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

这项提议包括初步实验，以证明一种新的催化剂家族将执行生物启发的甲烷选择性部分氧化。产物可能是甲醇，但潜在的一些烷烃可能是由C-C偶联反应形成的。由此可见，部分氧化制甲醇是最经济合理的反应选择。人们希望在氧化步骤中有一种选择性更高的催化剂。PIs一步一步分析各种选择：异质、同质、生物、全细胞和仿生，权衡成功的可能性。留给他们的是他们所说的生物启发方法。通过进一步的分析，他们得出了选择全氟烷基金属酞菁(一种卟啉的类似物)作为一种很有可能提高选择性的催化剂以及C-C偶联催化的可能性。一些支持性的计算是一致的。请注意，所需要的是一种低温和压力的运行方案。广泛的方面：这是一个急切的建议，因为没有数据来支持或驳斥这一论点。如果PI是正确的，这将是一个令人兴奋的机会。在中等条件下的良好表现将允许将滞留或废弃的甲烷作为液体化学品/燃料进行回收，这些液体化学品/燃料更易于处理、运输和利用。这也是一种温室气体减排战略。实验计划包括合成具有各种全氟烷基和各种金属离子的催化剂(不一定容易)，然后在直接的实验室设备中进行评估。计划使用化学和化学工程专业的学生来开展这项工作，其中包括本科生。将招收代表人数不足的学生，由于招生主要是非白人，这种参与是可能的。这个项目将吸引许多学生，因为它涉及催化剂合成，并寻求解决一个环境问题。

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.