硅酸盐学报

g-C₃N₄/NaNbO₃复合材料降解混合染料的热释电光催化性能

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徐利 ¹ , 邓树文 ² , 周小桔 ³ , 王会峰 ³ , 胡正龙 ³

硅酸盐学报 | 研究论文 2025,53(3): 594-606

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硅酸盐学报 |研究论文 2025 , 53 (3) : 594 -606

g-C₃N₄/NaNbO₃复合材料降解混合染料的热释电光催化性能

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徐利¹, 邓树文², 周小桔³, 王会峰³, 胡正龙³

作者信息

^1．湖北汽车工业学院，数理与光电工程学院，湖北十堰 442002

^2．湖北科技学院，智能应急服务大数据应用湖北省工程研究中心，湖北咸宁 437100

^3．湖北科技学院，电子与信息工程学院，湖北咸宁 437100

通讯作者:

邓树文（1979—），男，硕士，副教授。

胡正龙（1978—），男，博士，副教授。

作者简介:

徐利（1982—），女，硕士，讲师。

Pyrophotocatalytic Performance of g-C₃N₄/NaNbO₃ Composite Material for Degradation of Mixed Dyes

Li XU¹, Shuwen DENG², Xiaoju ZHOU³, Huifeng WANG³, Zhenglong HU³

Affiliations

^1.School of Mathematics, Physics and Optoelectronic Engineering, Hubei University of Automotive Technology, Shiyan 442002, Hubei, China

^2.Hubei Engineering Research Center for Big Data Application of Intelligent Emergency Services, Xianning 437100, Hubei, China

^3.School of electronic and Information Engineering, Hubei University of Science and Technology, Xianning 437100, Hubei, China

Corresponding Author:

DENG Shuwen (1979-), male, master, Associate Professor; E-mail: 5415112@qq.com;

HU Zhenglong (1978-), male, Ph.D., Associate Professor. huzhenglong@hbust.edu.cn

XU Li (1982-), female, master, Lecture. E-mail: Xu_lx@huat.edu.cn

出版时间: 2025-03-20 doi: 10.14062/j.issn.0454-5648.20240638

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摘要

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热释电效应诱导的热释电势已被证明是抑制载流子复合和促进电荷输运的有效策略之一。采用水热和烧结两步法制备了g-C₃N₄/NaNbO₃纳米棒复合材料。通过光照加冷热循环降解混合染料（酸性橙AO7、罗丹明RhB、甲基橙MO和亚甲基蓝MB），复合材料展现了优异的热释电光催化性能。结果表明，无需外部热源，经90 min 10次冷热循环，g-C₃N₄/NaNbO₃对混合染料的热释电光催化降解率达到96.9%，反应速率为0.038 6/min。此外，通过不同混合染料浓度、不同pH值、不同水源及5次重复使用的实验表明，复合催化剂具有强的环境适应性和稳定性。自由基探测实验表明，·O₂⁻、·OH和h⁺是反应中的活性物质，以·O₂⁻和·OH为主。根据捕获实验、Mott-Schottky曲线、密度泛函理论（DFT）计算表明，g-C₃N₄/NaNbO₃增强的热释电光催化活性归因于S型异质结的形成、g-C₃N₄和NaNbO₃之间的内建电场，以及热释电势导致的能带弯曲，加速了光生载流子的空间分离和迁移。这项工作表明g-C₃N₄/NaNbO₃复合材料是一种有前景的环保型热释电光催化剂，可以通过收集太阳能和昼夜温差热能来净化复杂的废水。

关键词

石墨相氮化碳/铌酸钠 / 热释电光催化 / 热释电势 / 复合材料 / 内建电场

Abstract

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Introduction

With the rapid development of industry, the discharge of dye wastewater from the textile and printing industries poses a huge threat to aquatic ecosystems and human health. Exploring efficient catalytic technologies to reduce water pollution is highly anticipated. Photocatalysis, as an efficient and environmentally friendly advanced oxidation technology for decomposing organic dyes, has attracted considerable attention. However, the low utilization rate of solar energy and severe photogenerated carrier recombination restrict the practical application of photocatalysis. In addition to solar energy, the thermal energy generated by cold-hot alternation can be also used as a clean and renewable energy source to induce positive and negative charges and generate pyroelectric potential, thereby achieving pyrocatalysis. Combining pyrocatalysis with photocatalysis can simultaneously collect solar energy and alternating heat energy, and the pyroelectric potential can serve as an internal driving force for dissociating photo generated exciton. This work constructed g-C₃N₄/NaNbO₃ composite materials for the absorption of g-C₃N₄ to visible light to enhance the utilization efficiency of sunlight. The Mott-Schottky curve was obtained by electrochemical workstation to analyze the conduction type and flat band potential of g-C₃N₄ and NaNbO.

Methods

A hydrated NaNbO₃ sample was obtained via hydrothermal reaction at 160 ℃ for 4 h with Nb₂O₅ and NaOH as raw materials. The hydrated NaNbO₃ prepared was then mixed, ground with a certain mass of melamine powder (in a mass ratio of 1∶2), and sintered at 500 ℃ for 2 h to obtain g-C₃N₄/NaNbO₃ composite material. The phase, morphology, and optical properties of the product was analyzed by X-ray diffraction (XRD), scanning electron microscopy (SEM), and ultraviolet-visible spectroscopy (UV-Vis). The pyrophotocatalytic performance of g-C₃N₄/NaNbO₃ composite materials was evaluated via degrading mixed dyes (i.e., methylene blue MB, methyl orange MO, rhodamine RhB, and acid orange AO7) under light irradiation and cold-hot cycling. The environmental adaptability of g-C₃N₄/NaNbO₃ composite materials was analyzed by changing the concentration, pH value, and water source of the mixed dye solution. The stability of g-C₃N₄/NaNbO₃ composite material was estimated through five repeated uses and the XRD patterns before and after use. The influence of g-C₃N₄/NaNbO₃ on the degradation performance of the mixed dyes was analyzed via adding different active substance trapping agents, and the main active species in the catalytic reaction was determined. The work function was calculated based on density functional theory (DFT) to analyze the electron transfer after contacting g-C₃N₄ and NaNbO₃.

