Manufacturing USA: GOALI: Designing Catalytic Membrane Reactors (CMRs) for Low Temperature CO2 Utilization and Methane Dry Reforming

随着大多数电力生产持续依赖化石燃料以及对二氧化碳排放的日益关注，通过甲烷（其在美国丰富）的干重整用于合成气生产的二氧化碳利用率越来越高。已经成为一个非常有吸引力的可能性。该项目的目标是设计高性能的催化膜反应器（CMR）的甲烷低温干重整（DRM）使用可加工的聚合物为基础的膜，并建立在这个过程中的二氧化碳转化，碳沉积和催化活性的选择性氢去除的影响的理解。该GOALI项目将得到一个重要的行业合作伙伴（Gas Technology Institute，GTI）的支持，一名研究生将在GTI实习，以评估工业环境中的CMR。该项目直接涉及美国能源部资助的快速推进过程强化部署（RAPID）研究所的一个重点领域，通过过程强化实现节能制造。拟议的研究计划旨在设计，制备和表征在低温下具有高活性的抗积炭催化剂，以及在聚苯并咪唑（PBI）中含有Pd纳米材料的混合基质材料（MMM），其具有上级的H2/CO2分离性能。这些催化剂随后将被整合到遗留集束弹药中，并在实验室规模上进行测试。将开发模型来描述选择性除氢对DRM反应的影响。本论文的创新之处主要体现在三个方面：（1）采用独特的火焰气溶胶工艺，设计并制备了具有良好低温活性和抗结焦性能的DRM纳米催化剂;（2）使用热稳定的、可加工的聚合物基膜开发用于低温DRM的CMR，以及（3）了解在低温下选择性脱除H2对DRM反应的影响（包括CO2转化、积碳和催化活性）。 将为DRM反应制备基于中空纤维的CMR并进行彻底表征;将开发预测模型以揭示材料和操作参数对CO2转化的影响;将针对低温贫氢条件优化催化剂;并将进行初步技术经济分析，从而更全面地了解CMR用于DRM反应的潜力。参与该计划的研究生和本科生将接触到反应工程，分离和材料科学的跨学科研究。研究结果将纳入布法罗大学的课程、一本受欢迎的教科书和方便用户的教学单元。外展活动将为来自布法罗地区代表性不足的群体的高中生和本科生提供教育模块和研究培训，并激励他们追求STEM职业。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。

With continued reliance on fossil fuels for most electricity production and increasing concerns about carbon dioxide emissions, carbon dioxide utilization for syngas production via dry reforming of methane (which is abundant in the U.S.) has become a very attractive possibility. The objectives of the proposed project are to design high performance catalytic membrane reactors (CMRs) for low temperature dry reforming of methane (DRM) using processible polymer-based membranes, and to build understanding of the effects of selective hydrogen removal on carbon dioxide conversion, carbon deposition and catalytic activity in this process. This GOALI project will be supported by a key industry partner (Gas Technology Institute, GTI), with one graduate student serving as an intern at GTI to evaluate the CMRs in an industrial setting. This project directly addresses a focus area of the DOE-funded Rapid Advancement in Process Intensification Deployment (RAPID) Institute through process intensification for energy-efficient manufacturing.The proposed research plan aims to design, prepare and characterize coke resistant catalysts with high activity at low temperatures, and mixed matrix materials (MMMs) containing Pd nanomaterials in polybenzimidazole (PBI) with superior H2/CO2 separation performance. The catalysts will be subsequently integrated in CMRs and tested at laboratory scale. Models will be developed to describe the effects of selective H2 removal on the DRM reaction. The proposed work is novel in three key respects: (1) Design and preparation of nano-catalysts for DRM with improved low-temperature activity and resistance to coking using a unique flame-based aerosol process; (2) development of CMRs for low-temperature DRM using thermally stable, processible polymer-based membranes, and (3) understanding of the effect of H2-selective removal on the DRM reaction at low temperatures (including CO2 conversion, carbon deposition and catalytic activity). CMRs based on hollow fibers will be prepared and thoroughly characterized for the DRM reaction; predictive models will be developed to uncover the effect of material and operating parameters on CO2 conversion; catalysts will be optimized for low temperature hydrogen-poor conditions; and preliminary techno-economic analysis will be performed, leading to a fuller understanding of the potential of CMRs for the DRM reaction. The graduate and undergraduate students participating in this program will be exposed to interdisciplinary research of reaction engineering, separation and materials science. The results will be incorporated into courses at the University at Buffalo, a popular textbook, and user-friendly teaching modules. Outreach activities will provide access to educational modules and research training to high school and undergraduate students from underrepresented groups in the Buffalo area and inspire them to pursue STEM careers.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.