Oxidation Catalysis with 3d Complexes Bearing Fluorinated Alkoxide Ligands

氧化反应在现代化学中非常重要和广泛。 最便宜和最可持续的氧化剂是大气氧（O2）。 这项研究扩展了波士顿大学Doerrer教授和Roxbury社区学院（RCC）Stieglitz教授实验室在制备新铜（Cu）催化剂方面的先前成功。 研究人员正在设计和开发新的催化剂，这些催化剂的寿命更长，反应性更高。 他们还在设计水溶性催化剂，以避免使用昂贵或有毒的有机溶剂。波士顿大学和罗克斯伯里社区学院之间的新合作开发了一个新的夏季研究班，汇集了过渡金属络合物和RCC与天然产品的经验BU的专业知识。 罗克斯伯里社区学院（RCC）是一所代表性不足的少数民族机构。 该研究展示了如何将可持续性概念纳入具有挑战性和重要的化学反应中。碳-氢（C-H）键的氧化仍然是具有许多剩余挑战的化学转化。 这项研究建立在最近成功的Cu/O2化学，已经证明了氟化醇盐配体的有效性，使高活性物种氧化碳-氢键。 氟化，螯合O-供体配体的开发，以确定螯合环的大小和总的金属络合物的电荷上的氧化反应的影响由{CunO 2}部分。 然后，研究人员确定了这种化学制剂用于氧化催化剂的潜在宽度。 最后，研究人员在最近的工作基础上，从d区中间使用更多的地球丰富的金属-铬，锰和铁-使用水，一种更可持续的溶剂中的氟化醇盐配体。 波士顿大学和罗克斯伯里社区学院之间的新合作开发了一个新的夏季研究班，汇集了过渡金属络合物和RCC与天然产品的经验BU的专业知识。 这一合作增强了RCC的能力，以培养代表性不足的少数民族学生的科学事业，同时让他们在一个高度研究密集型大学的研究。这一奖项反映了NSF的法定使命，并已被认为是值得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的支持。

Oxidation reactions are critically important and widespread in modern chemistry. The cheapest and most sustainable oxidant is atmospheric oxygen (O2). This research expands on prior successes in the laboratories of Professor Doerrer, Boston University and Professor Stieglitz of Roxbury Community College (RCC) in preparing new copper (Cu) catalysts. The researchers are designing and developing new catalysts that are longer lived and more selective in their reactivity. They are also designing water-soluble catalysts to avoid the use of expensive or toxic organic solvents. A new collaboration between Boston University and Roxbury Community College develops a new summer research class that brings together BU expertise in transition metal complexes and RCC experience with natural products. Roxbury Community College (RCC) is a predominantly under-represented minority institution. The research demonstrates how to incorporate sustainability concepts into challenging and important chemical reactions. Oxidation of carbon-hydrogen (C-H) bonds remains a chemical transformation with many remaining challenges. This research builds on recent success with Cu/O2 chemistry that has demonstrated the effectiveness of fluorinated alkoxide ligands in making highly reactive species for oxidizing carbon-hydrogen bonds. The fluorinated, chelating O-donor ligands are developed to determine the effect of chelate ring size and overall metal complex charge on the oxidation reactions by {CunO2} moieties. The researchers then determine the potential breadth of this chemical formulation for oxidation catalysts. Finally, the researchers build on recent work with more earth-abundant metals from the middle of the d-block - chromium, manganese, and iron - using the fluorinated alkoxide ligands in water, a more sustainable solvent. A new collaboration between Boston University and Roxbury Community College develops a new summer research class that brings together BU expertise in transition metal complexes and RCC experience with natural products. This collaboration enhances the capacities of RCC to train under-represented minority students for science careers, while exposing them to research at an highly research intensive university.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.