{"title":"磁场通过对磁矩和分子键的微妙调节促进电催化二氧化碳还原","authors":"Shilin Wei, Weiqi Liu, Peiyao Bai, Chuangchuang Yang, Xiao Kong, Lang Xu","doi":"10.1016/j.eehl.2024.02.003","DOIUrl":null,"url":null,"abstract":"<div><p>Introducing a magnetic-field gradient into an electrically driven chemical reaction is expected to give rise to intriguing research possibilities. In this work, we elaborate on the modes and mechanisms of electrocatalytic activity (from the perspective of alignment of magnetic moments) and selectivity (at the molecular level) for the CO<sub>2</sub> reduction reaction in response to external magnetic fields. We establish a positive correlation between magnetic field strengths and apparent current densities. This correlation can be rationalized by the formation of longer-range ordering of magnetic moments and the resulting decrease in the scattering of conduction electrons and charge-transfer resistances as the field strength increases. Furthermore, aided by the magnetic-field-equipped <em>operando</em> infrared spectroscopy, we find that applied magnetic fields are capable of weakening the C–O bond strength of the key intermediate ∗COOH and elongating the C–O bond length, thereby increasing the faradaic efficiency for the electroreduction of CO<sub>2</sub> to CO.</p></div>","PeriodicalId":29813,"journal":{"name":"Eco-Environment & Health","volume":"3 2","pages":"Pages 247-255"},"PeriodicalIF":0.0000,"publicationDate":"2024-02-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772985024000152/pdfft?md5=2d20ebee471e7163b020ece83e84d0bb&pid=1-s2.0-S2772985024000152-main.pdf","citationCount":"0","resultStr":"{\"title\":\"Magnetic fields promote electrocatalytic CO2 reduction via subtle modulations of magnetic moments and molecular bonding\",\"authors\":\"Shilin Wei, Weiqi Liu, Peiyao Bai, Chuangchuang Yang, Xiao Kong, Lang Xu\",\"doi\":\"10.1016/j.eehl.2024.02.003\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Introducing a magnetic-field gradient into an electrically driven chemical reaction is expected to give rise to intriguing research possibilities. In this work, we elaborate on the modes and mechanisms of electrocatalytic activity (from the perspective of alignment of magnetic moments) and selectivity (at the molecular level) for the CO<sub>2</sub> reduction reaction in response to external magnetic fields. We establish a positive correlation between magnetic field strengths and apparent current densities. This correlation can be rationalized by the formation of longer-range ordering of magnetic moments and the resulting decrease in the scattering of conduction electrons and charge-transfer resistances as the field strength increases. Furthermore, aided by the magnetic-field-equipped <em>operando</em> infrared spectroscopy, we find that applied magnetic fields are capable of weakening the C–O bond strength of the key intermediate ∗COOH and elongating the C–O bond length, thereby increasing the faradaic efficiency for the electroreduction of CO<sub>2</sub> to CO.</p></div>\",\"PeriodicalId\":29813,\"journal\":{\"name\":\"Eco-Environment & Health\",\"volume\":\"3 2\",\"pages\":\"Pages 247-255\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2024-02-29\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S2772985024000152/pdfft?md5=2d20ebee471e7163b020ece83e84d0bb&pid=1-s2.0-S2772985024000152-main.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Eco-Environment & Health\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2772985024000152\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Eco-Environment & Health","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2772985024000152","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
引用次数: 0
摘要
在电驱动化学反应中引入磁场梯度有望带来引人入胜的研究可能性。在这项研究中,我们详细阐述了二氧化碳还原反应在外部磁场作用下的电催化活性(从磁矩排列的角度)和选择性(分子水平)的模式和机制。我们在磁场强度和表观电流密度之间建立了正相关关系。随着磁场强度的增加,磁矩形成长程有序化,从而减少了传导电子的散射和电荷转移电阻,因此这种相关性是合理的。此外,在配备磁场的操作性红外光谱的帮助下,我们发现外加磁场能够减弱关键中间体 ∗COOH 的 C-O 键强度并拉长 C-O 键长度,从而提高 CO2 电还原为 CO 的法拉第效率。
Magnetic fields promote electrocatalytic CO2 reduction via subtle modulations of magnetic moments and molecular bonding
Introducing a magnetic-field gradient into an electrically driven chemical reaction is expected to give rise to intriguing research possibilities. In this work, we elaborate on the modes and mechanisms of electrocatalytic activity (from the perspective of alignment of magnetic moments) and selectivity (at the molecular level) for the CO2 reduction reaction in response to external magnetic fields. We establish a positive correlation between magnetic field strengths and apparent current densities. This correlation can be rationalized by the formation of longer-range ordering of magnetic moments and the resulting decrease in the scattering of conduction electrons and charge-transfer resistances as the field strength increases. Furthermore, aided by the magnetic-field-equipped operando infrared spectroscopy, we find that applied magnetic fields are capable of weakening the C–O bond strength of the key intermediate ∗COOH and elongating the C–O bond length, thereby increasing the faradaic efficiency for the electroreduction of CO2 to CO.
期刊介绍:
Eco-Environment & Health (EEH) is an international and multidisciplinary peer-reviewed journal designed for publications on the frontiers of the ecology, environment and health as well as their related disciplines. EEH focuses on the concept of “One Health” to promote green and sustainable development, dealing with the interactions among ecology, environment and health, and the underlying mechanisms and interventions. Our mission is to be one of the most important flagship journals in the field of environmental health.
Scopes
EEH covers a variety of research areas, including but not limited to ecology and biodiversity conservation, environmental behaviors and bioprocesses of emerging contaminants, human exposure and health effects, and evaluation, management and regulation of environmental risks. The key topics of EEH include:
1) Ecology and Biodiversity Conservation
Biodiversity
Ecological restoration
Ecological safety
Protected area
2) Environmental and Biological Fate of Emerging Contaminants
Environmental behaviors
Environmental processes
Environmental microbiology
3) Human Exposure and Health Effects
Environmental toxicology
Environmental epidemiology
Environmental health risk
Food safety
4) Evaluation, Management and Regulation of Environmental Risks
Chemical safety
Environmental policy
Health policy
Health economics
Environmental remediation