

浏览全部资源
扫码关注微信
1.辽宁石油化工大学化学化工与环境学部,辽宁 抚顺 113001
2.营口理工学院化学与环境工程系,辽宁 营口 115014
3.辽宁科技大学化学工程学院,辽宁 鞍山 114051
Received:23 March 2020,
Revised:2020-07-18,
Online First:17 December 2020,
Published:05 December 2020
移动端阅览
刘帅, 李学雷, 李启朦, 王彦娟, 张健, 封瑞江, 胡绍争. 木棉纤维改性氮化碳光催化降解有机污染物[J]. 化工学报, 2020, 71(12): 5530-5540
LIU Shuai, LI Xuelei, LI Qimeng, WANG Yanjuan, ZHANG Jian, FENG Ruijiang, HU Shaozheng. Kapok fiber modified carbon nitride photocatalytic degradation of organic pollutants[J]. CIESC Journal, 2020, 71(12): 5530-5540
刘帅, 李学雷, 李启朦, 王彦娟, 张健, 封瑞江, 胡绍争. 木棉纤维改性氮化碳光催化降解有机污染物[J]. 化工学报, 2020, 71(12): 5530-5540 DOI: 10.11949/0438-1157.20200304.
LIU Shuai, LI Xuelei, LI Qimeng, WANG Yanjuan, ZHANG Jian, FENG Ruijiang, HU Shaozheng. Kapok fiber modified carbon nitride photocatalytic degradation of organic pollutants[J]. CIESC Journal, 2020, 71(12): 5530-5540 DOI: 10.11949/0438-1157.20200304.
采用一步热解法制备了木棉纤维(KF)改性的石墨相氮化碳(g-C
3
N
4
)催化剂,并考察了催化剂光催化降解有机污染物的性能。采用XRD、UV-Vis DRS、FT-IR、TEM、XPS、N
2
吸附-脱附、PL表征对催化剂进行了结构、形貌、光学性能测试。结果表明,KF改性可以提高催化剂的比表面积,更大的比表面积可以提供更多的活性位点来参与光催化降解过程。UV-Vis DRS结果表明KF改性可以缩小催化剂的禁带宽度,提高催化剂对光能的吸收。在可见光下,KF改性的g-C
3
N
4
基催化剂对苯酚降解速率常数为0.259 h
-1
,是纯g-C
3
N
4
的4.2倍,且具有优异的催化稳定性和结构稳定性。
A kapok fiber (KF) modified graphite phase carbon nitride (g-C
3
N
4
) catalyst was prepared by a one-step pyrolysis method
and the photocatalytic degradation of organic pollutants was investigated. The structure and optical properties of KF-CN were characterized by XRD
UV-Vis DRS
TEM
PL
XPS
FT-IR and N
2
adsorption-desorption. The nitrogen adsorption-desorption isotherm results show that the presence of the mesoporous structure can improve the specific surface area of KF-CN. Elemental analysis characterization indicates the biochar modification is conductive to increase the C/N ratio of KF-CN. The XPS characterization also indicates that the introduction of carbon element can change the chemical environment of N element in the lattice of g-C
3
N
4
and thu
s increases the electron density of N element. The photocatalytic degradation of phenol experiment was carried out to investigate the performance of as-prepared kapok fiber modified graphite carbon nitride photocatalysts by using high-pressure sodium lamp as visible light source. The results show the KF(5%)-CN(600) displayed the highest phenol degradation rate constant of 0.259 h
-1
which is 4.2 times of that of neat g-C
3
N
4
.The activity of KF(5%)-CN(600) does not decrease significantly after 5 cycles
hinting its excellent catalytic stability and structural stability. The possible reaction mechanism was proposed.
Pawar R, Khare V, Lee S C. Hybrid photocatalysts using graphitic carbon nitride/cadmium sulfide/reduced graphene oxide (g-C3N4/CdS/RGO) for superior photodegradation of organic pollutants under UV and visible light[J ] . Dalton Trans., 2014, 43 : 12514-12527.
Dong G H, Jacobs D, Zang L, et al. Carbon vacancy regulated photoreduction of NO to N2 over ultrathin g-C3N4 nanosheets[J ] . Appl. Catal. B: Environ., 2017, 218 : 515-524.
