scholarly journals Spin-Polarized Oxygen Evolution Reaction Under Magnetic Field

Author(s):  
Xiao Ren ◽  
Tianze Wu ◽  
Yuanmiao Sun ◽  
Yan Li ◽  
Guoyu Xian ◽  
...  

<p><a></a><a>The oxygen evolution reaction (OER) is the bottleneck that limits the energy efficiency of water-splitting. The process involves four electrons’ transfer and the generation of triplet state O<sub>2</sub> from singlet state species (OH<sup>- </sup>or H<sub>2</sub>O). Recently, explicit spin selection was described as a possible way to promote OER in alkaline conditions, but the specific spin-polarized kinetics remains unclear. </a><a></a><a>Here, we report that </a><a>by using ferromagnetic ordered catalysts as the spin polarizer for spin selection under </a><a></a><a>a constant magnetic field</a>, <a>the OER can be enhanced.</a> However, it does not applicable to non-ferromagnetic catalysts. We found that the spin <a>polarization occurs at the first electron transfer step in OER</a>, where <a></a><a>coherent spin exchange happens </a>between the <a></a><a>ferromagnetic</a> catalyst and the adsorbed oxygen species <a>with fast kinetics</a>, under the principle of spin angular momentum conservation. In the next three electron transfer steps, as the adsorbed O species adopt fixed spin direction, the OER electrons need to follow the Hund rule and Pauling exclusion principle, thus to carry out spin polarization spontaneously and finally lead to the generation of triplet state O<sub>2</sub>. Here, we showcase spin-polarized kinetics of oxygen evolution reaction, which gives references in the understanding and design of spin-dependent catalysts.</p>

2021 ◽  
Author(s):  
Xiao Ren ◽  
Tianze Wu ◽  
Yuanmiao Sun ◽  
Yan Li ◽  
Guoyu Xian ◽  
...  

<p><a></a><a>The oxygen evolution reaction (OER) is the bottleneck that limits the energy efficiency of water-splitting. The process involves four electrons’ transfer and the generation of triplet state O<sub>2</sub> from singlet state species (OH<sup>- </sup>or H<sub>2</sub>O). Recently, explicit spin selection was described as a possible way to promote OER in alkaline conditions, but the specific spin-polarized kinetics remains unclear. </a><a></a><a>Here, we report that </a><a>by using ferromagnetic ordered catalysts as the spin polarizer for spin selection under </a><a></a><a>a constant magnetic field</a>, <a>the OER can be enhanced.</a> However, it does not applicable to non-ferromagnetic catalysts. We found that the spin <a>polarization occurs at the first electron transfer step in OER</a>, where <a></a><a>coherent spin exchange happens </a>between the <a></a><a>ferromagnetic</a> catalyst and the adsorbed oxygen species <a>with fast kinetics</a>, under the principle of spin angular momentum conservation. In the next three electron transfer steps, as the adsorbed O species adopt fixed spin direction, the OER electrons need to follow the Hund rule and Pauling exclusion principle, thus to carry out spin polarization spontaneously and finally lead to the generation of triplet state O<sub>2</sub>. Here, we showcase spin-polarized kinetics of oxygen evolution reaction, which gives references in the understanding and design of spin-dependent catalysts.</p>


2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Xiao Ren ◽  
Tianze Wu ◽  
Yuanmiao Sun ◽  
Yan Li ◽  
Guoyu Xian ◽  
...  

AbstractThe oxygen evolution reaction (OER) is the bottleneck that limits the energy efficiency of water-splitting. The process involves four electrons’ transfer and the generation of triplet state O2 from singlet state species (OH- or H2O). Recently, explicit spin selection was described as a possible way to promote OER in alkaline conditions, but the specific spin-polarized kinetics remains unclear. Here, we report that by using ferromagnetic ordered catalysts as the spin polarizer for spin selection under a constant magnetic field, the OER can be enhanced. However, it does not applicable to non-ferromagnetic catalysts. We found that the spin polarization occurs at the first electron transfer step in OER, where coherent spin exchange happens between the ferromagnetic catalyst and the adsorbed oxygen species with fast kinetics, under the principle of spin angular momentum conservation. In the next three electron transfer steps, as the adsorbed O species adopt fixed spin direction, the OER electrons need to follow the Hund rule and Pauling exclusion principle, thus to carry out spin polarization spontaneously and finally lead to the generation of triplet state O2. Here, we showcase spin-polarized kinetics of oxygen evolution reaction, which gives references in the understanding and design of spin-dependent catalysts.


Author(s):  
Hanna Lyle ◽  
Suryansh Singh ◽  
Michael Paolino ◽  
Ilya Vinogradov ◽  
Tanja Cuk

The conversion of diffusive forms of energy (electrical and light) into short, compact chemical bonds by catalytic reactions regularly involves moving a carrier from an environment that favors delocalization to one that favors localization.


2020 ◽  
Vol 8 (8) ◽  
pp. 4407-4415 ◽  
Author(s):  
Zechao Shen ◽  
Yongbin Zhuang ◽  
Weiwei Li ◽  
Xiaochun Huang ◽  
Freddy E. Oropeza ◽  
...  

Hole for faster OER: The hole state induced by Fe4+ promotes the OER process. It reduces the energy barrier for electron transfer at the interface and facilitates a faster electron transfer from reaction intermediates to the catalyst.


2002 ◽  
Vol 357 (1426) ◽  
pp. 1431-1440 ◽  
Author(s):  
Alison Telfer

During photosynthesis carotenoids normally serve as antenna pigments, transferring singlet excitation energy to chlorophyll, and preventing singlet oxygen production from chlorophyll triplet states, by rapid spin exchange and decay of the carotenoid triplet to the ground state. The presence of two β–carotene molecules in the photosystem II reaction centre (RC) now seems well established, but they do not quench the triplet state of the primary electron–donor chlorophylls, which are known as P 680 . The β–carotenes cannot be close enough to P 680 for triplet quenching because that would also allow extremely fast electron transfer from β–carotene to P + 680 , preventing the oxidation of water. Their transfer of excitation energy to chlorophyll, though not very efficient, indicates close proximity to the chlorophylls ligated by histidine 118 towards the periphery of the two main RC polypeptides. The primary function of the β–carotenes is probably the quenching of singlet oxygen produced after charge recombination to the triplet state of P 680 . Only when electron donation from water is disturbed does β–carotene become oxidized. One β–carotene can mediate cyclic electron transfer via cytochrome b 559. The other is probably destroyed upon oxidation, which might trigger a breakdown of the polypeptide that binds the cofactors that carry out charge separation.


2019 ◽  
Vol 7 (38) ◽  
pp. 22063-22069 ◽  
Author(s):  
Tong Wu ◽  
Shaoning Zhang ◽  
Kejun Bu ◽  
Wei Zhao ◽  
Qingyuan Bi ◽  
...  

The extraordinary oxygen evolution reaction (OER) in alkaline fuel cells and water-splitting systems demands a high electron transfer rate and catalysts with numerous active sites and massive hydroxyl groups.


2021 ◽  
Author(s):  
Xiwen Du ◽  
Zhe Li ◽  
Yi Feng ◽  
Xiuyao Lang ◽  
Wenjing Kang ◽  
...  

In this study, a core-shell structure (Ag@Co3O4) was constructed to modify valance state of cobalt cations precisely by continuously adjusting the shell thickness. There exists a volcano relationship between valence...


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