复合微量NCQDs对提高Ag<sub>2</sub>CO<sub>3</sub>半导体降解苯酚的光催化性能研究

引用本文: 田坚, 刘仁月, 刘珍, 余长林, 刘敏超. 复合微量NCQDs对提高Ag₂CO₃半导体降解苯酚的光催化性能研究[J]. 催化学报, 2017, 38(12): 1999-2008. doi: 10.1016/S1872-2067(17)62926-7 shu

Citation: Jian Tian, Renyue Liu, Zhen Liu, Changlin Yu, Minchao Liu. Boosting the photocatalytic performance of Ag₂CO₃ crystals in phenol degradation via coupling with trace N-CQDs[J]. Chinese Journal of Catalysis, 2017, 38(12): 1999-2008. doi: 10.1016/S1872-2067(17)62926-7 shu

复合微量NCQDs对提高Ag₂CO₃半导体降解苯酚的光催化性能研究

a 江西理工大学冶金与化学工程学院, 江西赣州 341000;
b 五邑大学化学与环境工程学院, 广东江门 529020;
c 福州大学能源与环境光催化国家重点实验室, 福建福州 350002
基金项目:
国家自然科学基金（21567008，21607064，21707055）；江西理工大学清江拔尖人才培养计划；江西省5511科技创新人才项目（20165BCB18014）；江西省主要学科学术带头人培养计划（20172BCB22018）；江西省自然科学基金（20161BAB203090）.

摘要: 半导体光催化具有无毒、无污染、低能耗等优点，广泛应用于水溶液中染料、药物分子的降解等.其中Ag₂CO₃半导体因其较窄的带隙能和显著的可见光吸收性能而引起广泛关注.但是Ag₂CO₃在光照下极不稳定.目前，主要是通过引入其它半导体等材料与其进行复合来提其催化活性与稳定性.
本文以一种具有良好的水溶性以及能够加快电子转移能力的碳量子点（CQDs）和氮掺杂的碳量子点（NCQDs）作为复合材料，利用简单的沉淀法制备出了CQDs/Ag₂CO₃、NCQDs/Ag₂CO₃等复合材料.结果表明，CQDs和NCQDs的存在能够很好的提升光催化性能.而且发现NCQDs除了具有碳量子点的特性外，还能够诱导电荷离域，更加有效的促进电子的转移.利用X射线衍射、扫描电镜、透射电镜、N₂物理吸附、元素成像、紫外-可见光漫反射吸收光谱、红外光谱以及光电流和交流阻抗测试等手段对所制备的CQDs/Ag₂CO₃和NCQDs/Ag₂CO₃进行了表征.结果表明，量子点的存在能够有效增大Ag₂CO₃的比表面积.紫外-可见漫反射吸收结果说明，量子点的存在还能够在一定程度上增大样品的可见光吸收性能.而光电流和交流阻抗测试结果证明，量子点的存在能显著降低载流子的迁移阻力，提高光生电子与空穴的分离效率.在量子点相同含量下，NCQDs能够更加有效的转移载流子.以350 W氙灯加可见光滤光片（λ ≥ 420 nm）作为光源进行光催化降解苯酚的性能测试.结果表明，NCQDs/Ag₂CO₃比CQDs/Ag₂CO₃表现出更高的活性，其对苯酚的降解率约为后者的2倍；同时NCQDs/Ag₂CO₃还具有更佳的稳定性能.自由基捕获试验说明，在光催化过程中，主要的活性物种为·OH与·O₂^-.NCQDs能够提高Ag₂CO₃活性与稳定性的原因在于，NCQDs能够提高了催化剂的比表面积，增强光催化剂的光吸收性能.另外NCQDs能够比CQDs更有效的转移电子，提高光生e^-和h⁺的分离效率，产生更多的光催化降解活性物种.

关键词:

English

Boosting the photocatalytic performance of Ag₂CO₃ crystals in phenol degradation via coupling with trace N-CQDs

a School of Metallurgy and Chemical Engineering, Jiangxi University of Science and Technology, Ganzhou 341000, Jiangxi, China;
b School of Chemistry and Environmental Engineering, Wuyi University, Jiangmen 529020, Guangdong, China;
c State Key Laboratory of Photocatalysis on Energy and Environment, Fuzhou University, Fuzhou 350002, Fujian, China
Received Date: 04 September 2017
Revised Date: 09 October 2017
Fund Project:
This was supported by the National Natural Science Foundation of China (21567008, 21607064, 21707055), Program of Qingjiang Excellent Young Talents, Jiangxi University of Science and Technology, Program of 5511 Talents in Scientific and Technological Innovation of Jiangxi Province (20165BCB18014), Academic and Technical Leaders of the Main Disciplines in Jiangxi Province (20172BCB22018), and Jiangxi Province Natural Science Foundation (20161BAB203090).

Abstract: A series of N-CQDs/Ag₂CO₃ composite crystals (where N-CQDs=Nitrogen doped carbon quantum dots) were prepared by adding different volumes of a solution of N-CQDs during Ag₂CO₃ crystal growth. Under irradiation from a 350-W Xe lamp light (with optical filter, λ ≥ 420 nm), the performance of N-CQDs/Ag₂CO₃ in photocatalytic degradation of phenol was evaluated. The as-prepared samples were analyzed by XRD, SEM, TEM, BET, element mapping, UV-vis DRS, FT-IR, XPS, transient photocurrent response and EIS testing. The results showed that after coupling with trace amounts of N-CQDs, both the photocatalytic activity and stability of Ag₂CO₃ were greatly boosted. The addition of N-CQDs solution influenced the crystallization of Ag₂CO₃, resulting in a distinct decrease in Ag₂CO₃ crystal size and an obvious increase in surface area. Moreover, the charge transfer resistance was greatly reduced, and the separation efficiency of photogenerated electrons and holes was strongly promoted. The presence of NCQDs on the surface of the catalysts facilitates the transfer of photogenerated electrons, slowing the photocorrosion rate of Ag₂CO₃, and then resulting in higher stability than bare Ag₂CO₃ in degradation. The synergistic effect of the improvement of morphology and charge transfer rate thus accounted for the superior photocatalytic performance of N-CQDs/Ag₂CO₃.

Key words:

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复合微量NCQDs对提高Ag₂CO₃半导体降解苯酚的光催化性能研究

English

Boosting the photocatalytic performance of Ag₂CO₃ crystals in phenol degradation via coupling with trace N-CQDs

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