增强无金属供体-受体共轭光催化剂的内电场以实现四环素的高效光催化降解和二氧化碳还原

IF 3.7 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Guangyu Wu, Geng Li, Yonggong Tang, Guoyu Tai, Yuwei Pan, Jiangang Han, Weinan Xing
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引用次数: 0

摘要

在 g-C3N4 中构建交替的供体-受体(D-A)单元是通过改善电荷载流子分离来提高光催化性能的有效策略,同时还能解决能源短缺问题并促进废水修复。本文以 g-C3N4 为受体单元,以不同质量的 5-溴-2-噻吩甲醛(BTC)为供体单元,通过一步热聚合法制备了一系列 D-A 型共轭光催化剂(CNBTC-X)。与 g-C3N4、CNBTC-10、CNBTC-30 和 CNBTC-70 相比,CNBTC-50 在二氧化碳还原和四环素(TC)去除方面具有更高的光催化性能。独特的电子-供体-受体结构的引入有效地促进了光诱导载流子的分离和转移,同时减少了内部载流子的转移阻碍。光催化实验表明,在可见光照射条件下,CNBTC-50 光催化剂的三氯甲烷去除率高达 94.6%。与原始 g-C3N4 相比,CNBTC-50 的光催化降解反应速率常数显著提高了约 3.87 倍。研究考察了催化剂浓度、pH 值和 TC 浓度等各种反应参数对降解活性的影响。此外,还利用 LC-MS 对 TC 降解过程中的中间产物和途径进行了全面分析。此外,CNBTC-50 还表现出显著的光催化二氧化碳还原活性,其还原速率分别达到 20.83 μmol g-1 h-1 (CO)和 9.36 μmol g-1 h-1 (CH4),分别是 g-C3N4 的 10.68 倍和 5.98 倍。这项工作旨在为合理设计非金属 D-A 结构催化剂提供有价值的指导,并有效整合反应体系,将二氧化碳还原与抗生素去除结合起来。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Enhancing Internal Electric Field of Metal-Free Donor-Acceptor Conjugated Photocatalysts for Efficient Photocatalytic Degradation of Tetracycline and CO<sub>2</sub> Reduction.

Enhancing Internal Electric Field of Metal-Free Donor-Acceptor Conjugated Photocatalysts for Efficient Photocatalytic Degradation of Tetracycline and CO2 Reduction.

Constructing alternating donor-acceptor (D-A) units within g-C3N4 represents an effective strategy for enhancing photocatalytic performance through improved charge carrier separation while concurrently addressing energy shortages and facilitating wastewater remediation. Here, a series of D-A-type conjugated photocatalysts (CNBTC-X) are prepared using g-C3N4 as an acceptor unit and different masses of 5-bromo-2-thiophenecarboxaldehyde (BTC) as a donor unit by a one-step thermal polymerization. CNBTC-50 presents higher photocatalytic properties for CO2 reduction coupled with tetracycline (TC) removal than those of g-C3N4, CNBTC-10, CNBTC-30, and CNBTC-70. The introduction of the unique electron-donor-acceptor structure effectively drives the separation and transfer of photoinduced carriers while reducing the internal carrier transfer hindrance. Photocatalytic experiments reveal that the CNBTC-50 photocatalyst achieves up to 94.6% TC removal under visible light irradiation conditions. Compared with that of the pristine g-C3N4, the photocatalytic degradation reaction rate constant of CNBTC-50 is significantly increased by about 3.87 times. The study examines the influence of various reaction parameters on degradation activity, including catalyst concentration, pH, and TC concentration. Additionally, LC-MS is utilized to perform a comprehensive analysis of the intermediates and pathways involved in TC degradation. Furthermore, CNBTC-50 demonstrates remarkable photocatalytic CO2 reduction activity, achieving rates of 20.83 μmol g-1 h-1 (CO) and 9.36 μmol g-1 h-1 (CH4), which are 10.68 and 5.98 times more efficient than those of g-C3N4, respectively. This work aims to offer valuable guidance for the rational design of nonmetal D-A-structured catalysts and effectively integrates reaction systems to couple CO2 reduction with antibiotic removal.

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来源期刊
Langmuir
Langmuir 化学-材料科学:综合
CiteScore
6.50
自引率
10.30%
发文量
1464
审稿时长
2.1 months
期刊介绍: Langmuir is an interdisciplinary journal publishing articles in the following subject categories: Colloids: surfactants and self-assembly, dispersions, emulsions, foams Interfaces: adsorption, reactions, films, forces Biological Interfaces: biocolloids, biomolecular and biomimetic materials Materials: nano- and mesostructured materials, polymers, gels, liquid crystals Electrochemistry: interfacial charge transfer, charge transport, electrocatalysis, electrokinetic phenomena, bioelectrochemistry Devices and Applications: sensors, fluidics, patterning, catalysis, photonic crystals However, when high-impact, original work is submitted that does not fit within the above categories, decisions to accept or decline such papers will be based on one criteria: What Would Irving Do? Langmuir ranks #2 in citations out of 136 journals in the category of Physical Chemistry with 113,157 total citations. The journal received an Impact Factor of 4.384*. This journal is also indexed in the categories of Materials Science (ranked #1) and Multidisciplinary Chemistry (ranked #5).
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