Boron nitride quantum dots decorated ultrathin porous g-C3N4: Intensified exciton dissociation and charge transfer for promoting visible-light-driven molecular oxygen activation

被引:620
作者
Yang, Yang [1 ,2 ]
Zhang, Chen [1 ,2 ]
Huang, Danlian [1 ,2 ]
Zeng, Guangming [1 ,2 ]
Huang, Jinhui [1 ,2 ]
Lai, Cui [1 ,2 ]
Zhou, Chengyun [1 ,2 ]
Wang, Wenjun [1 ,2 ]
Guo, Hai [1 ,2 ]
Xue, Wenjing [1 ,2 ]
Deng, Rui [1 ,2 ]
Cheng, Min [1 ,2 ]
Xiong, Weiping [1 ,2 ]
机构
[1] Hunan Univ, Coll Environm Sci & Engn, Changsha 410082, Hunan, Peoples R China
[2] Hunan Univ, Minist Educ, Key Lab Environm Biol & Pollut Control, Changsha 410082, Hunan, Peoples R China
基金
中国国家自然科学基金;
关键词
Boron nitride quantum dots; Ultrathin porous g-C3N4; Exciton dissociation; Photocatalytic molecular oxygen activation; H2O2; production; GRAPHITIC CARBON NITRIDE; FREE EFFICIENT PHOTOCATALYST; ONE-STEP SYNTHESIS; AQUEOUS-SOLUTION; H-BN; TETRACYCLINE DEGRADATION; HYDROGEN-PEROXIDE; HEAVY-METALS; WASTE-WATER; BAND-GAP;
D O I
10.1016/j.apcatb.2018.12.049
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Graphitic carbon nitride (g-C3N4) has enormous potential for photocatalysis, but only possesses moderate activity because of excitonic effects and sluggish charge transfer. Herein, metal-free heterostructure photocatalyst constructed by boron nitride quantum dots (BNQDs) and ultrathin porous g-C3N4 (UPCN) was successfully developed for overcoming these defects. Results showed that the BNQDs loaded UPCN can simultaneously promote the dissociation of excitons and accelerate the transfer of charges owing to the negatively charged functional groups on the surface of BNQDs as well as the ultrathin and porous nanostructure of g-C3N4. Benefiting from the intensified exciton dissociation and charge transfer, the BNQDs/UPCN (BU) photocatalyst presented superior visible-light-driven molecular oxygen activation ability, such as superoxide radical (center dot O-2(-)) generation and hydrogen peroxide (H202) production. The average '02- generation rate of the optimal sample (BU-3) was estimated to be 0.25 umol L-1 min-1, which was about 2.3 and 1.6 times than that of bulk g-C3N4 and UPCN. Moreover, the H2O2 production by BU-3 was also higher than that of bulk g-C3N4 (22.77 umol L-1) and UPCN (36.13 ttmol L-1), and reached 72.30 ttmol L-1 over 60 min. This work reveals how rational combination of g-C3N4 with BNQDs can endow it with improved photocatalytic activity for molecular oxygen activation, and provides a novel metal-free and highly efficient photocatalyst for environmental remediation and energy conversion.
引用
收藏
页码:87 / 99
页数:13
相关论文
共 71 条
[1]   One-step synthesis of Co-doped UiO-66 nanoparticle with enhanced removal efficiency of tetracycline: Simultaneous adsorption and photocatalysis [J].
Cao, Jiao ;
Yang, Zhao-hui ;
Xiong, Wei-ping ;
Zhou, Yao-yu ;
Peng, Yan-rong ;
Li, Xin ;
Zhou, Cheng-yun ;
Xu, Rui ;
Zhang, Yan-ru .
CHEMICAL ENGINEERING JOURNAL, 2018, 353 :126-137
[2]   Molecular Design of Polymer Heterojunctions for Efficient Solar-Hydrogen Conversion [J].
