{"title":"通过手性混合Mn/Fe/Ni/ co基过渡金属氧化物解读自旋极化在析氧中的作用。","authors":"Utkarsh Utkarsh, Sachidananda Sahu, Anujit Balo, Dibyendu Barik, Koyel Banerjee Ghosh","doi":"10.1002/asia.202500137","DOIUrl":null,"url":null,"abstract":"<p>Oxygen evolution reaction (OER) plays a crucial role in energy storage and conversion technologies. However, its higher overpotential challenges the scientific community to overcome it. Recent advancements in OER demonstrate that inducing spin-polarization at the anode either employing chiral molecular modification or magnetic substrate, augmentation of OER is possible. Adopting this idea, we evaluated the effect of chiral molecular modification of mixed-transition metal-based spinel oxide on the spin-polarized charge transfer during OER. Chiral molecular functionalization of the catalyst has been carried out using chiral analogs of phenylalanine, which enhances the stability and catalytic activity of the catalyst by controlling the electron's spin utilizing the chiral-induced spin selectivity (CISS) effect. The experimental results show that the chiral molecule integrated catalyst decreases the overpotential by ∼200 mV at 10 mA cm<sup>−2</sup> with respect to the achiral one. Moreover, it increases the current density by ∼2 times at 2.1 V (vs. RHE) and decreases hydrogen peroxide production significantly compared to its achiral analog. The results of these studies are explained by controlling the spin-polarization of the anodic current during water oxidation employing CISS effect. Hence, this study opens new avenues for enhancing the performance of the catalysts for sustainable energy applications utilizing spin-polarized charge transfer.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":"20 17","pages":""},"PeriodicalIF":3.3000,"publicationDate":"2025-06-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Deciphering the Role of Spin-Polarization in Oxygen Evolution via Chiral Mixed Mn/Fe/Ni/Co-Based Transition Metal Oxide\",\"authors\":\"Utkarsh Utkarsh, Sachidananda Sahu, Anujit Balo, Dibyendu Barik, Koyel Banerjee Ghosh\",\"doi\":\"10.1002/asia.202500137\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Oxygen evolution reaction (OER) plays a crucial role in energy storage and conversion technologies. However, its higher overpotential challenges the scientific community to overcome it. Recent advancements in OER demonstrate that inducing spin-polarization at the anode either employing chiral molecular modification or magnetic substrate, augmentation of OER is possible. Adopting this idea, we evaluated the effect of chiral molecular modification of mixed-transition metal-based spinel oxide on the spin-polarized charge transfer during OER. Chiral molecular functionalization of the catalyst has been carried out using chiral analogs of phenylalanine, which enhances the stability and catalytic activity of the catalyst by controlling the electron's spin utilizing the chiral-induced spin selectivity (CISS) effect. The experimental results show that the chiral molecule integrated catalyst decreases the overpotential by ∼200 mV at 10 mA cm<sup>−2</sup> with respect to the achiral one. Moreover, it increases the current density by ∼2 times at 2.1 V (vs. RHE) and decreases hydrogen peroxide production significantly compared to its achiral analog. The results of these studies are explained by controlling the spin-polarization of the anodic current during water oxidation employing CISS effect. Hence, this study opens new avenues for enhancing the performance of the catalysts for sustainable energy applications utilizing spin-polarized charge transfer.</p>\",\"PeriodicalId\":145,\"journal\":{\"name\":\"Chemistry - An Asian Journal\",\"volume\":\"20 17\",\"pages\":\"\"},\"PeriodicalIF\":3.3000,\"publicationDate\":\"2025-06-02\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemistry - An Asian Journal\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://aces.onlinelibrary.wiley.com/doi/10.1002/asia.202500137\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemistry - An Asian Journal","FirstCategoryId":"1","ListUrlMain":"https://aces.onlinelibrary.wiley.com/doi/10.1002/asia.202500137","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
析氧反应(OER)在能量存储和转化技术中起着至关重要的作用。然而,它的高过电位给科学界提出了克服它的挑战。近年来OER的研究进展表明,无论是采用手性分子修饰还是磁性衬底,都可以在阳极处诱导自旋极化,从而增加OER。采用这一思路,我们评估了混合过渡金属基尖晶石氧化物的手性分子修饰对OER过程中自旋极化电荷转移的影响。利用苯丙氨酸的手性类似物对催化剂进行了手性分子功能化,利用手性诱导自旋选择性(CISS)效应控制电子自旋,提高催化剂的稳定性和催化活性。实验结果表明,与非手性催化剂相比,手性分子集成催化剂在10 mA cm-2下的过电位降低了~ 200 mV。此外,与非手性类似物相比,它在2.1 V时的电流密度增加了约2倍(与RHE相比),并且显著降低了过氧化氢的产量。这些研究结果是通过利用CISS效应控制水氧化过程中阳极电流的自旋极化来解释的。因此,本研究为利用自旋极化电荷转移提高可持续能源应用催化剂的性能开辟了新的途径。
Deciphering the Role of Spin-Polarization in Oxygen Evolution via Chiral Mixed Mn/Fe/Ni/Co-Based Transition Metal Oxide
Oxygen evolution reaction (OER) plays a crucial role in energy storage and conversion technologies. However, its higher overpotential challenges the scientific community to overcome it. Recent advancements in OER demonstrate that inducing spin-polarization at the anode either employing chiral molecular modification or magnetic substrate, augmentation of OER is possible. Adopting this idea, we evaluated the effect of chiral molecular modification of mixed-transition metal-based spinel oxide on the spin-polarized charge transfer during OER. Chiral molecular functionalization of the catalyst has been carried out using chiral analogs of phenylalanine, which enhances the stability and catalytic activity of the catalyst by controlling the electron's spin utilizing the chiral-induced spin selectivity (CISS) effect. The experimental results show that the chiral molecule integrated catalyst decreases the overpotential by ∼200 mV at 10 mA cm−2 with respect to the achiral one. Moreover, it increases the current density by ∼2 times at 2.1 V (vs. RHE) and decreases hydrogen peroxide production significantly compared to its achiral analog. The results of these studies are explained by controlling the spin-polarization of the anodic current during water oxidation employing CISS effect. Hence, this study opens new avenues for enhancing the performance of the catalysts for sustainable energy applications utilizing spin-polarized charge transfer.
期刊介绍:
Chemistry—An Asian Journal is an international high-impact journal for chemistry in its broadest sense. The journal covers all aspects of chemistry from biochemistry through organic and inorganic chemistry to physical chemistry, including interdisciplinary topics.
Chemistry—An Asian Journal publishes Full Papers, Communications, and Focus Reviews.
A professional editorial team headed by Dr. Theresa Kueckmann and an Editorial Board (headed by Professor Susumu Kitagawa) ensure the highest quality of the peer-review process, the contents and the production of the journal.
Chemistry—An Asian Journal is published on behalf of the Asian Chemical Editorial Society (ACES), an association of numerous Asian chemical societies, and supported by the Gesellschaft Deutscher Chemiker (GDCh, German Chemical Society), ChemPubSoc Europe, and the Federation of Asian Chemical Societies (FACS).