法。
- 前記変性されたリン酸カルシウムは、陽子、カリウムカチオン、ナトリウムカチオン、マグネシウムカチオン、バリウムカチオン、及びストロンチウムカチオンから選ばれる少なくとも1つのカチオンを含むことを特徴とする請求項46乃至48の何れかに記載の方法。
- 前記ドーパントは治療薬であることを特徴とする請求項1乃至49の何れかに記載の方法。
- 前記治療薬は担体材料の表面上又は担体材料の中に固定されることを特徴とする請求項50に記載の方法。
- 前記担体材料は、ポリマー、リン酸カルシウム、二酸化チタン、シリカ、バイオポリマー、生体適合性ガラス、ゼオライト、脱塩骨、脱タンパク骨、同種移植骨、及びそれらの複合組合せから選ばれることを特徴とする請求項51に記載の方法。
- 前記ポリマーは、ポリウレタン、ポリエチレンテプタレート、PLLA‐ポリグリコール酸(PGA)共重合体(PLGA)、ポリカプロラクトン、ポリ‐(ヒドロキシ酪酸塩/ヒドロキシ吉草酸塩)共重合体、ポリ(ビニルピロリドン)、ポリテトラフルオロエチレン、ポリ(2−メタクリル酸ヒドロキシエチル)、ポリ(エーテルウレタン尿素)、シリコーン、アクリル、エポキシド、ポリエステル、ウレタン、パーレン、ポリホスファゼンのポリマー、フッ素ポリマー、ポリアミド、ポリオレフィン、及びこれらの混合物及び共重合体から選ばれることを特徴とする請求項52に記載の方法。
- 前記バイオポリマーは、多糖類、ゼラチン、コラーゲン、アルギン酸塩、ヒアルロン酸、アルギン酸、カラギーナン、コンドロイチン、ペクチン、キトサン、及びそれらの誘導体、混合物、共重合体から選ばれることを特徴とする請求項52に記載の方法。
- 前記治療薬は、抗癌剤、抗炎症薬、免疫抑制剤、抗生物質、ヘパリン、機能タンパク質、調節タンパク質、構造タンパク質、オリゴペプチド、抗原ペプチド、核酸、免疫原、及びそれらの組合せから選ばれることを特徴とする請求項51に記載の方法。
- 前記抗癌剤は、アシビシン、アクラルビシン、アコダゾール、アクロナイシン、アドゼレシン、アラノシン、アルデスロイキン、アロプリノール・ナトリウム、アルトレタミン、アミノグルテチミド、アモナフィド、アンプリジェン、アムサクリン、アンドロゲン、アングイジン、グリシン酸アフィディコリン、アサレイ、アスパラギナーゼ、5−アザシチジン、アザチオプリン、カルメット・ゲラン菌(BCG)、ベイカーのアンチフォル(可溶性)、β−2'−デオキシチオグアノシン、塩酸ビスアントレン、硫酸ブレオマイシン、ブスルファン、ブチオニンスルフォキシミン、BWA 773U82,BW 502U83.HCl,メシル酸BW 7U85、セラセミド、カルベチマー、カルボプラチン、カルムスチン、クロラムブシル、クロロキノキサリン−スルホンアミド、クロロゾトシン、クロモマイシンA3、シスプラチン、クラドリビン、コルチコステロイド、コリネバクテリリウム・パルバム、CPT−11、クリスナトール、サイクロシチジン、シクロホスファミド、シタラビン、シテムベナ、ダビスマレアート、ダカルバジン、ダクチノマイシン、塩酸ダウノルビシン、デアザウリジン、デクスラゾキサン、ジアンヒドロガラクチトール、ジアジクオン、ジブロモズルシトール、ジデムニンB、ジエチルジチオカルバマート、ジグリコアルデヒド、ジヒドロ‐5‐アザシチジン、ドキソルビシン、エキノマイシン、エダトレキサート、エデルフォシン、エフロルニチン、エリオットの溶液、エルサミトルシン、エピルビシン、エソルビシン、エストラムスチンホスファート、エストロゲン、エタニダゾール、エチオホス、エトポシド、ファドラゾール、ファザラビン、フェンレチニド、フィルグラスチム、フィナステリド、フラボン酢酸、フロクスウリジン、リン酸フルダラビン、5−フルオロウラシル、フルオゾール(登録商標)、フルタミド、硝酸ガリウム、ゲムシタビン、酢酸ゴセレリン、ヘプスルファム、ヘキサメチレンビスアセトアミド、ホモハリングトニン、硫酸ヒドラジン、4−ヒドロキシアンドロステンジオン、ヒドロキシ尿素、塩酸イダルビシン、イホスファミド、インターフェロンα、インターフェロンβ、インターフェロンγ、インターロイキン−1αおよびインターロイキン−1β、インターロイキン−3、インターロイキン−4、インターロイキン−6、4−イポメアノール、イプロプラチン、イソトレチノイン、ロイコボリンカルシウム、酢酸ロイプロリド、レバミソール、リポゾーマル・ダウノルビシン、リポソームカプセル化ドキソルビシン、ロムスチン、ロニダミン、メイタンシン、塩酸メクロレタミン、メルファラン、メノガリル、メルバロン、6−メルカプトプリン、メスナ、カルメット・ゲラン菌のメタノール抽出残渣、メトトレキサート、N−メチルホルムアミド、ミフェプリストン、ミトグアゾン、マイトマイシン−C、ミトタン、塩酸ミトキサントロン、単球/マクロファージ・コロニー刺激因子、ナビロン、ナホキシジン、ネオカルチノスタチン、酢酸オクトレオチド、オルマプラチン、オキサリプラチン、パクリタキセル、パーラ、ペントスタチン、ピペラジンジオン、ピポブロマン、ピラルビシン、ピリトレキシム、塩酸ピロキサントロン、PIXY-321、プリカマイシン、ポルフィマーナトリウム、プレドニムスチン、プロカルバジン、プロゲスチン、ピラゾフリン、ラゾキサン、サルグラモスチム、セムスチン、スピロゲルマニウム、スピロムスチン、ストレプトニグリン、ストレプトゾシン、スロフェヌル、スラミン・ナトリウム、タモキシフェン、タキソテール、テガフル、テニポシド、テレフタルアミジン、テロキシロン、チオグアニン、チオテパ、チミジン・インジェクション、チアゾフリン、トポテカン、トレミフェン、トレチノイン、塩酸トリフルオペラジン、トリフルリジン、トリメトレキサート、腫瘍壊死因子、ウラシル・マスタード、硫酸ビンブラスチン、硫酸ビンクリスチン、ビンデシン、ビノレルビン、ビンゾリジン、ヨシ−864、ゾルビシン、及びそれらの混合物から選ばれることを特徴とする請求項55に記載の方法。
- 前記抗炎症薬は、非ステロイド性抗炎症薬、COX−2阻害剤、グルココルチコイド、及びそれらの混合物から選ばれることを特徴とする請求項55に記載の方法。
- 前記非ステロイド性抗炎症薬は、アスピリン、ジクロフェナク、インドメタシン、スリンダク、ケトプロフェン、フルルビプロフェン、イブプロフェン、ナプロキセン、ピロキシカム、テノキシカム、トルメチン、ケトロラク、オキサプロシン、メフェナム酸、フェノプロフェン、ナブメトン、アセトアミノフェン、及びそれらの混合物から選ばれることを特徴とする請求項57に記載の方法。
- 前記COX−2阻害剤は、ニメスリド、NS−398、フロスリド、L−745337、セレコキシブ、ロフェコキシブ、SC−57666、DuP−697、パレコキシブナトリウム、JTE−522、バルデコキシブ、SC−58125、エトリコキシブ、RS−57067、L−748780、L−761066、APHS、エトドラク、メロキシカム、S−2474、及びそれらの混合物から選ばれることを特徴とする請求項57に記載の方法。
- 前記グルココルチコイドは、ヒドロコルチゾン、コルチゾン、プレドニゾン、プレドニゾロン、メチルプレドニゾロン、メプレドニゾン、トリアムシノロン、パラメタゾン、フルプレドニソロン、ベータメタゾン、デキサメタゾン、フルドロコルチゾン、デゾキシコルチコステロン、及びそれらの混合物から選ばれることを特徴とする請求項57に記載の方法。
- 前記抗生物質は、トブラマイシン、バンコマイシン、ゲンタマイシン、アンピシリン、ペニシリン、セファロスポリンC、セファレキシン、セファクロール、セファマンドール、シプロフロキサシン、及びそれらの混合物から選ばれることを特徴とする請求項55に記載の方法。