Chen, Jie ;
Dong, Chung-Li ;
Zhao, Daming ;
Huang, Yu-Cheng ;
Wang, Xixi ;
Samad, Leith ;
Dang, Lianna ;
Shearer, Melinda ;
Shen, Shaohua ;
Guo, Liejin .
ADVANCED MATERIALS, 2017, 29 (21)
[3]   Bioremediation of soils contaminated with polycyclic aromatic hydrocarbons, petroleum, pesticides, chlorophenols and heavy metals by composting: Applications, microbes and future research needs [J].
Chen, Ming ;
Xu, Piao ;
Zeng, Guangming ;
Yang, Chunping ;
Huang, Danlian ;
Zhang, Jiachao .
BIOTECHNOLOGY ADVANCES, 2015, 33 (06) :745-755
[4]   Synthesis of Au-CuS-TiO2 nanobelts photocatalyst for efficient photocatalytic degradation of antibiotic oxytetracycline [J].
Chen, Qinghua ;
Wu, Shuna ;
Xin, Yanjun .
CHEMICAL ENGINEERING JOURNAL, 2016, 302 :377-387
[5]   Metal-organic frameworks for highly efficient heterogeneous Fenton-like catalysis [J].
Cheng, Min ;
Lai, Cui ;
Liu, Yang ;
Zeng, Guangming ;
Huang, Danlian ;
Zhang, Chen ;
Qin, Lei ;
Hu, Liang ;
Zhou, Chengyun ;
Xiong, Weiping .
COORDINATION CHEMISTRY REVIEWS, 2018, 368 :80-92
[6]   Efficient degradation of sulfamethazine in simulated and real wastewater at slightly basic pH values using Co-SAM-SCS /H2O2 Fenton-like system [J].
Cheng, Min ;
Zeng, Guangming ;
Huang, Danlian ;
Lai, Cui ;
Liu, Yang ;
Zhang, Chen ;
Wan, Jia ;
Hu, Liang ;
Zhou, Chengyun ;
Xiong, Weiping .
WATER RESEARCH, 2018, 138 :7-18
[7]   Hydroxyl radicals based advanced oxidation processes (AOPs) for remediation of soils contaminated with organic compounds: A review [J].
Cheng, Min ;
Zeng, Guangming ;
Huang, Danlian ;
Lai, Cui ;
Xu, Piao ;
Zhang, Chen ;
Liu, Yang .
CHEMICAL ENGINEERING JOURNAL, 2016, 284 :582-598
[8]   Simultaneous removal of Cd(II) and ionic dyes from aqueous solution using magnetic graphene oxide nanocomposite as an adsorbent [J].
Deng, Jiu-Hua ;
Zhang, Xiu-Rong ;
Zeng, Guang-Ming ;
Gong, Ji-Lai ;
Niu, Qiu-Ya ;
Liang, Jie .
CHEMICAL ENGINEERING JOURNAL, 2013, 226 :189-200
[9]   Insight into highly efficient simultaneous photocatalytic removal of Cr(VI) and 2,4-diclorophenol under visible light irradiation by phosphorus doped porous ultrathin g-C3N4 nanosheets from aqueous media: Performance and reaction mechanism [J].
Deng, Yaocheng ;
Tang, Lin ;
Zeng, Guangming ;
Zhu, Zhejing ;
Yan, Ming ;
Zhou, Yaoyu ;
Wang, Jiajia ;
Liu, Yani ;
Wang, Jingjing .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2017, 203 :343-354
[10]   Core-shell Ag2CrO4/N-GQDs@g-C3N4 composites with anti-photocorrosion performance for enhanced full-spectrum-light photocatalytic activities [J].
Feng, Chengyang ;
Deng, Yaocheng ;
Tang, Lin ;
Zeng, Guangming ;
Wang, Jiajia ;
Yu, Jiangfang ;
Liu, Yani ;
Peng, Bo ;
Feng, Haopeng ;
Wang, Jingjing .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2018, 239 :525-536