摘要
卤氧化铋(BiOX)基光催化材料因具有优异的光催化性能近年来发展突飞猛进。为开发可见光响应的高效BiOX基光催化剂,以盐酸四环素为氯源和碳源,结合水热法和退火处理成功合成了碳掺杂的微纳米花球状固溶体(Bi_(4)O_(5)Br_(1.87)Cl_(0.13))。利用TEM,SEM,XPS,XRD等分析技术对其进行了微观形貌、化学结构、光电化学性质、光催化降解性能的表征。结果表明:Bi_(4)O_(5)Br_(1.87)Cl_(0.13)为纳米片组装的花球状形貌,其中Cl和C元素的引入诱导其价带和导带轨道发生高程度的杂化,产生一定的杂质能级。该杂质能级增强了催化剂对可见光的吸收,同时提供电荷传输的通道,促进电荷分离。另外,Bi_(4)O_(5)Br_(1.87)Cl_(0.13)相比于未改性的Bi_(4)O_(5)Br_(2)具有更窄的禁带宽度,在可见光下可获得更高的电子-空穴激发效率。通过300℃的退火处理,获得碳掺杂量为3.58%(质量分数)的Bi_(4)O_(5)Br_(1.87)Cl_(0.13)-300,其具有最优异的光催化性能。在35 W卤素灯光照下,1 h内Bi_(4)O_(5)Br_(1.87)Cl_(0.13)-300对甲基橙(10 mg/L)的降解率可达到88.29%,而Bi_(4)O_(5)Br_(2)在相同条件下对甲基橙的降解率仅有28.53%。分步降解研究表明,Bi_(4)O_(5)Br_(1.87)Cl_(0.13)-300优异的光催化性能主要是球形表面的纳米片状多级结构提供了大量的表面位点参与反应。研究成果为增强BiOX材料的光催化性能提供了新的参考。
Bismuth halide oxide based photocatalytic materials have made rapid progress in recent years due to their excellent photocatalytic performace.In this project,in order to develop effective visible light responsive BiOX based photocatalyst,carbon-doped micro and nano-flower spherical solid solution(Bi_(4)O_(5)Br_(1.87)Cl_(0.13))were successfully synthesized by combining the hydrothermal method and annealing treatment,with tetracycline hydrochloride as the chlorine and carbon sources.TEM,SEM,XPS,XRD and other analytical techniques were used to characterize its micro morphology,chemical structure,photoelectrochemical properties,and photocatalytic degradation performance.The results showed that Bi_(4)O_(5)Br_(1.87)Cl_(0.13) was a spherical morphology of nanosheet assembly,in which the introduction of chlorine and carbon elements induced a high degree of hybridization in the valence and conduction band orbitals,resulting in a certain impurity energy level.This impurity energy level enhanced the absorption of visible light by the catalyst,while providing a channel for charge transport and promoting charge separation.Moreover,Bi_(4)O_(5)Br_(1.87)Cl_(0.13) had a narrower forbidden bandwidth compared to the unmodified Bi_(4)O_(5)Br_(2),which meant that a higher electron-hole excitation efficiency obtained in visible light.The Bi_(4)O_(5)Br_(1.87)Cl_(0.13)-300 with a carbon doping of 3.58%(mass fraction)was obtained by annealing at 300℃with the most excellent photocatalytic performance.The degradation of methyl orange(10 mg/L)by Bi_(4)O_(5)Br_(1.87)Cl_(0.13)-300 could reach 88.29%in one hour under the light of 35 W halogen lamp,while the degradation of methyl orange by Bi_(4)O_(5)Br_(2) under the same conditions was only 28.53%.The stepwise degradation study showed that the excellent photocatalytic degradation performance of Bi_(4)O_(5)Br_(1.87)Cl_(0.13)-300 mainly came from the nanosheet-like multistage structure on the spherical surface,which provided a large number of surface sites involved in the reaction.The present
作者
彭灵芝
刘嘉
杨阳
汤森培
PENG Lingzhi;LIU Jia;YANG Yang;TANG Senpei(School of Chemistry and Chemical Engineering,Jishou University,Jishou 416000,China)
出处
《环境工程》
CAS
CSCD
北大核心
2023年第5期125-133,171,共10页
Environmental Engineering
基金
国家自然科学基金(22005117)
湖南省自然科学基金(2022JJ40337)
关键词
微纳米花球状固溶体
可见光催化
卤氧化铋
碳掺杂
micro-and nano-flower spherical solid solution
visible light catalysis
bismuth halide oxide
carbon doping
