硫酸根对聚合氮化碳光催化活性的影响
收稿日期: 2022-01-06
网络出版日期: 2022-09-22
基金资助
国家自然科学基金项目(21601171)
Effect of sulfate on photocatalytic activity of polymerized carbon nitride
Received date: 2022-01-06
Online published: 2022-09-22
在pH=1条件下分别加入硫酸根、硝酸根、磷酸根对三聚氰胺进行处理,采用高温煅烧法制备了一系列聚合氮化碳材料,并通过X射线衍射(XRD)、扫描电子显微镜(SEM)、紫外-可见漫反射光谱(UV-Vis DRS)等分析手段对样品进行了表征。以罗丹明B(RhB)为污染物,探究了在可见光下聚合氮化碳对RhB的光催化降解性能、稳定性以及降解机理。加入0.12 mol硫酸根处理的聚合氮化碳(CN-0.04SO42-)在45 min内对RhB的降解率为99.1%,其伪一级动力学常数是未加硫酸根的23.0倍,硫酸根能有效地增强聚合氮化碳的光催化活性。CN-0.04SO42-经过3次循环实验对RhB的降解率略有下降,说明其具有良好的稳定性。活性物种捕获实验表明,影响光催化降解RhB的主要活性物种是·O2-和·OH。
马炳香 , 申云霞 , 李娜 , 李敏 , 韦尧意 , 赵宇 . 硫酸根对聚合氮化碳光催化活性的影响[J]. 无机盐工业, 2022 , 54(9) : 150 -157 . DOI: 10.19964/j.issn.1006-4990.2022-0009
A series of polymerized carbon nitride were prepared by high temperature calcination method after the treatment of melamine with adding SO42-,NO3- and PO43- under the condition of pH=1,respectively.The samples were characterized by X-ray diffraction(XRD),scanning electron microscopy(SEM),UV-Visible diffuse reflectance spectroscopy(UV-Vis DRS),etc.Using rhodamine B(RhB) as pollutant,the photocatalytic degradation activity,stability and degradation mechanism of polymerized carbon nitride were explored under visible light.The degradation of RhB by polymerized carbon nitride(CN-0.04SO42-) with 0.12 mol SO42- was 99.1% within 45 min,and its pseudo?first?order kinetic constant was 23.0 times greater than that of no SO42-.SO42-,which could effectively enhance the photocatalytic activity of polymerized carbon nitride.The degradation of CN-0.04SO42- was decreased slightly after three cycles,indicating that it had good stability.Active species capture experiment showed that ·O2- and ·OH were the main active species affecting photocatalytic degradation of RhB.
Key words: carbon nitride; photocatalytic; degradation
| [1] | ONG W J, TAN L L, NG Y H, et al.Graphitic carbon nitride(g-C3N4)-based photocatalysts for artificial photosynthesis and environmental remediation:Are we a step closer to achieving sustainability?[J].Chemical Reviews,2016,116(12):7159-7329. |
| [2] | PELAEZ M, NOLAN N T, PILLAI S C, et al.A review on the visible light active titanium dioxide photocatalysts for environmental applications[J].Applied Catalysis B:Environmental,2012,125:331-349. |
| [3] | WEN Jiuqing, XIE Jun, CHEN Xiaobo, et al.A review on g-C3N4-based photocatalysts[J].Applied Surface Science,2017,391:72-123. |
| [4] | GAO Shuying, WANG Xuyu, SONG Changjian, et al.Engineering carbon-defects on ultrathin g-C3N4 allows one?pot output and dramatically boosts photoredox catalytic activity[J].Applied Catalysis B:Environmental,2021,295.Doi:0.1016/j.apcatb.2021.120272. |
| [5] | LI Xiaogang, BI Wentuan, ZHANG Lei, et al.Single?atom Pt as co?catalyst for enhanced photocatalytic H2 evolution[J].Advanced Materials:Deerfield Beach,Fla.,2016,28(12):2427-2431. |
| [6] | FU Junwei, XU Quanlong,LOW J,et al.Ultrathin 2D/2D WO3/g-C3N4 step?scheme H2-production photocatalyst[J].Applied Catalysis B:Environmental,2019,243:556-565. |
| [7] | MENG Fanpeng, WANG Jun, TIAN Wenjie, et al.Graphitic carbon nitride nanosheets via acid pretreatments for promoted photocatalysis toward degradation of organic pollutants[J].Journal of Colloid and Interface Science,2022,608:1334-1347. |
| [8] | 李佳慧,李克艳,宋春山,等.聚合氮化碳的制备、改性及光催化还原二氧化碳性能研究[J].无机盐工业,2021,53(12):21-28. |
| [8] | LI Jiahui, LI Keyan, SONG Chunshan, et al.Study on preparation,modification and carbon dioxide photocatalytic reduction performance of polymeric carbon nitride[J].Inorganic Chemicals Industry,2021,53(12):21-28. |
| [9] | WANG Longyan, HONG Yuanzhi, LIU Enli, et al.A bottom?up acidification strategy engineered ultrathin g-C3N4 nanosheets towards boosting photocatalytic hydrogen evolution[J].Carbon,2020,163:234-243. |
