Preparation of Cu2O/CuO-g-C3N4 Adsorbent by One-step Thermal Polymerization and Adsorption Properties for Methyl Orange

doi:10.19894/j.issn.1000-0518.220235

Chinese Journal of Applied Chemistry ›› 2023, Vol. 40 ›› Issue (3): 420-429.DOI: 10.19894/j.issn.1000-0518.220235

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Preparation of Cu₂O/CuO-g-C₃N₄ Adsorbent by One-step Thermal Polymerization and Adsorption Properties for Methyl Orange

Bo XIONG, Tai-Hua LI, Wu-Ping ZHOU, Chang-Yu LIU(), Xiao-Long XU()

School of Biotechnology and Health Sciences，Wuyi University，Jiangmen 529020，China

Received:2022-07-08 Accepted:2023-02-19 Published:2023-03-01 Online:2023-03-27
Contact: Chang-Yu LIU,Xiao-Long XU
About author:xyxl@wyu.edu.cn
wyuchemcyliu@126.com；
Supported by:
the National Natural Science Foundation of China(21974097);the Education Department of Guangdong Province(2020KSYS004);Guangdong Province's Special Fund for Science and Technology Innovation Strategy （College Students' Science and Technology Innovation Cultivation）(pdjh2022b0531);the Science and Technology Bureau of Jiangmen(2019030102360012639);the Undergraduate Training Programs of Wuyi University(202111349019)

Abstract

Abstract:

In this paper， Cu₂O/CuO graphite carbon nitride adsorbent is prepared by one-step thermal polymerization with cuprous oxide and dicyandiamide as precursors. The introduction of copper oxide expands the π conjugation system of g-C₃N₄ effectively， which is conducive to the adsorption of dyes with benzene ring structure through π-π interaction； Cu₂O/CuO-g-C₃N₄ adsorbent has mesoporous structures with various pore sizes， which increases its specific surface area and provides sufficient active sites for dye adsorption. The adsorption influencing factors of methyl orange， such as the preparation conditions of adsorbent， dosage， dye concentration， adsorption time， stirring speed， pH， etc.， are studied. The maximal absorption ratio is 96.11% under the optimal conditions. The kinetic analysis shows that the adsorption process is a quasi first-order kinetic model. According to the adsorption isothermal experiment， the adsorption isotherm belongs to Langmuir adsorption isotherm. In the whole adsorption experiment， the maximum equilibrium adsorption amount is 241.25 mg/g.

Key words: Cu modified carbon absorbent, Methyl orange, Thermal polymerization, Graphite carbon nitride

CLC Number:

O647.3

Bo XIONG, Tai-Hua LI, Wu-Ping ZHOU, Chang-Yu LIU, Xiao-Long XU. Preparation of Cu₂O/CuO-g-C₃N₄ Adsorbent by One-step Thermal Polymerization and Adsorption Properties for Methyl Orange[J]. Chinese Journal of Applied Chemistry, 2023, 40(3): 420-429.

Figures/Tables 12

Fig.1 SEM images of （A） g-C3N4 and （B） Cu2O/CuO-g-C3N4

Fig.2 XRD patterns of g-C3N4， CuO， Cu2O and Cu2O/CuO-g-C3N4

Fig.3 XPS spectra of （A） Cu2O/CuO-g-C3N4，（B） C1s，（C） N1s，（D） O1s and （E） Cu2p

Fig.4 Nitrogen adsorption-desorption isotherm and the pore-size distribution curve （inset） of Cu2O/CuO-g-C3N4

Fig.5 Adsorption efficiency for different （A） adsorbents，（B） polymerization temperature，（C） Cu2O dosage（w% is mass fraction of Cu2O in precursor） and （D） polymerization duration at 500 ℃ （20 mg adsorbent added into 100 mL 30 mg/L MO solution， pH = 6.0， 1400 r/min）

Fig.6 UV-Vis spectra （A） and photos （inset） of 30 mg/L MO solution with different adsorption duration；（B） adsorption efficiency with different MO concentration （20 mg adsorbent added into 100 mL MO solution， pH=6.0， 1400 r/min）

Table 1 Equilibrium adsorption amount comparation between this work and references

