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手性氧化铁纳米颗粒中的自旋选择性析氧反应:固有磁矩和手性的协同影响。

Spin-Selective Oxygen Evolution Reaction in Chiral Iron Oxide Nanoparticles: Synergistic Impact of Inherent Magnetic Moment and Chirality.

作者信息

Nair Aruna Narayanan, Fernandez Sara, Marcos-Hernández Mariana, Romo Daniel Rascon, Singamaneni Srinivasa Rao, Villagran Dino, Sreenivasan Sreeprasad T

机构信息

Department of Chemistry and Biochemistry, The University of Texas at El Paso, El Paso, Texas 79968, United States.

Department of Physics, The University of Texas at El Paso, El Paso, Texas 79968, United States.

出版信息

Nano Lett. 2023 Oct 11;23(19):9042-9049. doi: 10.1021/acs.nanolett.3c02752. Epub 2023 Sep 22.

Abstract

Electron spin polarization is identified as a promising avenue for enhancing the oxygen evolution reaction (OER), which is the bottleneck that limits the energy efficiency of water-splitting. Here, we report that both ferrimagnetic (f-FeO) and superparamagnetic iron oxide (s-FeO) catalysts can exhibit external magnetic field (Hext)-induced OER enhancement, and the activity is proportional to their intrinsic magnetic moment. Additionally, the chirality-induced spin selectivity (CISS) effect was utilized in synergy with Hext to get a maximum enhancement of up to 89% improvement in current density (at 1.8 V vs RHE) with a low onset potential of 270 mV in s-FeO catalysts. Spin polarization and the resultant spin selectivity suppress the production of HO and promote the formation of ground state triplet O during the OER. Furthermore, the design of chiral s-FeO with synergistic spin potential effect demonstrates a high spin polarization of ∼42%, as measured using conductive atomic force microscopy (c-AFM).

摘要

电子自旋极化被认为是增强析氧反应(OER)的一条有前景的途径,析氧反应是限制水分解能量效率的瓶颈。在此,我们报道亚铁磁性(f-FeO)和超顺磁性氧化铁(s-FeO)催化剂都能表现出外部磁场(Hext)诱导的OER增强,且活性与其固有磁矩成正比。此外,手性诱导自旋选择性(CISS)效应与Hext协同作用,在s-FeO催化剂中实现了电流密度最大提高89%(相对于可逆氢电极在1.8 V时),起始电位低至270 mV。自旋极化和由此产生的自旋选择性在OER过程中抑制了HO的产生,并促进了基态三重态O的形成。此外,通过导电原子力显微镜(c-AFM)测量,具有协同自旋势效应的手性s-FeO设计显示出约42%的高自旋极化。

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