Hu S Z, Jin R R, Lu G, et al. The properties and photocatalytic performance comparison of Fe3+-doped g-C3N4 and Fe2O3/g-C3N4 composite catalysts[J ] . RSC Adv., 2014, 4 : 24863-24869.
Hu S Z, Qu X Y, Li P, et al. Photocatalyti c oxygen reduction to hydrogen peroxide over copper doped graphitic carbon nitride hollow microsphere: the effect of Cu(I)-N active sites[J ] . Chem. Eng. J., 2018, 334 : 410-418.
Lan Z A, Zhang G G, Wang X C. A facile synthesis of Br-modified g-C3N4 semiconductors for photoredox water splitting[J ] . Appl. Catal. B: Environ., 2016, 192 : 116-125.
Liu D X, Zhang J, Li C, et al. In - situ fabrication of atomic charge transferring path for constructing heterojunction photocatalysts with hierarchical structure[J ] . Appl. Catal. B: Environ., 2019, 248 : 459-465.
Dong G H, Ho W K, Wang C Y. Selective photocatalytic N2 fixation dependent on g-C3N4 induced by nitrogen vacancies[J ] . J. Mater. Chem. A, 2015, 3 : 23435-23441.
Li H, Shang J, Ai Z H. Efficient visible light nitrogen fixation with BiOBr nanosheets of oxygen vacancies on the exposed {001} facets[J ] . J. Am. Chem. Soc., 2015, 137 : 6393-6399.
Bao N, Hu X, Zhang Q, et al. Synthesis of porous carbon-doped g-C3N4 nanosheets with enhanced visible-light photocatalytic activity[J ] . Appl. Surf. Sci., 2017, 403 : 682-690.
Tong Z W, Yang D, Zhao X Y, et al. Bio-inspired synthes is of three-dimensional porous g-C3N4@carbon microflowers with enhanced oxygen evolution reactivity[J ] . Chem. Eng. J., 2018, 337 : 312-321.
Jin Z, Chen J, Huang S, et al. A facile approach to fabricating carbonaceous material/g-C3N4 composites with superior photocatalytic activity[J ] . Catal. Today, 2018, 315 : 149-154.
Liu J Y, Xu H, Xu Y G, et al. Graphene quantum dots modified mesoporous graphite carbon nitride with significant enhancement of photocatalytic activity[J ] . Appl. Catal. B: Environ., 2017, 207 : 429-437.
Wang F L, Chen P, Feng Y P, et al. Facile synthesis of N-doped carbon dots/g-C3N4 photocatalyst with enhanced visible-light photocatalytic activity for the degradation of indomethacin[J ] . Appl. Catal. B: Environ., 2017, 207 : 103-113.
Fang S, Xia Y, Lv K L, et al. Effect of carbon-dots modification on the structure and photocatalytic activity of g-C3N4[J ] . Appl. Catal. B: Environ., 2016, 185 : 225-232.
Cao Y F, Xie L J, Sun G H, et al. Hollow carbon microtubes from kapok fiber: structural evolution and energy storage performance[J ] . Sustain. Energy Fuels, 2018, 2 : 455-465.
Wang Y, Wang X C, Antonietti M. Polymeric graphi tic carbon nitride as a heterogeneous organocatalyst: from photochemistry to multipurpose catalysis to sustainable chemistry[J ] . Angew. Chem. Int. Ed., 2012, 51 : 68-89.
鲍勇霖. 高光催化活性类石墨相氮化碳的制备与优化[D]. 沈阳: 辽宁大学, 2019.
Bao Y L. Preparation and optimization of graphite-like carbon nitride with high photocatalytic activity[D]. Shenyang: Liaoning University, 2019.
Wang X C, Chen X F, Thomas A, et al. Metal-containing carbon nitride compounds: a new functional organic-metal hybrid material[J ] . Adv. Mater., 2009, 21 : 1609-1612.
高龙. 活性炭负载氮化碳活化过一硫酸氢盐降解酸性橙7的研究[D]. 武汉: 武汉纺织大学, 2017.
Gao L. Degradation of acid orange 7 by activated mono-bisulfate with carbon nitride on activated carbon[D]. Wuhan: Wuhan Textile University, 2017.
