Novel Polyisobutylene-Based Materials and Surfaces; Enzyme-Catalyzed Functionalization and ?Modular? Surface Construction

新型聚异丁烯基材料和表面；

• 批准号: 0804878
• 负责人: Judit Puskas
• 金额: $ 47万
• 依托单位: University of Akron
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2008
• 资助国家: 美国
• 起止时间: 2008-05-15 至 2016-01-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0804878&HistoricalAwards=false
• 关键词: Novel; Polyisobutylene; Based; Materials; Surfaces

TECHNICAL SUMMARY:This award, co-funded by the Division of Materials Research and the Office of International Science and Engineering, aims at the synthesis and characterization of novel self-assembling nanostructured thermoplastic elastomeric (TPE) biomaterials based on polyisobutylene (PIB). Specifically, efforts to synthesize new "Entropy-driven" TPEs (ENTPE) will continue. Under the current NSF support it was discovered that the dendritic (arborescent or tree-like) arbPIB midblock of ENTPEs facilitates phase separation and TPE behavior even with very short plastic and elastomeric end blocks. These novel ENTPE materials were further reinforced with nano-size fillers (carbon and silica) to yield strong rubbery nanocomposites (ENTPEC), and their biocompatibility was demonstrated in vitro and in vivo in rabbits. Based on this discovery, new ENTPEs will be synthesized with short end blocks, capable of hydrogen bonding (e.g., polypeptides). Compounding these materials with nanofillers will yield new ENTPEC nanocomposites. In order to control surface chemistry and patterning for improved tissue integration, a new "modular" approach using ElectroNanoSprayingTM is proposed, which allows the construction of gradient surfaces with various chemistries and topologies. Spraying ENTPE onto the surface of ENTPEC will yield well-controlled nanopatterns of the same chemistry. Surface chemistry will be controlled by spraying low molecular weight (MW) functionalized PIBs (PIB-F) where F is a biologically active compound (nucleic acid base, peptide, protein, etc.) onto the surface of ENTPECs. The PIB-Fs will be precision synthesized from PIB-OH made by living carbocationic polymerization and functionalized using a novel enzyme-catalyzed transesterification process that yields complete conversion under mild conditions this also emerged from the current grant. The "modular" approach will give unprecedented control over surface chemistry and surface patterning independently, and will contribute to new fundamental understanding of the effects of surface properties on the biocompatibility of polymeric materials. NON-TECHNICAL SUMMARY:This project is aimed at the synthesis and characterization of novel biomaterials based on polyisobutylene (PIB). These materials are soft and transparent like silicone rubber, but self-assemble into a network without any chemical treatment which is necessary to make silicone rubber. In 2004, one PIB-based material was FDA-approved as the coating on drug-eluting coronary stents. More than a million of those stents have been implanted into patients, saving lives. The proposed new materials will have improved combination of properties. In addition, a new approach to surface modification to improve biocompatibility will be tested in this project. For this goal new polymers will be synthesized via "green polymer chemistry" using enzymes as catalysts, and sprayed to the surface of the novel biomaterials. This new "modular" approach will give independent control over surface chemistry and patterning, providing unprecedented insight into the effect of these properties on biocompatibility. The new materials may replace silicone rubber in certain applications (for example, as the shell of breast implants where impermeability is required). This project is interdisciplinary, building on collaborators (Nanocopoeia Inc. Minnesota, BioMedical Research Associates Akron, the University of Washington, Pomeranian Medical Academy of Poland, University of Bordeaux, France). It is complementary to a recently approved grant by German Research Foundation (DFG) as well as the grant approved by the Polish Ministry of Science and Education, to test various properties of the new biomaterials. The grant will support 1 partial female Post-doctoral fellow (Nanocopoeia's NSF grant will complement this to full time), four Ph. D. students (3 Americans - two of them females, one Hispanic), future REU (Research Experience for Undergraduates) students, an RET (Research Experience for Teachers), and high school students. It will also support international student exchanges and project meetings directly, and international students indirectly. The project will expose students to a great variety of scientific disciplines (polymer chemistry, organic chemistry, material science, biochemistry, surface science, polymer engineering, biomedical engineering, proteomics etc.). They will also have a chance to carry out part of their research in Germany, Poland and Ireland. Exposure to different cultures, organizations and work ethics will prepare the students to work better in the global economy, making them more attractive to potential employers. We will also embark on a new program connecting science and art, in collaboration with the Myers School of Art at the University of Akron to broaden the horizon for students of both disciplines.

