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简便制备磷掺杂超薄石墨相氮化碳纳米片和五氧化二铋复合材料的无介体型 Z 型光催化剂,可见光下增强四环素的降解。

Facile fabrication of mediator-free Z-scheme photocatalyst of phosphorous-doped ultrathin graphitic carbon nitride nanosheets and bismuth vanadate composites with enhanced tetracycline degradation under visible light.

机构信息

College of Environmental Science and Engineering, Hunan University, Changsha 410082, China; Key Laboratory of Environmental Biology and Pollution Control, Hunan University, Ministry of Education, Changsha 410082, China.

College of Environmental Science and Engineering, Hunan University, Changsha 410082, China; Key Laboratory of Environmental Biology and Pollution Control, Hunan University, Ministry of Education, Changsha 410082, China.

出版信息

J Colloid Interface Sci. 2018 Jan 1;509:219-234. doi: 10.1016/j.jcis.2017.09.016. Epub 2017 Sep 7.

Abstract

To realize the sustainable employment of solar energy in contaminant degradation and environmental recovery, design and development of an efficient photocatalyst is urgently needed. Herein, a novel direct Z-scheme composite photocatalysts consist of phosphorous-doped ultrathin g-CN nanosheets (PCNS) and bismuth vanadate (BiVO) are developed via a one-pot impregnated precipitation method. The as-prepared hybrid nanocomposite was utilized for the degradation tetracycline (TC) under visible light irradiation. Among the composites with various PCNS/BiVO ratios, the prepared PCNS/BVO-400 photocatalyst presents the best performance, showing a TC (10mg/L) removal efficiency of 96.95% within 60min, more than double that of pristine BiVO (41.45%) and higher than that of pure PCNS (71.78%) under the same conditions. The effects of initial TC concentration, catalyst dosage, pH value and different water sources have been studied in detail. The improved photocatalytic performance of the as-prepared PCNS/BiVO nanocomposites could be attributed to the promoted separation efficiency of the photogenerated electrons and the enhanced charge carrier lifetime (1.65ns) owing to the synergistic effect between the PCNS and BiVO. The degradation intermediates and decomposition pathway of TC were also analyzed and proposed. Additionally, radical trapping experiments and ESR measurement indicated that the photogenerated holes (h), superoxide radical (O) and hydroxyl radical (OH) all participated in the TC removal procedure in the reaction system. The high performance of PCNS/BVO-400 in real wastewater indicated the potential of the prepared composite in practical application. This work provides an efficient and promising approach for the formation of high performance Z-scheme photocatalyst and study the possibility for real wastewater treatment.

摘要

为了实现太阳能在污染物降解和环境修复中的可持续利用,迫切需要设计和开发高效的光催化剂。在此,通过一锅浸渍沉淀法制备了一种新型的直接 Z 型复合光催化剂,由磷掺杂的超薄 g-CN 纳米片(PCNS)和五氧化二铋(BiVO)组成。所制备的杂化纳米复合材料用于可见光照射下四环素(TC)的降解。在所制备的具有不同 PCNS/BiVO 比例的复合材料中,制备的 PCNS/BVO-400 光催化剂表现出最佳性能,在 60min 内可将 10mg/L 的 TC 去除效率达到 96.95%,在相同条件下,比原始 BiVO(41.45%)提高了一倍以上,比纯 PCNS(71.78%)更高。详细研究了初始 TC 浓度、催化剂用量、pH 值和不同水源对其的影响。所制备的 PCNS/BiVO 纳米复合材料的光催化性能提高归因于光生电子的分离效率提高和载流子寿命(1.65ns)增强,这归因于 PCNS 和 BiVO 之间的协同效应。还分析并提出了 TC 的降解中间产物和分解途径。此外,自由基捕获实验和 ESR 测量表明,在反应体系中,光生空穴(h)、超氧自由基(O)和羟基自由基(OH)都参与了 TC 的去除过程。PCNS/BVO-400 在实际废水中的高性能表明了所制备的复合材料在实际应用中的潜力。这项工作为形成高性能 Z 型光催化剂提供了一种高效、有前景的方法,并研究了在实际废水处理中的可能性。

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