EFRI E3P: Tuning Catalyst Design to Recycle Mixed Polymer Streams

EFRI E3P：调整催化剂设计以回收混合聚合物流

• 批准号: 2029394
• 负责人: Steven Crossley
• 金额: $ 200万
• 依托单位: University of Oklahoma Norman Campus
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-01-01 至 2024-12-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2029394&HistoricalAwards=false
• 关键词: EFRI; E3P; Tuning; Catalyst; Design

This project aims to develop a new approach to upgrade and recycle multilayer polymer films. Multilayer films generally perform better and require much less plastic material in applications such as packaging, but their complexity makes them far more challenging to recycle than other simpler forms of plastic like rigid bottles. The investigators in this project aim to develop catalysts that selectively target and convert components of the multilayer films, allowing the remaining polymer to be recycled using conventional methods. This catalytic targeting will be accomplished by modifying the surface of several promising catalyst supports and incorporating active sites on their surface to allow selective targeting and conversion of polymers or impurities of interest. Three families of catalysts will be evaluated based on their effectiveness for targeting and converting the components of interest, ease of separation from the multilayer polymer mixture, and effective re-use. A model will be constructed to determine the cost-effectiveness of each approach to refocus efforts on families of catalysts that exhibit the greatest potential for economically recycling multilayer films. The scientific and engineering research will be accompanied by public perception surveys and education interventions aimed at communicating the importance of this problem to the general public and thereby increasing public awareness, acceptance, and participation. Ultimately, this proposal will lay the groundwork for the cost-effective recycling of more advanced multilayered plastics. This will ideally enable the technological advantages that accompany multilayer plastics such as longer food shelf lives without sacrificing the ability to effectively recycle the plastics involved.Because multilayer films typically consist of very diverse sets of polymers, as well as trace amounts of tie layers, they are not compatible with traditional recycling technologies focused on a specific chemistry. Common approaches for their conversion are delamination or dissolution-precipitation using costly solvent-based processes that can easily become cost prohibitive when multiple streams are present. This proposal aims to develop a set of catalytic particles that target specific families of polymers in these multi-component films such that the nonpolar residue can be readily recycled. Polar polymers will be selectively targeted by manipulating external functional groups on three families of catalysts - carbon nanotubes, silica particles, and zeolites. These families are chosen based on their ease of introducing surface functionalities, effectiveness in targeting molten polymers, recovery, and regeneration after conversion of polar components. The team will further test the hypothesis that trace amounts of added water can serve to remotely activate some polar molecules through remote polarization and protonation, further extending the rates and selectivity activation of polar molecules in these blends. Resulting kinetic data will be incorporated into a techno-economic model to compare this approach with solvent-based approaches. This technical component of the research will be carried out in parallel with public perception surveys to guide improved public education regarding the importance of this problem, with this information being incorporated into the team’s outreach efforts. Outreach activities involving middle and high school students will be developed, while also creating research opportunities for undergraduate and graduate students spanning the diverse fields of Chemical Engineering and Psychology.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