Results and discussion

The g-C₃N₄/NaNbO₃ composite material prepared by a two-step method of hydrothermal and mixed sintering is sheet-like g-C₃N₄ covering the surface of NaNbO₃ nanorods with the diameters of 100-300 nm. The photocatalytic degradation efficiencies of g-C₃N₄, NaNbO₃, and g-C₃N₄/NaNbO₃ composite materials for RhB are 19%, 71%, and 84%, respectively. Combined with the pyroelectric catalysis, the photocatalytic efficiency of g-C₃N₄/NaNbO₃ increases to 97.3%. The results show that the formation of g-C₃N₄ and NaNbO₃ composites can enhance the photocatalytic performance, and the pyroelectric potential generated by temperature fluctuations can further separate the photo-generated electron hole pairs, thus improving the photocatalytic degradation efficiency. Under illumination and cold-hot cycling, g-C₃N₄/NaNbO₃ exhibits a pyrophotocatalytic degradation efficiency of 96.9% for mixed dyes, with a degradation reaction rate of 0.038 6 min^-1. The degradation efficiency of g-C₃N₄/NaNbO₃ decreases with the increase of initial concentrations of mixed dye solution (i.e., 2×10^-5 mol/L, 4×10^-5 mol/L, 6×10^-5 mol/L and 8×10^-5 mol/L). The pyro-photocatalytic degradation efficiency of the mixed dye is 96.9%, 70.8%, and 54.3% when the pH value of the solution is 2.6, 7.1 and 11, respectively, indicating that g-C₃N₄/NaNbO₃ composite catalyst is suitable for working in acidic and neutral environments. Also, g-C₃N₄/NaNbO₃ composite material has a better catalytic activity in deionized water and tap water, while its pyrophotocatalytic performance reduces in river water and lake water. The experimental results of adding sacrificial agents show that ·O₂^-, ·OH, and h⁺ are all active substances in the thermal electric photocatalytic degradation, among which ·O₂⁻ and ·OH play a particularly significant role in the catalytic degradation. The results of UV-Vis spectra, the Mott-Schottky curve and DFT calculations indicate that g-C₃N₄/NaNbO₃ composite material broadens the absorption range of the solar spectrum, forms an S-type heterojunction, and the pyroelectric potential generated by the pyroelectric effect promotes the dissociation of photo generated carriers, thus improving the pyrophotocatalytic performance.

Conclusions

The constructed g-C₃N₄/NaNbO₃ composite material utilized a wide solar spectral absorption range and a photothermal effect of g-C₃N₄. The formation of S-type heterojunction between g-C₃N₄ and NaNbO₃ was conducive to the separation and migration of photo generated carriers. Also, the pyroelectric potential induced by temperature fluctuation could result in band bending, and further promoted the separation of photo generated carriers in NaNbO₃, demonstrating an enhanced pyrophotocatalytic performance. This work could provide an efficient catalyst that simultaneously utilized solar energy and environmental thermal energy to achieve sewage treatment and environmental remediation.

Key words

graphitic carbon nitride/sodium niobate / pyrophotocatalysis / pyroelectric potential / composite material / build-in electric field

引用本文

徐利, 邓树文, 周小桔, 王会峰, 胡正龙. g-C₃N₄/NaNbO₃复合材料降解混合染料的热释电光催化性能. 硅酸盐学报, 2025 , 53 (3) : 594 -606 . DOI: 10.14062/j.issn.0454-5648.20240638

Li XU, Shuwen DENG, Xiaoju ZHOU, Huifeng WANG, Zhenglong HU. Pyrophotocatalytic Performance of g-C₃N₄/NaNbO₃ Composite Material for Degradation of Mixed Dyes[J]. Journal of the Chinese Ceramic Society, 2025 , 53 (3) : 594 -606 . DOI: 10.14062/j.issn.0454-5648.20240638

基金

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国家自然科学基金(12304539)
湖北科技学院博士科研启动基金(BK202316)
湖北科技学院科研项目(2020-22GP08; 2024-2025X08)

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2025年第53卷第3期

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文章信息

doi: 10.14062/j.issn.0454-5648.20240638

接收时间：2024-10-08
首发时间：2026-10-22
出版时间：2025-03-20

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收稿日期：2024-10-08
修回日期：2024-10-24

基金

国家自然科学基金(12304539)

湖北科技学院博士科研启动基金(BK202316)

湖北科技学院科研项目(2020-22GP08; 2024-2025X08)

作者信息

^1．湖北汽车工业学院，数理与光电工程学院，湖北十堰 442002

^2．湖北科技学院，智能应急服务大数据应用湖北省工程研究中心，湖北咸宁 437100

^3．湖北科技学院，电子与信息工程学院，湖北咸宁 437100

通讯作者:

邓树文（1979—），男，硕士，副教授。

胡正龙（1978—），男，博士，副教授。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20240638

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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