Kudo A, Miseki Y. Heterogeneous photocatalyst materials for water splitting[J ] . Chem. Soc. Rev., 2009, 38 (1): 253-278.
Lei W W, Portenhault D, Dimova R, et al. Boron carbon nitride nanostructures from salt melts: tunable water-soluble phosphors[J ] . J. Am. Chem. Soc., 2011, 133 (18): 5300-5303.
Zhao Z W, Sun Y J, Dong F, et al. Template synthesis of carbon self-doped g-C3N4 with enhanced visible to near-infrared absorption and photocatalytic performance[J ] . RSC. Adv., 2015, 5 : 39549-39556.
Hu S Z, Chen X, Li Q, et al. Fe3+ doping promoted N2 photofixation ability of honeycombed graphitic carbon nitride: the experimental and density functional theory simulation analysis[J ] . Appl. Catal. B: Environ., 2017, 201 : 58-69.
Hu P, Chen C J, Zeng R, et al. Facile synthesis of bimodal porous graphitic carbon nitride nanosheets as efficient photocatalysts for hydrogen evolution[J ] . Nano Energy, 2018, 50 : 376-382.
Li C M, Yu S Y, Dong H J, et al. Mesoporous ferriferrous oxide nanoreactors modified on graphitic carbon nitride towards improvement of physical, photoelectrochemical properties and photocatalytic performance[J ] . J. Colloid. Interf. Sci., 2018, 531 : 331-342.
Yan H J, Chen Y, Xu S M. Synthesis of graphitic carbon nitride by directly heating sulfuric acid treated melamine for enhanced photocatalytic H2 production from water under visible light[J ] . Int. J. Hydrogen Energ., 2012, 37 : 125.
Liu J Y, Fang W J, Wei Z D, et al. Efficient photocatalytic hydrogen evolution on N -deficient g-C3N4 achieved by a molten salt post-treatment approach[J ] . Appl. Catal. B: Environ., 2018, 238 (15): 465-470.
Li X F, Zhang J, Shen L H, et al. Preparation and characterization of graphitic carbon nitride through pyrolysis of melamine[J ] . Appl. Phys. A: Mater., 2009, 94 (2): 387-392.
Wang S M, Li D L, Sun C, et al. Synthesis and characterization of g-C3N4/Ag3VO4 composites with significantly enhanced visible-light photocatalytic activity for triphenylmethane dye degradation[J ] . Appl. Catal. B: Environ., 2014, 144 : 885-892.
Tong Z W, Yang D, Xiao T X, et al. Biomimetic fabrication of g-C3N4/TiO2 nanosheets with enhanced photocatalytic activity toward organic pollutant degradation[J ] . Chem. Eng. J., 2015, 260 : 117-125.
Ma Y J, Li X L, Yang Z, et al. Morphology control and photocatalysis enhancement by in situ hybridization of cuprous oxide with nitrogen-doped carbon quantum dots[J ] . Langmuir., 2016, 32 (37): 9418-9427.
Li X Y, Wang D S, Cheng G X, et al. Preparation of polyaniline-modified TiO2 nanoparticles and their photocatalytic activity under visible light illumination[J ] . Appl. Catal. B: Environ., 2008, 81 : 267-273.
Ikeda S, Sugiyama N, Murakami S, et al. Quantitative analysis of defective sites in titanium (Ⅳ) oxide photocatalyst powders[J ] . Phys. Chem. Chem. Phys., 2003, 5 : 778-783.
Zhou L, Song W, Chen Z Q, et al. Degradation of organic pollutants in wastewater by bicarbonate-activated hydrogen peroxide with a supported cobalt catalyst[J ] . Environ. Sci. Technol., 2013, 47 : 3833-3839.
Cao S W, Low J X, Yu J G, et al. Polymeric photocatalysts based on graphitic carbon nitride[J ] . Adv. Mater., 2015, 27 : 2150-2176.
Chang F, Zhang J, Xie Y C, et al. Fabrication, characterization, and photocatalytic performance of exfoliated g-C3N4–TiO2 hybrids[J ] . Appl. Surf. Sci., 2014, 311 : 574-581.
0
Views
1
下载量
1
CSCD
Publicity Resources
Related Articles
Related Author
Related Institution
京公网安备11010102001995号