Graphene-based nanomaterial	Q_e/（mg·g^－1）	Ref.
PmPD/rGO/Nickle ferrite	136	［23］
Al-doped CNTs	69.70	［24］
Cu-Mo MOFs	48.13	［25］
Clay	41.67	［26］
Nitrogen-doped graphene gels	232	［27］
rGO	224	［28］
Cu₂O/CuO-g-C₃N₄	241.25	This work

Fig.7 Adsorption efficiency with different （A） dosage of Cu2O/CuO-g-C3N4，（B） MO concentration，（C） stirring rate and （D） pH （All experiments are executed at 20 mg adsorbent add into 100 mL 30 mg/L MO solution， pH=6.0 and stirring velocity of 1400 r/min unless mentioned otherwise）

Fig.8 Adsorption kinetics （A） and isotherm curve （B） of MO on the Cu2O/CuO-g-C3N4 absorbent （（A） 20 mg adsorbent added into 100 mL 30 mg/L MO solution， pH=6.0， 1400 r/min and （B） 20 mg adsorbent added into 100 mL MO solution， pH=6.0， 180 r/min shaking）

Table 2 Kinetic parameter fitting of MO adsorption

Preudo-first-order model
	ρ₀/（mg·L^-1）	K₁	q_e/（mg·g^-1）	r
MO	30	0.004 2	144.75	0.999

Table 3 Parameters for Langmuir model for MO adsorption

Langmuir constants
q_e/（mg·g^-1）	K_L/（L·mg^-1）	r
185	0.002 3	0.990

Fig.9 UV-Vis spectra and photos （inset） for MO desorption with different pH （20 mg adsorbent saturated with MO added into 100 mL PBS， magnetic stirring rate： 1400 r/min）

