升温速率对尿素热解制g-C3N4光催化剂构效影响研究
收稿日期: 2021-05-11
网络出版日期: 2022-04-18
基金资助
国家自然科学基金(21978181)
Study on effect of heating rate on structure-activity of g-C3N4 photocatalyst by pyrolysis of urea
Received date: 2021-05-11
Online published: 2022-04-18
尿素热解可制备高附加值下游产品石墨相氮化碳（g-C3N4）,热解条件显著影响其光催化性能。以工业级尿素为前驱体,考察了升温速率对产物g-C3N4结构和光催化性能的影响,并用于光催化氧化降解有机染料和光催化还原生产双氧水。结果表明,快速升温（15 ℃/min）所得g-C3N4（GCN-15）结晶度高、无定型结构少、带隙窄、光利用率高、共轭结构完整,利于光生电子传递,因此具有更好的光催化性能。其对罗丹明B（RhB）和亚甲基蓝（MB）光氧化降解速率分别是慢速升温（2 ℃/min）所得g-C3N4（GCN-2）的4倍和2倍,8 h光还原双氧水产量提高18.37%。
杨文博 , 吴潘 , 何坚 , 刘长军 , 蒋炜 . 升温速率对尿素热解制g-C3N4光催化剂构效影响研究[J]. 无机盐工业, 2022 , 54(4) : 169 -174 . DOI: 10.19964/j.issn.1006-4990.2021-0310
High value added downstream products graphitic carbon nitride（g-C3N4） can be prepared by pyrolysis of urea,but its photocatalytic performance is significantly affected by pyrolysis conditions.Industrial grade urea was used as precursor,the effect of heating rate on the structure and photocatalytic performance of g-C3N4 was investigated,and g-C3N4 was used for photocatalytic oxidation degradation of organic dyes and photocatalytic reduction to produce H2O2.The results showed that g-C3N4（GCN-15） with rapid heating rate（15 °C/min） had high crystallinity,less amorphous structure,more complete conjugated structure and narrow band gap,which was beneficial to the transfer of photogenerated electrons and the improvement of photocatalytic performance.The photodegradation rates of RhB and MB by GCN-15 were 4 and 2 times higher than those by GCN-2,respectively,and the yield of H2O2 produced in 8 hours was increased by 18.37%.
| [1] | ONG W J, TAN L L, NG Y H, et al. Graphitic carbon nitride(g-C3N4)-based photocatalysts for artificial photosynjournal and environmental remediation:Are we a step closer to achieving sustainability?[J]. Chemical Reviews, 2016, 116(12):7159-7329. |
| [2] | CHEN Zhongshan, ZHANG Sai, LIU Yang, et al. Synjournal and fabrication of g-C3N4-based materials and their application in elimination of pollutants[J]. Science of the Total Environment, 2020, 731.Doi: 10.1016/j.scitotenv.2020.139054. |
| [3] | HAO Qiang, JIA Guohua, WEI Wei, et al. Graphitic carbon nitride with different dimensionalities for energy and environmental applications[J]. Nano Research, 2019, 13(1):18-37. |
| [4] | 孙海杰, 刘欣改, 陈志浩, 等. BiOI/g-C3N4光催化降解甲基橙研究[J]. 无机盐工业, 2021, 53(4):90-94. |
| [5] | PANNERI S, GANGULY P, NAIR B N, et al. Role of precursors on the photophysical properties of carbon nitride and its application for antibiotic degradation[J]. Environ.Sci.Pollut.Res., 2017, 24(9):8609-8618. |
| [6] | ZHENG Yu, ZHANG Zisheng, LI Chunhu. A comparison of graphitic carbon nitrides synthesized from different precursors through pyrolysis[J]. J.Photochem.Photobiol.A:Chem., 2017, 332:32-44. |
| [7] | DONG Fan, WU Liwen, SUN Yanjun, et al. Efficient synjournal of polymeric g-C3N4 layered materials as novel efficient visible light driven photocatalysts[J]. Journal of Materials Chemistry, 2011, 21:15171-15174. |
| [8] | YAO Shanshan, XUE Sikang, PENG Sihuang, et al. Synjournal of graphitic carbon nitride at different thermal-pyrolysis temperature of urea and it application in lithium-sulfur batteries[J]. Journal of Materials Science:Materials in Electronics, 2018, 29(20):17921-17930. |
| [9] | DEVINA R P, RISHABH S, NEHRA S P, et al. Effect of calcination temperature,pH and catalyst loading on photodegradation efficiency of urea derived graphitic carbon nitride towards methylene blue dye solution[J]. RSC Advances, 2019, 9:15381-15391. |
