Zeeman Effect-Boosted Spin-Polarized Band Splitting in Diluted Magnetic Photocatalysis Semiconductors for Efficient CO2 Photoreduction

IF 16 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY ACS Nano Pub Date : 2024-12-20 DOI:10.1021/acsnano.4c14424
Shuhui Xia, Xin Yin, Yuehui Chen, Liang Zhang, Jianyong Yu, Bin Ding, Jianhua Yan
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Abstract

Magnetic field regulation is an effective strategy to improve the photocatalytic activity of magnetic semiconductor photocatalysts, but it is not suitable for widely used nonmagnetic photocatalytic semiconductors. Here, we report a Zeeman effect-driven spin-polarized band splitting phenomenon in diluted magnetic semiconductors that show efficient photocatalytic CO2 reduction under visible-light irradiation. A flexible Ni2+-doped BaTiO3 nanofiber film is used as the diluted magnetic semiconductor model to prove this concept. The interstitial Ni2+ dopant induces the spin-polarized bands in Ni-BaTiO3 nanofibers to split under light excitation, generating spin-excited electrons and holes. This Zeeman effect induced by the magnetic field is more obvious since it intensifies the spin-polarized band splitting and generates more spin-excited electrons and holes, suppressing the carrier recombination and extending the carrier lifetime for CO2 photoreduction. As a result, the evolution rates of CO and CH4 are as high as 86.47 and 96.06 μmol/g/h under a small magnetic field of 50 mT. The proposed mechanism of Zeeman effect-driven spin-polarized band splitting is feasible to improve the CO2 photoreduction efficiency of broadly applied diluted magnetic semiconductors.

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稀释磁光催化半导体中塞曼效应增强的自旋极化带分裂用于高效CO2光还原
磁场调节是提高磁性半导体光催化剂光催化活性的有效策略,但不适用于广泛应用的非磁性光催化半导体。在这里,我们报道了一种塞曼效应驱动的自旋极化带分裂现象,在稀释的磁性半导体中,在可见光照射下显示出有效的光催化CO2还原。采用柔性掺杂Ni2+的BaTiO3纳米纤维薄膜作为稀释磁性半导体模型来证明这一概念。Ni2+掺杂使Ni-BaTiO3纳米纤维中的自旋极化带在光激发下发生分裂,产生自旋激发电子和空穴。磁场诱导的这种塞曼效应更为明显,因为它加剧了自旋极化带分裂,产生了更多的自旋激发电子和空穴,抑制了载流子复合,延长了CO2光还原的载流子寿命。结果表明,在50 mT的小磁场下,CO和CH4的析出速率分别高达86.47和96.06 μmol/g/h。提出的塞曼效应驱动的自旋极化能带分裂机制对于提高广泛应用的稀释磁性半导体的CO2光还原效率是可行的。
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来源期刊
ACS Nano
ACS Nano 工程技术-材料科学:综合
CiteScore
26.00
自引率
4.10%
发文量
1627
审稿时长
1.7 months
期刊介绍: ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.
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