- 前記タンパク質は、アルブミン、カゼイン、ゼラチン、リソソーム、フィブロネクチン、フィブリン、キトサン、ポリリシン、ポリアラニン、ポリシステイン、骨形成タンパク質(BMP)、上皮細胞増殖因子(EGF)、線維芽細胞増殖因子(bFGF)、神経成長因子(NGF)、骨由来増殖因子(BDGF)、形質転換成長因子‐.ベータ.1(TGF−.ベータ.1)、形質転換成長因子‐.ベータ.(TGF−.ベータ.)、アルギニン‐グリシン‐アスパラギン酸のトリペプチド(RGD)、ビタミンD3、デキサメタゾン、ヒト成長ホルモン(hGH)、上皮細胞増殖因子、形質転換成長因子α、形質転換成長因子β、ワクチニア成長因子、線維芽細胞増殖因子、インスリン様成長因子、血小板由来増殖因子、軟骨由来増殖因子、インターロイキン−2、神経成長因子、造血細胞成長因子、リンパ球増殖因子、骨形成タンパク質、骨形成因子、軟骨形成因子、及びそれらの混合物から選ばれる請求項55に記載の方法。
- 前記へパリンは、組み換えへパリン、へパリン誘導体、へパリン類似物又はそれらの組合せから選ばれることを特徴とする請求項55に記載の方法。
- 前記オリゴペプチドは殺菌性のオリゴペプチドであることを特徴とする請求項55に記載の方法。
- 前記免疫原は、ウイルス抗原、細菌性抗原、真菌抗原、寄生虫抗原、腫瘍抗原、腫瘍抗原のペプチド断片、転移特異的抗原、能動又は受動ワクチン、合成ワクチン、又はサブユニット・ワクチンであることを特徴とする請求項55に記載の方法。
- 前記ドーパントは放射線不透性材料であることを特徴とする請求項1乃至51の何れかに記載の方法。
- 前記放射線不透性材料は、アルカリ土類金属、遷移金属、希土類金属、酸化物、硫酸塩、リン酸塩、及びそれらの組合せから選ばれることを特徴とする請求項66に記載の方法。
- 前記放射線不透性材料はポリマーであることを特徴とする請求項66に記載の方法。
- 前記第1粒子セットと前記第2粒子セットは同じ流動体ジェットから前記表面に供給されることを特徴とする請求項1乃至68の何れかに記載の方法。
- 前記第1粒子セットと前記第2粒子セットは別々の流動体ジェットから前記表面に供給されることを特徴とする請求項1乃至69の何れかに記載の方法。
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IL197430A (en) | 2014-01-30 |
US20150079286A1 (en) | 2015-03-19 |
JP2013136148A (ja) | 2013-07-11 |
AU2007296573A1 (en) | 2008-03-20 |
WO2008033867A2 (en) | 2008-03-20 |
US8119183B2 (en) | 2012-02-21 |
CA2663036A1 (en) | 2008-03-20 |
EP2061629A2 (en) | 2009-05-27 |
USRE45877E1 (en) | 2016-02-02 |
EP2061629B1 (en) | 2011-05-18 |
KR101494909B1 (ko) | 2015-02-23 |
US9695505B2 (en) | 2017-07-04 |
JP2010502468A (ja) | 2010-01-28 |
US9242268B2 (en) | 2016-01-26 |
US20120114830A1 (en) | 2012-05-10 |
KR20090106449A (ko) | 2009-10-09 |
JP5784053B2 (ja) | 2015-09-24 |
US20150190841A1 (en) | 2015-07-09 |
US8889212B2 (en) | 2014-11-18 |
US20080274671A1 (en) | 2008-11-06 |
JP6069401B2 (ja) | 2017-02-01 |
US9034422B2 (en) | 2015-05-19 |
IL197430A0 (en) | 2009-12-24 |
AU2007296573B2 (en) | 2013-01-17 |
US20160168690A1 (en) | 2016-06-16 |
CA2663036C (en) | 2016-06-21 |
WO2008033867A3 (en) | 2008-06-19 |
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