该奖项由材料研究部和国际科学与工程办公室共同资助，旨在合成和表征基于聚异丁烯（PIB）的新型自组装纳米结构热塑性弹性体（TPE）生物材料。 具体而言，将继续努力合成新的“熵驱动”TPE（ENTPE）。在当前NSF的支持下，发现ENTPE的树枝状（树枝状或树状）arbPIB中间嵌段促进相分离和TPE行为，即使具有非常短的塑性和弹性体端嵌段。 这些新的ENTPE材料进一步加强与纳米尺寸的填料（碳和二氧化硅），以产生强橡胶纳米复合材料（ENTPEC），并证明其生物相容性在体外和体内的兔子。基于这一发现，新的ENTPE将被合成为具有短末端嵌段，能够形成氢键（例如，多肽）。将这些材料与纳米填料混合将产生新的ENTPEC纳米复合材料。为了控制表面化学和图案化以改善组织整合，提出了一种使用ElectroNanoSprayingTM的新的“模块化”方法，该方法允许构建具有各种化学和拓扑结构的梯度表面。将ENTPE喷涂到ENTPEC的表面上将产生具有相同化学性质的良好控制的纳米颗粒。 通过喷涂低分子量（MW）功能化PIB（PIB-F）控制表面化学，其中F是生物活性化合物（核酸碱基、肽、蛋白质等）。在ENTPEC的表面上。PIB-Fs将由活性碳阳离子聚合制成的PIB-OH精确合成，并使用新型酶催化酯交换过程进行官能化，该过程在温和条件下产生完全转化，这也是目前的资助。“模块化”的方法将提供前所未有的控制表面化学和表面图案独立，并将有助于新的基本理解的表面性能对聚合物材料的生物相容性的影响。 非技术总结：该项目旨在合成和表征基于聚异丁烯（PIB）的新型生物材料。这些材料像硅橡胶一样柔软透明，但自组装成网络，而无需任何化学处理，这是制造硅橡胶所必需的。2004年，一种基于PIB的材料被FDA批准作为药物洗脱冠状动脉支架的涂层。超过100万个这样的支架已经被植入病人体内，挽救了生命。所提出的新材料将具有改进的性能组合。此外，本项目还将测试一种新的表面改性方法，以改善生物相容性。为了实现这一目标，将通过“绿色聚合物化学”，使用酶作为催化剂合成新的聚合物，并喷涂到新型生物材料的表面。这种新的“模块化”方法将对表面化学和图案化进行独立控制，为这些特性对生物相容性的影响提供前所未有的见解。在某些应用中，新材料可能会取代硅橡胶（例如，作为乳房植入体的外壳，要求不渗透）。该项目是跨学科的，建立在合作者（Nanocoptosis Inc.明尼苏达州，阿克伦生物医学研究协会，华盛顿大学，波兰波美拉尼亚医学院，法国波尔多大学）。它是德国研究基金会（DFG）最近批准的赠款以及波兰科学和教育部批准的赠款的补充，用于测试新生物材料的各种特性。该补助金将支持1名部分女性博士后研究员（Nanococopy的NSF补助金将补充这一全职），4名博士。学生（3名美国人-其中两名女性，一名西班牙裔），未来REU（本科生研究经验）的学生，RET（教师研究经验）和高中生。它还将直接支持国际学生交流和项目会议，并间接支持国际学生。该项目将使学生接触到各种科学学科（高分子化学，有机化学，材料科学，生物化学，表面科学，聚合物工程，生物医学工程，蛋白质组学等）。他们还将有机会在德国、波兰和爱尔兰进行部分研究。接触不同的文化，组织和职业道德将使学生在全球经济中更好地工作，使他们对潜在雇主更具吸引力。我们还将与阿克伦大学迈尔斯艺术学院合作，开展一项连接科学和艺术的新计划，以拓宽这两个学科学生的视野。