化工新型材料

化工新型材料 ›› 2020, Vol. 48 ›› Issue (6) : 216-221.

科学研究

Cu₂O-CuO/g-C₃N₄复合光催化剂的制备及其催化性能研究

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Preparation and performance of Cu₂O-CuO/g-C₃N₄ photocatalyst

Xia Fen, Tao Yu, Huang Zihao, Tao Xianyun, Teng Xuegang, Yang Renchun

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Received		Published
2019-01-02		2020-06-20
Issue Date	Revised Date
2020-07-02	2019-01-02

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摘要

以碱式碳酸铜为铜源,葡萄糖为还原剂,通过液-固两相水热还原法,在氮化碳(g-C₃N₄)表面原位沉积制备了系列氧化亚铜-氧化铜/氮化碳(Cu₂O-CuO/g-C₃N₄)光催化剂。采用扫描电子显微镜、透射电子显微镜、能量色散谱仪、X射线衍射仪、紫外-可见分光光度计和X射线光电子能谱仪表征分析了催化剂的微观形貌、晶型结构、表面元素价态和氧空位情况。研究结果表明:Cu₂O-CuO的引入可使g-C₃N₄催化剂的光吸收发生显著红移,具有更宽的可见光响应;随着Cu⁺含量的增加,催化剂样品氧空位(O_ads/O_latt)的变化规律遵循Cu₂O-CuO/g-C₃N₄-100>Cu₂O-CuO/g-C₃N₄-50>Cu₂O-CuO/g-C₃N₄-10。光催化性能研究表明:对于罗丹明B与亚甲基蓝的光催化降解,Cu₂O-CuO的引入可提高g-C₃N₄的光降解性能;同时O_ads/O_latt的提高有助于提高其光催化性能。

Abstract

The Cu₂O-CuO/g-C₃N₄ photocatalysts were prepared by solid-liquid two-phase hydrothermal reduction using alkaline copper carbonate as copper source and glucose as reducing agent.The microstructure,crystal structure,valence state and oxygen vacancy of various catalysts were characterized by SEM,TEM,EDS,XRD,UV-Vis and XPS.The results showed that:the introduction of Cu₂O-CuO promoted a significant red shift and a wider visible light response compared with that of g-C₃N₄.With the increase of Cu⁺,the changes of oxygen vacancy (O_ads/O_latt) of the samples followed as:Cu₂O-CuO/g-C₃N₄-100>Cu₂O-CuO/g-C₃N₄-50>Cu₂O-CuO/g-C₃N₄-10.The results indicated that the photocatalytic activity of the catalysts could be improved via introducing Cu₂O-CuO for the degradation of RhB and MB.Moreover,the increase of O_ads/O_latt ratio was helpful to improving its photocatalytic performance.

关键词

氮化碳 / 氧化亚铜-氧化铜 / 水热还原反应 / 氧空位 / 光催化降解

Key words

g-C₃N₄ / Cu₂O-CuO / hydrothermal reduction / oxygen vacancy / photocatalytic degradation

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Cu₂O-CuO/g-C₃N₄复合光催化剂的制备及其催化性能研究[J]. 化工新型材料, 2020, 48(6): 216-221 DOI:

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参考文献

原文顺序 | 出版日期 | 本文引用

[1] Wang X,Blechert S,Antonietti M.Polymeric graphitic carbon nitride for heterogeneous photocatalysis[J].ACS Catal,2012,2(8):1596-1606.
[2] Cao S,Yu J.g-C₃N₄-based photocatalysts for hydrogen generation[J].J Phys Chem Lett,2014,5(12):2101-2107.
[3] Zhao Z,Sun Y,Dong F.Graphitic carbon nitride based nanocomposites:a review[J].Nanoscale,2015,7(1):15-37.
[4] Yu H,Shi R,Zhao Y,et al.Smart utilization of carbon dots in semiconductor photocatalysis[J].Adv Mater,2016,28(43):9454-9477.
[5] Shalom M,Inal S,Fettkenhauer C,et al.Improving carbon nitride photocatalysis by supramolecular preorganization of monomers[J].J Am Chem Soc,2013,135(19):7118-7121.
[6] Zhao X,Ma Z,Wu D,et al.Computational study of catalytic effect of C₃N₄,on H₂,release from complex hydrides[J].Int J Hydrogen Energy,2015,40(29):8897-8902.
[7] Wang X,Maeda K,Thomas A,et al.A metal-free polymeric photocatalyst for hydrogen production from water under visible light[J].Nat Mater,2009,8(1):76.
[8] Zhang Y W,Liu J H,Wu G,et al.Porous graphitic carbon nitride synthesized via direct polymerization of urea for efficient sunlight-driven photocatalytic hydrogen production[J].Nanoscale,2012,4(17):5300-5303.
[9] Liu G,Niu P,Sun C,et al.Unique electronic structure induced high photoreactivity of sulfur-doped graphitic C₃N₄[J].J Am Chem Soc,2010,132(33):11642-11648.
[10] Li J,Shen B,Hong Z,et al.A facile approach to synthesize novel oxygen-doped g-C₃N₄ with superior visible-light photoreactivity[J].Chem Commun,2012,48(98):12017-12019.
[11] Liu G,Niu P,Sun C,et al.Unique electronic structure induced high photoreactivity of sulfur-doped graphitic-C₃N₄[J].J Am Chem Soc,2010,132(33):11642-11648.
[12] Zhang Y,Mori T,Ye J,et al.Phosphorus-doped carbon nitride solid:enhanced electrical conductivity and photocurrent generation[J].J Am Chem Soc,2010,132(18):6294-6295.
[13] Wang Y,Di Y,Antonietti M,et al.Excellent visible-light photocatalysis of fluorinated polymeric carbon nitride solids[J].Chem Mater,2010,22(18):5119-5121.
[14] Deng Y,Liu K,Cao H,et al.Synthesis of graphene with both high nitrogen content and high surface area by annealing composite of graphene oxide and g-C₃N₄[J].J Iran Chem Soc,2015,12(5):807-814.
[15] Rajendra Pawar C,Suhee Kang,Sung Hoon Ahn,et al.Gold nanoparticle modified graphitic carbon nitride/multi-walled carbon nanotube (g-C₃N₄/CNTs/Au) hybrid photocatalysts for effective water splitting and degradation[J].RSC Adv,2015,5(31):24281-24292.
[16] Zhang M,Xu J,Zong R,et al.Enhancement of visible light photocatalytic activities via porous structure of g-C₃N₄[J].Appl Catal B:Environ,2014,147(8):229-235.
[17] Yang S,Gong Y,Zhang J,et al.Exfoliated graphitic carbon nitride nanosheets as efficient catalysts for hydrogen evolution under visible light[J].Adv Mater,2013,25(17):2452-2456.
[18] Xu Z,Zhang C,Zou Z,et al.Enhanced photocatalytic activity by the construction of a TiO₂/carbon nitride nanosheets heterostructure with high surface area via direct interfacial assembly[J].Nano Res,2017,10(7):2193-2209.
[19] Zhang H,Liu F,Wu H,et al.In situ synthesis of g-C₃N₄/TiO₂ heterostructures with enhanced photocatalytic hydrogen evolution under visible light[J].RSC Adv,2017,7(64):40327-40333.
[20] Yan H,Yang H.TiO₂-g-C₃N₄ composite materials for photocatalytic H₂ evolution under visible light irradiation[J].Journal of Alloys & Compounds,2011,509(4):26-29.
[21] Cao S W,Yuan Y P,Fang J,et al.In-situ growth of CdS quantum dots on g-C₃N₄ nanosheets for highly efficient photocatalytic hydrogen generation under visible light irradiation[J].Int J Hydrogen Energy,2013,38(3):1258-1266.
[22] Wang Y,Wang Z,Muhammad S,et al.Graphite-like C₃N₄ hybridized ZnWO₄ nanorods:synthesis and its enhanced photocatalysis in visible light[J].Cryst Eng Comm,2012,14(15):5065-5070.
[23] Pan C,Xu J,Wang Y,et al.Dramatic activity of C₃N₄/BiPO₄ photocatalyst with core/shell structure formed by self-assembly[J].Adv Funct Mater,2012,22(7):1518-1524.
[24] Huang Y,Yan C F,Guo C Q,et al.Synthesis of GO-modified Cu₂O nanosphere and the photocatalytic mechanism of water splitting for hydrogen production[J].Int J Hydrogen Energy,2017,42(7):4007-4016.
[25] Rather R A,Singh S,Pal B.A Cu⁺¹/Cu⁰-TiO₂ mesoporous nanocomposite exhibits improved H₂ production from H₂O under direct solar irradiation[J].J Catal,2017,346:1-9.
[26] Cao S,Low J,Yu J,et al.Polymeric photocatalysts based on graphitic carbon nitride[J].Adv Mater,2015,27(13):2150-2176.
[27] Yang R C,Lu X J,Huang X,et al.Bi-component Cu₂O-CuCl composites with tunable oxygen vacancies and enhanced photocatalytic properties[J].Appl Catal B:Environ,2015,170-171(1301):225-232.
[28] Yang R C,Lu X J,Zhang H,et al.Glycol-assisted construction of three-dimensionally ordered microporous ZnO-Cu₂O-TiO₂ with enhanced photocatalytic properties[J].Appl Surf Sci,2016,36:237-243.
[29] 滕雪刚,杨仁春,任超,等.C/TiO₂-SO^2-₄的制备及其光解水性能[J].化工学报,2017,68(11):4414-4422.
[30] Yang R C,Zhang Z H,Ren Y M,et al.Green synthesis of bi-component copper oxide composites and enhanced photocatalytic performance[J].Mater Sci Tech-Lond,2015,31(1):25-30.
[31] Yang R C,Lu X J,Zhang Z H,et al.Three-dimensionally ordered macroporous LaMnO₃ with tunable oxygen vacancies via nitric acid-aided modulating and their catalytic combustion properties[J].RSC Adv,2015,5(119):98404-98411.