Department of Chemical and Biological Physics, Weizmann Institute of Science, Rehovot 76100, Israel.
Department of Engineering "Enzo Ferrari," University of Modena and Reggio Emilia, 41125 Modena, Italy.
Proc Natl Acad Sci U S A. 2022 Jul 26;119(30):e2202650119. doi: 10.1073/pnas.2202650119. Epub 2022 Jul 18.
Controlled reduction of oxygen is important for developing clean energy technologies, such as fuel cells, and is vital to the existence of aerobic organisms. The process starts with oxygen in a triplet ground state and ends with products that are all in singlet states. Hence, spin constraints in the oxygen reduction must be considered. Here, we show that the electron transfer efficiency from chiral electrodes to oxygen (oxygen reduction reaction) is enhanced over that from achiral electrodes. We demonstrate lower overpotentials and higher current densities for chiral catalysts versus achiral ones. This finding holds even for electrodes composed of heavy metals with large spin-orbit coupling. The effect results from the spin selectivity conferred on the electron current by the chiral assemblies, the chiral-induced spin selectivity effect.
控制氧气还原对于开发燃料电池等清洁能源技术很重要,对需氧生物的存在也至关重要。该过程始于三重基态氧,最终产物都处于单重态。因此,必须考虑氧气还原中的自旋约束。在这里,我们表明手性电极对氧(氧还原反应)的电子转移效率高于非手性电极。我们证明了手性催化剂相对于非手性催化剂具有更低的过电位和更高的电流密度。即使对于由具有大自旋轨道耦合的重金属组成的电极,这一发现也是成立的。这种效应是由手性组装体赋予电子电流的自旋选择性引起的,即手性诱导自旋选择性效应。