该项目旨在开发一种升级和回收多层聚合物薄膜的新方法。多层薄膜通常在包装等应用中表现更好，并且需要更少的塑料材料，但其复杂性使得它们比其他更简单形式的塑料（如硬质瓶子）回收更具挑战性。该项目的研究人员旨在开发能够选择性地靶向和转化多层薄膜成分的催化剂，从而允许使用传统方法回收剩余的聚合物。这种催化靶向将通过修饰几种有前途的催化剂载体的表面并在其表面上掺入活性位点来实现，以允许选择性靶向和转化感兴趣的聚合物或杂质。将根据其靶向和转化感兴趣组分的有效性、从多层聚合物混合物中分离的难易程度以及有效的再利用来评估三类催化剂。将构建一个模型来确定每种方法的成本效益，以便将工作重点重新集中在具有经济回收多层薄膜潜力的催化剂系列上。科学和工程研究将伴随公众认知调查和教育干预，旨在向公众传达这一问题的重要性，从而提高公众的认识、接受度和参与度。最终，该提案将为更先进的多层塑料的经济高效回收奠定基础。这将理想地实现多层塑料的技术优势，例如更长的食品保质期，而不会牺牲有效回收所涉及塑料的能力。由于多层薄膜通常由非常多样化的聚合物组以及微量的连接层组成，因此它们与专注于特定化学物质的传统回收技术不兼容。其转化的常见方法是使用昂贵的溶剂型工艺进行分层或溶解沉淀，当存在多个流时，这些工艺很容易变得成本过高。该提案旨在开发一套催化颗粒，针对这些多组分薄膜中的特定聚合物族，以便非极性残留物可以轻松回收。通过操纵三类催化剂（碳纳米管、二氧化硅颗粒和沸石）上的外部官能团，将选择性地靶向极性聚合物。选择这些家族的依据是它们引入表面功能的容易程度、靶向熔融聚合物的有效性、极性组分转化后的回收和再生。该团队将进一步测试这一假设，即微量添加的水可以通过远程极化和质子化来远程激活一些极性分子，进一步提高这些混合物中极性分子的激活速率和选择性。所得的动力学数据将被纳入技术经济模型中，以将该方法与基于溶剂的方法进行比较。该研究的技术部分将与公众认知调查同时进行，以指导改善公众对这一问题重要性的教育，并将这些信息纳入团队的外展工作中。将开展涉及中学生和高中生的外展活动，同时也为化学工程和心理学各个领域的本科生和研究生创造研究机会。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Effect of Water on Cumene Dealkylation over H-ZSM-5 Zeolites

水对 H-ZSM-5 沸石上异丙苯脱烷基的影响

• DOI: 10.1021/acscatal.2c05759
• 发表时间: 2023
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: Chau, Han K.;Mai, Hien D.;Gumidyala, Abhishek;Pham, Tram N.;Bui, Dai-Phat;D’Amico, Andrew D.;Alalq, Ismaeel;Glatzhofer, Daniel T.;White, Jeffery L.;Crossley, Steven P.
• 通讯作者: Crossley, Steven P.

Role of Water on Zeolite-Catalyzed Dehydration of Polyalcohols and EVOH Polymer

水在沸石催化多元醇和 EVOH 聚合物脱水中的作用

• DOI: 10.1021/acscatal.2c05303
• 发表时间: 2023
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: Chau, Han K.;Nguyen, Quy P.;Jerdy, Ana Carolina;Bui, Dai-Phat;Lobban, Lance L.;Wang, Bin;Crossley, Steven P.
• 通讯作者: Crossley, Steven P.

Shifts in catalyst deactivation mechanisms as a function of surface coverage during Friedel-Crafts acylation in zeolites

沸石傅克酰化过程中催化剂失活机制随表面覆盖度的变化

• DOI: 10.1016/j.jcat.2023.07.009
• 发表时间: 2023
• 期刊: Journal of Catalysis
• 影响因子: 7.3
• 作者: Alalq, Ismaeel;Nguyen-Phu, Huy;Crossley, Steven
• 通讯作者: Crossley, Steven

Development of an objective measure of knowledge of plastic recycling: The outcomes of plastic recycling knowledge scale (OPRKS)

制定塑料回收知识的客观衡量标准：塑料回收知识量表（OPRKS）的结果

• DOI: 10.1016/j.jenvp.2023.102143
• 发表时间: 2023
• 期刊: Journal of Environmental Psychology
• 影响因子: 6.9
• 作者: Holt, Jenna R.;Bui, Dai-Phat;Chau, Han;Wang, Kathy;Trevisi, Luis M.;Jerdy, Ana Carolina;Lobban, Lance;Crossley, Steven;Feltz, Adam
• 通讯作者: Feltz, Adam