无机材料学报

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SiO2增强自敏性氮化碳微球及可见光光降解盐酸四环素研究

曹青青, 陈翔宇, 吴健豪, 王筱卓, 王乙炫, 王禹涵, 李春颜, 茹菲, 李兰, 陈智   

  1. 中国计量大学 材料化学学院, 杭州 310018
  • 收稿日期:2024-01-04 修回日期:2024-03-03 出版日期:2024-03-08 网络出版日期:2024-03-08
  • 作者简介:曹青青(2000-), 女, 硕士研究生. E-mail: 2024225003@qq.com.
  • 基金资助:
    国家重点研发计划项目(2023YFF0612600); 浙江省尖兵领雁项目(2023C02038); 宁波市重大科技任务攻关项目(2022Z178); 中建股份科技重点研发项目(CSCEC-2021-Z-5); 国家级大学生创新创业训练计划资助项目(202210356009); 浙江省高分子材料表界面重点实验室开放基金(SISPM-2022-03)

Enhanced Visible-light Photodegradation of TC-HCl on Self-sensitive Carbon-nitride Microspheres by Introducing SiO2

CAO Qingqing, CHEN Xiangyu, WU Jianhao, WANG Xiaozhuo, WANG Yixuan, WANG Yuhan, LI Chunyan, RU Fei, LI Lan, CHEN Zhi   

  1. College of Materials and Chemistry, China Jiliang University, Hangzhou 310018, China
  • Received:2024-01-04 Revised:2024-03-03 Published:2024-03-08 Online:2024-03-08
  • About author:CAO Qingqing (2000-), female, Master candidate. E-mail: 2024225003@qq.com

摘要: 光催化技术在水中新污染物的治理中应用广泛。自敏性氮化碳(SSCN)是一种新型的非金属光催化剂, 其表面的自敏性高分子可以有效地拓宽可见光吸收范围, 但该材料存在严重的团聚现象, 抑制了其光催化活性和稳定性。SiO2的分散性好, 被广泛用作载体构建复合结构应用于光催化领域。本研究首先用Stöber法制备了SiO2微球, 随后利用水热法原位合成了SiO2/SSCN复合材料。采用多种表征手段对样品的物相结构、微观形貌、光电性能进行了分析。制备的复合材料应用于光催化降解水中盐酸四环素, 并表现出增强的降解活性, 其活性与SiO2加入量密切相关, 当SiO2与SSCN的质量比为0.04:1时, 复合材料的光催化活性和稳定性最佳, 光照60 min可降解42%的盐酸四环素, 经5次循环后其光催化效率仍然能够维持在约38%。引入的SiO2为SSCN提供分散位点, 改善了SSCN较为严重的团聚现象, 使SSCN表面TBO能够快速分解至表面活性位点暴露的最佳含量, 提升了SSCN对可见光的利用率, 促进了光生电荷的分离效率, 从而有效地提升了SSCN的光催化活性及稳定性。本研究为优化催化剂的光催化活性和提高稳定性及新污染物治理应用提供一个新思路。

关键词: 自敏性氮化碳, 二氧化硅, 光催化, 新污染物治理, 活性增强

Abstract: Photocatalysis is widely employed to treat emerging pollutants in water, due to its well-organized attributes. Self-sensitive carbon nitride (SSCN) represents a novel class of non-metallic photocatalyst that has garnered significant attention for its distinctive properties, which contrast with traditional graphitic carbon nitride (g-C3N4). The macromolecule surface layer can effectively extend the range of visible light absorption. Nevertheless, severe agglomeration constrains its photocatalytic efficacy and stability. SiO2 sphere material, known for their excellent dispersibility, have been extensively utilized as catalyst support to construct composite structures for photocatalytic application. In this work, SiO2 microspheres were initially synthesized by the Stöber method, followed by the preparation of SiO2/SSCN composites through an in-situ hydrothermal process. The microstructure, phase structure, and photoelectric properties of the samples were systematically investigated using a combination of characterization techniques. It is discovered that the SiO2 within the composites effectively disperses the SSCN. The resulting composite material was applied to the photocatalytic degradation of antibiotic pollutants in water, exhibiting enhanced degradation activity. The activity was closely correlated with the quantity of SiO2. At mass ratio of SiO2 to SSCN of 0.04:1, the composite achieved optimal photocatalytic activity and demonstrated good stability. After 60 min of irradiation, 42% of tetracycline hydrochloride was degraded, and the photocatalytic efficiency remained at 38% after 5 cycles. The incorporation of the SiO2 component offers supplementary sites for the dispersion of SSCN, mitigating serious agglomeration phenomenon of SSCN. This facilitates the rapid decomposition of TBO on the surface of SSCN under light irradiation, allowing the achievement of the optimal content of TBO on surface active sites. Consequently, the utilization efficiency of visible light on SSCN is significantly improved, and a higher separation rate of photogenerated electron-hole pairs is simultaneously observed. These attributes culminate in significantly improved photocatalytic activity for the degradation of tetracycline hydrochloride on SSCN under visible light irradiation. These advantages may position the as-synthesized SiO2 dispersed SSCN as prospective candidate for practical application. This research offers a novel route for enhancing the photocatalytic activity and stability of catalysts.

Key words: self-sensitive carbon nitride, silicon dioxide, photocatalysis, new pollutant treatment, enhanced activity

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