铁分散MoO3−x/MXene的协同等离子体共振杂化增强氮光热还原

IF 4 3区 工程技术 Q2 ENGINEERING, CHEMICAL AIChE Journal Pub Date : 2025-01-29 DOI:10.1002/aic.18745
Ying Tang, Dongsheng Xie, Xiaomin Guo, Lining Fang, Hui Zeng, Zebao Rui
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引用次数: 0

摘要

等离子体光化学固氮技术由于其在提高太阳-氨转化效率方面的显著增强效应而受到广泛关注。然而,金属等离子体光催化剂中较弱的N2吸附亲和力和金属-半导体等离子体光催化剂中难以克服的界面障碍导致电荷载流子快速重组,而不是参与N2到nh3的转化。本文制备了一种具有协同等离子共振杂化结构的fe分散MoO3−x/MXene光热催化剂,用于光热固定N2。由MXene和MoO3−x衍生的杂化等离子体共振效应在紫外-可见-近红外范围内诱发了强烈的光学响应,并产生了高能载流子,而诱导的光热效应进一步加速了电子的提取、输运和表面反应动力学。此外,丰富的氧空位和铁位可以加强N2吸附,并将高能电子提供给反键系统,促进N - H耦合过程。在太阳光照条件下,NH3的生成速率高达87.1 μmol g−1 h−1。
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Synergistic plasmon resonance hybridization of iron-dispersed MoO3−x/MXene for enhanced nitrogen photothermal reduction

Plasmonic photochemical N2 fixation has received widespread attention owing to the attractive plasmonic enhancement effects in improving solar-to-NH3 conversion efficiency. However, the weak N2 adsorption affinity in metallic plasmonic photocatalysts and insurmountable interfacial barriers in metal–semiconductor plasmonic photocatalysts lead to rapid charge carrier recombination instead of participating in N2-to-NH3 conversion. Herein, a photothermal catalyst Fe-dispersed MoO3−x/MXene with synergistic plasmon resonance hybridization structure is fabricated for photothermal N2 fixation. The hybrid plasmon resonance effects derived from MXene and MoO3−x induce a strong optical response across the ultraviolet–visible-near-infrared range and generation of energetic charge carriers, and the induced photothermal effect further accelerates electron extraction, transport, and surface reaction kinetics. Moreover, the abundant oxygen vacancies and Fe sites can intensify the N2 adsorption and donate the energetic electrons into the anti-bonding system for the stimulative NH coupling process. A high NH3 formation rate of 87.1 μmol g−1 h−1 is achieved under solar-level illumination.

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来源期刊
AIChE Journal
AIChE Journal 工程技术-工程:化工
CiteScore
7.10
自引率
10.80%
发文量
411
审稿时长
3.6 months
期刊介绍: The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.
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