| [10] | HUANG Zhijun, LI Fengbo, CHEN Bingfeng, et al.Porous and low-defected graphitic carbon nitride nanotubes for efficient hydrogen evolution under visible light irradiation[J].RSC Advances,2015,5(124):102700-102706. |
| [11] | TANG Yunqi, YUAN Meng, JIANG Baojiang, et al.Inorganic acid-derived hydrogen?bonded organic frameworks to form nitro?gen?rich carbon nitrides for photocatalytic hydrogen evolution[J].Journal of Materials Chemistry A,2017,5(41):21979-21985. |
| [12] | ZHOU Chengyun, LAI Cui, HUANG Danlian, et al.Highly porous carbon nitride by supramolecular preassembly of monomers for photocatalytic removal of sulfamethazine under visible light driven[J].Applied Catalysis B:Environmental,2018,220:202-210. |
| [13] | NIU Ping, ZHANG Lili, LIU Gang, et al.Graphene?like carbon nitride nanosheets for improved photocatalytic activities[J].Advanced Functional Materials,2012,22(22):4763-4770. |
| [14] | LIN Qiuyan, LI Li, LIANG Shijing, et al.Efficient synthesis of monolayer carbon nitride 2D nanosheet with tunable concentration and enhanced visible?light photocatalytic activities[J].Applied Catalysis B:Environmental,2015,163:135-142. |
| [15] | LIU Chuang, DONG Xiaoli, HAO Yuchen, et al.A novel supramolecular preorganization route for improving g-C3N4/g-C3N4 metal?free homojunction photocatalysis[J].New Journal of Chemistry,2017,41(20):11872-11880. |
| [16] | ZHOU Chengyun, ZENG Zhuotong, ZENG Guangming, et al.Visible?light?driven photocatalytic degradation of sulfamethazine by surface engineering of carbon nitride:Properties,degradation pathway and mechanisms[J].Journal of Hazardous Materials,2019,380.Doi:10.1016/j.jhazmat.2019.120815. |
| [17] | TONG Jincheng, ZHANG Li, LI Fei, et al.An efficient top-down approach for the fabrication of large?aspect?ratio g-C3N4 nano?sheets with enhanced photocatalytic activities[J].Physical Chemistry Chemical Physics:PCCP,2015,17(36):23532-23537. |
| [18] | CUI Yanjuan, TANG Yubin, WANG Xinchen.Template?free synthesis of graphitic carbon nitride hollow spheres for photocatalytic degradation of organic pollutants[J].Materials Letters,2015, 161:197-200. |
| [19] | CUI Yanjuan, DING Zhengxin, FU Xianzhi, et al.Construction of conjugated carbon nitride nanoarchitectures in solution at low temperatures for photoredox catalysis[J].Angewandte Chemie:International Ed.in English,2012,51(47):11814-11818. |
| [20] | LI Xibao, KANG Bangbang, DONG Fan, et al.Enhanced photocatalytic degradation and H2/H2O2 production performance of S-pCN/WO2.72 S-scheme heterojunction with appropriate surface oxygen vacancies[J].Nano Energy,2021,81.Doi:10.1016/j.nanoen.2020.105671. |
| [21] | LAN Huachun, LI Lili, AN Xiaoqiang, et al.Microstructure of carbon nitride affecting synergetic photocatalytic activity:Hydrogen bonds vs.structural defects[J].Applied Catalysis B:Environmental,2017,204:49-57. |
| [22] | YU Kai, YANG Shaogui, HE Huan, et al.Visible light-driven photocatalytic degradation of rhodamine B over NaBiO3:Pathways and mechanism[J].The Journal of Physical Chemistry A,2009,113(37):10024-10032. |
| [23] | HU Shaozheng, MA Lin, YOU Jiguang, et al.Enhanced visible light photocatalytic performance of g-C3N4 photocatalysts co?do?ped with iron and phosphorus[J].Applied Surface Science,2014, 311:164-171. |
| [24] | 班昌胜,李军,金央,等.超分子前体制备g-C3N4/g-C3N4同质结及光催化性能研究[J].无机盐工业,2022,54(3):125-131. |
| [24] | BAN Changsheng, LI Jun, JIN Yang, et al.Study on preparation of g-C3N4/g-C3N4 homojunction by supramolecular precursor and its photocatalytic property[J].Inorganic Chemicals Industry,2022,54(3):125-131. |
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