References 28

1	GUSAIN R， KUMAR N， RAY S S， et al. Recent advances in carbon nanomaterial-based adsorbents for water purification［J］. Coord Chem Rev， 2020， 405： 213111.
2	SUN W H， LIU D F， ZHANG M H， et al. Application of electrode materials and catalysts in electrocatalytic treatment of dye wastewater［J］. Frontiers Chem Sci Eng， 2021， 15（6）： 1427-1443.
3	FRAGA L E， FRANCO J H， ORLANDI M O， et al. Photoelectrocatalytic oxidation of hair dye basic red 51 at W/WO₃/TiO₂ bicomposite photoanode activated by ultraviolet and visible radiation［J］. J Environ Chem Eng， 2013， 1（3）： 194-199.
4	AREMU O H， AKINTAYO C O， NAIDOO E B， et al. Synthesis and applications of nano-sized zinc oxide in wastewater treatment： a review［J］. Int J Environ Sci Technol， 2021， 18（10）： 3237-3256.
5	HUSSAIN S， ANEGGI E， GOI D， et al. Catalytic activity of metals in heterogeneous Fenton-like oxidation of wastewater contaminants： a review［J］. Environ Chem Lett， 2021， 19（3）： 2405-2424.
6	MENG W Q， WANG G H， ZHANG M， et al. Generation of acid-base by bipolar membrane electrodialysis process during desalination of pesticide containing wastewater［J］. Desalin Water Treat， 2021， 217： 91-100.
7	BERA S P， GODHANIYA M， KOTHARI C， et al. Emerging and advanced membrane technology for wastewater treatment： a review［J］. J Basic Microb， 2022， 62（3/4）： 245-259.
8	BAGHERI H， HONARVAR B， ABBASI M， et al. Experimental evaluation of Farashband gas refinery wastewater treatment through activated carbon and natural zeolite adsorption process［J］. Desalin Water Treat， 2021， 225： 190-202.
9	JIANG S， XI J F， DAI H Q， et al. Multifunctional cellulose paper-based materials and their application in complex wastewater treatment［J］. Int J Biol Macromol， 2022， 207： 414-423.
10	FENG S， YANG W B， ZHANG L J， et al. Casein-hydroxyapatite composite microspheres for strontium-containing wastewater treatment［J］. ACS ES&T Water， 2021， 1（4）： 900-909.
11	TANG Y， LI Y， ZHAN L， et al. Removal of emerging contaminants （bisphenol A and antibiotics） from kitchen wastewater by alkali-modified biochar［J］. Sci Total Environ， 2022， 805： 150158.
12	HAN D X， ZHAO H J， GAO L L， et al. Preparation of carboxymethyl chitosan/phytic acid composite hydrogels for rapid dye adsorption in wastewater treatment［J］. Colloids Surf A： Physicochem Eng Aspects， 2021， 628： 127355.
13	HUANG X S， YIN R， QIAN L， et al. Processing conditions dependent tunable negative permittivity in reduced graphene oxide-alumina nanocomposites［J］. Ceram Int， 2019， 45（14）： 17784-17792.
14	CHEN Y， GAO X， LIU X W， et al. Water collection from air by ionic liquids for efficient visible-light-driven hydrogen evolution by metal-free conjugated polymer photocatalysts［J］.Renew Ener， 2020， 147： 594-601.
15	TRUONG H B， BAE S， CHO J， et al. Advances in application of g-C₃N₄-based materials for treatment of polluted water and wastewater via activation of oxidants and photoelectrocatalysis： a comprehensive review［J］. Chemosphere， 2022， 286： 131737.
16	LU X L， XU K， CHEN P Z， et al. Facile one step method realizing scalable production of g-C₃N₄ nanosheets and study of their photocatalytic H₂ evolution activity［J］. J Mater Chem A， 2014， 2（44）： 18924-18928.
17	ZHANG S T， LI G Q， DUAN L Y， et al. g-C₃N₄ synthesized from NH₄SCN in a H₂ atmosphere as a high performance photocatalyst for blue light-driven degradation of rhodamine B［J］. Rsc Adv， 2020， 10（33）： 19669-19685.
18	MA D N， LI X M， WANG X Q， et al. Preparation of g-C₃N₄ Nanosheets/CuO with enhanced catalytic activity on the thermal decomposition of ammonium perchlorate［J］. Eur J Inorg Chem， 2021， 2021（10）： 982-988.
19	WU L F， ZHANG Z Z， YANG M M， et al. Facile synthesis of CuO/g-C₃N₄ hybrids for enhancing the wear resistance of polyimide composite［J］. Eur Polym J， 2019， 116： 463-470.
20	WANG Q Y， XU H L， HUANG W T， et al. Metal organic frameworks-assisted fabrication of CuO/Cu₂O for enhanced selective catalytic reduction of NOx by NH₃ at low temperatures［J］. J Hazard Mater， 2019， 364： 499-508.
21	ZAYED A M， WAHED M， MOHAMED E A， et al. Insights on the role of organic matters of some Egyptian clays in methyl orange adsorption： isotherm and kinetic studies［J］. Appl Clay Sci， 2018， 166： 49-60.
22	LIU Y， WU Y H， PANG H W， et al. Study on the removal of water pollutants by graphite phase carbon nitride materials［J］. Prog Chem， 2019， 31（6）： 831-846.
23	WANG W， CAI K， WU X F， et al. A novel poly（m-phenylenediamine）/reduced graphene oxide/nickel ferritemagnetic adsorbent with excellent removal ability of dyes and Cr（VI）［J］. J Alloy Compd， 2017， 722： 532-543.
24	KANG D J， YU X L， GE M F， et al. Novel Al-doped carbon nanotubes with adsorption and coagulation promotion for organic pollutant removal［J］. J Environ Sci， 2017， 54： 1-12.
25	IMAN K， SHAHID M， KHAN M S， et al. Topology magnetism and dye adsorption properties of metal organic frameworks （MOFs） synthesized from bench chemicals［J］. CrystEngComm， 2019， 21（35）： 5299-5309.
26	ZAYED A M， WAHED M， MOHAMED E A， et al. Insights on the role of organic matters of some Egyptian clays in methyl orange adsorption： isotherm and kinetic studies［J］. Appl Clay Sci， 2018， 166： 49-60.
27	GENG J Y， SI L L， GUO H T， et al. 3D nitrogen-doped graphene gels as robust and sustainable adsorbents for dyes［J］. New J Chem， 2017， 41（24）： 15447-15457.
28	MINITHA C R， LALITHA M， JEYACHANDRAN Y L， et al. Adsorption behaviour of reduced graphene oxide towards cationic and anionic dyes： co-action of electrostatic and π-π interactions［J］. Mater Chem Phys， 2017， 194： 243-252.

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Preparation of Cu₂O/CuO-g-C₃N₄ Adsorbent by One-step Thermal Polymerization and Adsorption Properties for Methyl Orange

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