EAGER: Partial Oxidation of Methane Using Supported, Fluoroalkylated Phthalocyanine Catalysts

10223373 Barat该提案涵盖了初步实验，以证明一种新的催化剂家族，该家族将进行甲烷的生物启发选择性部分氧化。产物可能是甲醇，但可能由C-C偶联反应形成一些烷烃。显然，部分氧化为甲醇是最经济和合理的反应选择。人们希望在氧化步骤期间具有更高选择性的催化剂。PI逐步分析选项：异质性，同质性，生物，全细胞和仿生，权衡成功的可能性。他们只剩下他们所谓的生物启发方法。通过进一步的分析，他们选择全氟烷基金属酞菁（卟啉的类似物）作为非常可能的催化剂，以提高选择性，并且也可能进行C-C偶联催化。一些支持计算是一致的。注意，所需的是低温和低压操作制度。更广泛的方面：这是一个EAGER的建议，因为没有数据存在，以支持或反驳的论点。如果PI是正确的，这将是一个令人兴奋的机会。在温和条件下的良好性能将允许回收搁浅或废弃的甲烷作为液体化学品/燃料，这更容易处理，运输和利用。这也是一种温室气体减排战略。实验计划涉及催化剂合成（不一定容易）的催化剂与各种全氟烷基基团和各种金属离子，然后在简单的实验室设备进行评估。 计划使用化学和化学工程专业的学生来完成这项工作，包括本科生。将寻求代表性不足的学生，因为入学人数主要是非白人，这种参与是可能的。该项目将吸引许多学生，因为它涉及催化剂合成并寻求解决环境问题。

10223373BaratThis proposal covers initial experiments to prove out a new family of catalysts which will carry out the biologically-inspired selective partial oxidation of methane. Products are likely methanol, but potentially some alkane hydrocarbons may be formed from C-C coupling reactions. It is clear that partial oxidation to methanol is the most economical and logical reaction choice. One would desire a catalyst with more selectivity during the oxidation step. The PIs step through an analysis of the options: heterogeneous, homogeneous, biological, whole cell, and biomimetic, weighing the possibility for success. They are left with what they term the bio-inspired approach. By further analysis they arrive at the choice of perfluoroalkyl metal phthalocyanine (an analogue of porphyrin) as a very likely catalyst for improved selectivity and also the possibility of C-C coupling catalysis as well. Some supporting calculations are consistent. Note that what is desired is a low temperature and pressure operating regime.Broader Aspects:This is an EAGER proposal because no data exists to support or refute the contention. If the PIs were correct, this would be an exciting opportunity. Good performance at moderate conditions would allow for the recovery of stranded or waste methane as liquid chemicals/fuels, which are far easier to handle, transport and utilize. This also is a GHG reducing strategy. The experimental program involves catalyst synthesis (not necessarily easy) of catalysts with various perfluoroalkyl groups and various metal ions, and then evaluation in straightforward laboratory equipment. Plans are to use a mix of chemistry and chemical engineering students to carry out the work, including undergraduates. Under-represented students will be sought, and because the enrollment is predominantly non-white, this involvement is likely. This project will have appeal to a number of students, as it involves catalyst synthesis and seeks to solve an environmental problem.