摘要
以盐酸胍为前驱体、Zr(NO_(3))_(4)·5H_(2)O为锆源,通过热聚合法制备了Zr掺杂g-C_(3)N_(4)光催化剂(Zr/g-C_(3)N_(4))。采用XRD、SEM、UV-Vis DRS、PL、XPS、N_(2)吸附-脱附对催化剂的结构、形貌、光学性能进行了表征与分析。结果表明,掺杂后的Zr/g-C_(3)N_(4)光催化剂拓宽了可见光的吸收,增大了比表面积,且降低了光生电子-空穴的复合,具有较好的光催化活性。在可见光照射下,60 min内,5Zr/g-C_(3)N_(4)[即Zr(NO_(3))_(4)·5H_(2)O质量为盐酸胍质量的5%]对罗丹明B(RhB)的光催化降解率达99.29%,光催化降解过程符合一级动力学方程,其速率常数为0.08647 min^(-1),约是纯g-C_(3)N_(4)的8.3倍。此外,5Zr/g-C_(3)N_(4)对甲基橙和盐酸四环素也表现出良好的光催化性能,在60 min内对二者的降解率分别为98.02%和84.47%(5Zr/g-C_(3)N_(4)降解RhB、MO及TC-HCl的投加量均为0.05 g,且均未调整溶液pH)。降解Rh B的主要活性物种为超氧自由基,并推测了可能的反应机理。
Zr-doped g-C_(3)N_(4)photocatalysts (Zr/g-C_(3)N_(4)) were prepared by thermal polymerization of guanidine hydrochloride and Zr(NO_(3))_(4)·5H_(2)O.The structure,morphology,and optical properties of the catalysts synthesized were then characterized and analyzed by XRD,SEM,UV-Vis DRS,PL,XPS and N_(2) adsorption-desorption.The results showed that the doped Zr/g-C_(3)N_(4)photocatalysts,leading to wider visible-light absorption range,increasing the specific surface area,and reducing the recombination of photogenerated electron-hole pairs,demonstrated good photocatalytic activity.The photocatalytic degradation rate of rhodamine B (RhB) by 5Zr/g-C_(3)N_(4)[Zr(NO_(3))_(4)·5H_(2)O was 5%of the mass of guanidine hydrochloride]reached 99.29%within 60 min under visible-light irradiation.Furthermore,the photocatalytic degradation process conformed to the first-order kinetic equation,and the rate constant was 0.08647 min^(-1),8.3-fold that of pure g-C_(3)N_(4).Meanwhile,5Zr/g-C_(3)N_(4)also exhibited excellent photocatalytic performance for methyl orange(MO) and tetracycline hydrochloride(TC-HCl) degradation,with degradation rates of 98.02%and 84.47%within 60 min,respectively (the dosage of 5Zr/g-C_(3)N_(4)for the degradation of RhB,MO and TC-HCl was 0.05 g,and the pH of the solution was not adjusted).It was found that the main active species involved in RhB degradation was superoxide radical,based on which the possible reaction mechanism was speculated.
作者
张仰全
李龙飞
周峰
苑兴洲
胡绍争
张健
ZHANG Yangquan;LI Longfei;ZHOU Feng;YUAN Xingzhou;HU Shaozheng;ZHANG Jian(School of Petrochemical Engineering,Liaoning Petrochemical University,Fushun 113001,Liaoning,China;Dalian Research Institute of Petroleum and Petrochemicals,SINOPEC,Dalian 116000,Liaoning,China)
出处
《精细化工》
EI
CAS
CSCD
北大核心
2022年第10期2112-2121,共10页
Fine Chemicals
关键词
氮化碳
锆掺杂
光催化
降解
水处理技术
carbon nitride
zirconium doping
photocatalysis
degradation
water treatment technology