| [10] | YUAN Yupeng, XU Wentao, YIN Lisha, et al. Large impact of heating time on physical properties and photocatalytic H2 production of g-C3N4 nanosheets synthesized through urea polymerization in Ar atmosphere[J]. International Jouranl of Hydrogen Energy, 2013, 38(30):13159-13163. |
| [11] | NOSAKA Y, NOSAKA A Y. Generation and detection of reactive oxygen species in photocatalysis[J]. Chemical Reviews, 2017, 117(17):11302-11336. |
| [12] | WANG Y, WANG X, ANTONIETTI M. Polymeric graphitic carbon nitride as a heterogeneous organocatalyst:From photochemistry to multipurpose catalysis to sustainable chemistry[J]. Angew.Chem. Int.Ed.Engl., 2012, 51(1):68-89. |
| [13] | ZHU Junjiang, XIAO Ping, LI Hailong, et al. Graphitic carbon nitride:Synjournal,properties,and applications in catalysis[J]. ACS Applied Materials & Interfaces, 2014, 6(19):16449-16465. |
| [14] | YANG Jian, LIANG Yujun, LI Kai, et al. One-step synjournal of novel K+ and cyano groups decorated triazine-/heptazine-based g-C3N4 tubular homojunctions for boosting photocatalytic H2 evolution[J]. Applied Catalysis B:Environmental, 2020, 262:1-12. |
| [15] | ZHANG Jinshui, ZHANG Mingwen, YANG Can, et al. Nanospherical carbon nitride frameworks with sharp edges accelerating charge collection and separation at a soft photocatalytic interface[J]. Adv.Mater., 2014, 26(24):4121-4126. |
| [16] | XING Weinan, TU Wenguang, HAN Zhonghui, et al. Template-induced high-crystalline g-C3N4 nanosheets for enhanced photocatalytic H2 evolution[J]. ACS Energy Letters, 2018, 3(3):514-519. |
| [17] | IQBAL W, QIU B, ZHU Q, et al. Self-modified breaking hydrogen bonds to highly crystalline graphitic carbon nitrides nanosheets for drastically enhanced hydrogen production[J]. Appl.Catal.B: Environ., 2018, 232:306-313. |
| [18] | GUTZLER R. Band-structure engineering in conjugated 2D polymers[J]. Phys.Chem.Chem.Phys., 2016, 18(42):29092-29100. |
| [19] | SAMANTA S, YADAV R, KUMAR A, et al. Surface modified C,O co-doped polymeric g-C3N4 as an efficient photocatalyst for visible light assisted CO2 reduction and H2O2 production[J]. Applied Catalysis B:Environmental, 2019, 259:1-19. |
| [20] | ZHANG Hao, JIA Luhan, WU Pan, et al. Improved H2O2 photogeneration by KOH-doped g-C3N4 under visible light irradiation due to synergistic effect of N defects and K modification[J]. Applied Surface Science, 2020, 527:1-11. |
| [21] | JI Xueqiang, YUAN Xiaohong, WU Jiajie, et al. Tuning the photocatalytic activity of graphitic carbon nitride by plasma-based surface modification[J]. ACS Applied Materials & Interfaces, 2017, 9(29):24616-24624. |
| [22] | DONG Guohui, HO Wingkei, WANG Chuanyi. Selective photocatalytic N2 fixation dependent on g-C3N4 induced by nitrogen vacancies[J]. Journal of Materials Chemistry A, 2015, 3(46):23435-23441. |
| [23] | XIE Yao, LI Yunxiang, HUANG Zhaohui, et al. Two types of cooperative nitrogen vacancies in polymeric carbon nitride for efficient solar-driven H2O2 evolution[J]. Applied Catalysis B:Environmental, 2020, 265:1-7. |
| [24] | JAISWAL M, MENON R. Polymer electronic materials:A review of charge transport[J]. Polymer International, 2006, 55(12):1371-1384. |
| [25] | 赵洪霞, 沈晨, 陈秀英, 等. 基于EPR技术的5种纳米金属氧化物光生活性物种的形成研究[J]. 环境科学学报, 2017, 37(7):2609-2615. |
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