显示结相互作用的OEC四核模型:应用于电催化氧化水到过氧化的电催化氧化
Zhiji Han1, Kyle T Horak1, Heui Beom Lee1
1Division of Chemistry and Chemical Engineering, California Institute of Technology , Pasadena, California 91125, United States.
Journal of the American Chemical Society
|June 8, 2017
概括
研究人员合成了复合体,以模拟光系统II中的氧进化复合体 (OEC). 氧化物复合体显示出O-O键形成的电催化活性,这对于水的氧化至关重要.
科学领域:
- 生物有机化学 生物有机化学
- 光催化作用的光催化
- 协调化学 协调化学
背景情况:
- 光系统II中的氧进化复合体 (OEC) 对于光合作用中的水氧化至关重要.
- 开发OEC的合成模型有助于理解其结构和功能.
- 第二个协调球相互作用在酶催化中起着至关重要的作用.
研究的目的:
- 为了合成位点差异化的四核化合物.
- 为了结合生物相关相互作用的键替代剂.
- 研究这些复合物的电催化活性,以形成O-O键.
主要方法:
- 合成四核复合体,具有不同的协调号码.
- 将pyrazolate连接物与arylamine替代物结合在一起,以进行结.
- 电化学研究以评估水氧化和基质氧化催化.
主要成果:
- 成功合成了具有三个六坐标和一个五坐标Mn中心的位点差异化复合物.
- 结网在较低坐标金属中心支持阴离子联体 (OH-,Cl-).
- 氧化物复合物表现出O-O键形成的电催化活性,观察到水氧化为H2O2.2.
- 9,10-二甲烯的电化学氧化通过H原子抽象和氧化产生了~50%的法拉代性产量.
结论:
- 合成的复合物作为OEC的功能模型.
- 结合相互作用对于稳定关键中间体至关重要.
- 氧化物复合体显示出作为氧化水的电催化剂的潜力,尽管有竞争反应.
相关概念视频
Electron Transport Chain: Complex III and IV
9.5K
During the electron transport chain, electrons from NADH and FADH2 are first transferred to complexes I and II, respectively. These two complexes then transfer the electrons to ubiquinol, which carries them further to complex III. Complex III passes the electrons across the intermembrane space to Cyt c, which carries them further to complex IV. Complex IV donates electrons to oxygen and reduces it to water. As electrons pass through complexes I, III, and IV, the energy released aids the pumping...
9.5K
Electron Transport Chains
114.2K
The final stage of cellular respiration is oxidative phosphorylation that consists of two steps: the electron transport chain and chemiosmosis. The electron transport chain is a set of proteins found in the inner mitochondrial membrane in eukaryotic cells. Its primary function is to establish a proton gradient that can be used during chemiosmosis to produce ATP and generate electron carriers, such as NAD+ and FAD, that are used in glycolysis and the citric acid cycle.
The ETC is comprised of...
The ETC is comprised of...
114.2K
Electron Transport Chain: Complex I and II
19.3K
The mitochondrial electron transport chain (ETC) is the main energy generation system in the eukaryotic cells. However, mitochondria also produce cytotoxic reactive oxygen species (ROS) due to the large electron flow during oxidative phosphorylation. While Complex I is one of the primary sources of superoxide radicals, ROS production by Complex II is uncommon and may only be observed in cancer cells with mutated complexes.
ROS generation is regulated and maintained at moderate levels necessary...
ROS generation is regulated and maintained at moderate levels necessary...
19.3K
The Supercomplexes in the Crista Membrane
3.1K
The mitochondrial cristae membrane is the primary site for the oxidative phosphorylation (OXPHOS) process of energy conversion mediated through respiratory complexes I to V. These complexes have been widely studied for decades, and it has been proven that they form supramolecular structures called respiratory supercomplexes (SC). These higher-order complexes may be crucial in maintaining the biochemical structure and improving the physiological activity of the individual complexes while...
3.1K
Oxygenic Photosynthesis
856
Oxygenic photosynthesis is a fundamental process in which light energy is harnessed to drive the oxidation of water, leading to the production of molecular oxygen (O₂), adenosine triphosphate (ATP), and nicotinamide adenine dinucleotide phosphate (NADPH). This process is essential for sustaining aerobic life on Earth and is primarily carried out by cyanobacteria, algae, and plants. The core of oxygenic photosynthesis lies in the thylakoid membranes, where chlorophyll pigments facilitate...
856
Radical Oxidation of Allylic and Benzylic Alcohols
3.0K
Activated manganese(IV) oxide can selectively oxidize allylic and benzylic alcohols via a radical intermediate mechanism. Primary allylic alcohols are oxidized to aldehydes, while secondary allylic alcohols yield ketones. The redox reaction of potassium permanganate with an Mn(II) salt such as manganese sulfate (under either alkaline or acidic conditions), followed by thorough drying, yields the oxidizing agent: activated MnO2. While MnO2 is insoluble in the solvents used for the reaction, the...
3.0K

![Protein Film Infrared Electrochemistry Demonstrated for Study of H2 Oxidation by a [NiFe] Hydrogenase](/_next/image?url=https%3A%2F%2Fcloudfront.jove.com%2FCDNSource%2Fteasers%2F55858.jpg&w=3840&q=50)
