Please wait a minute...
Journal of Chinese Society for Corrosion and protection  2024, Vol. 44 Issue (5): 1164-1176    DOI: 10.11902/1005.4537.2023.371
Current Issue | Archive | Adv Search |
Preparation of Co3O4-Zn Composite Coating and Its Simulated Antifouling Activity of Enzymes Catalyst
JIANG Ze1,2,3, ZHAI Xiaofan2,3(), ZHANG Yu2,3, SUN Jiawen2,3, JIANG Quantong2,3, WANG Youqiang1(), DUAN Jizhou2,3(), HOU Baorong2,3
1 School of Mechanical and Automotive Engineering, Qingdao University of Technology, Qingdao 266520, China
2 CAS Key Laboratory of Marine Environmental Corrosion and Bio-fouling, Institute of Oceanology, Chinese Academy of Sciences, Qingdao 266071, China
3 Open Studio for Marine Corrosion and Protection, Pilot National Laboratory for Marine Science and Technology (Qingdao), Qingdao 266235, China
Cite this article: 

JIANG Ze, ZHAI Xiaofan, ZHANG Yu, SUN Jiawen, JIANG Quantong, WANG Youqiang, DUAN Jizhou, HOU Baorong. Preparation of Co3O4-Zn Composite Coating and Its Simulated Antifouling Activity of Enzymes Catalyst. Journal of Chinese Society for Corrosion and protection, 2024, 44(5): 1164-1176.

Download:  HTML  PDF(12151KB) 
Export:  BibTeX | EndNote (RIS)      
Abstract  

Nanoparticles Co3O4 with peroxidase catalytic activity were co-deposited with Zn by electrodeposition to obtain a novel Co3O4-Zn composite coating on Q235 carbon steel. Ultrasound and sodium oleate (NaoI) were introduced during the co-deposition of Co3O4 and Zn, which strongly promoted dispersion and adsorption of Co3O4 on the co-deposited surface coating. The characterization by SEM and XRD revealed that Co3O4 was obviously dispersed into the Zn matrix. The addition of NaoI effectively increased the deposited amount of Co3O4 in the Co3O4-Zn coatings. Besides, the antimicrobial performance of the Co3O4-Zn coatings was evaluated with three typical fouling bacteria, namely, Escherichia coli (E. coli), Staphylococcus aureus (S. aureus), and Pseudomonas aeruginosa (P. aeruginosa). Results showed that the coverage of these three bacteria on Co3O4-Zn coatings decreased over 98%, illustrating that the Co3O4-Zn coatings showed high and broad-spectrum antimicrobial performance. It was also found that the Co3O4-Zn coating in the presence of hydrogen peroxide (H2O2) produced superoxide radicals (·O2-) and hydroxyl radicals (·OH), which played dominant roles in the antimicrobial process. Finally, the antimicrobial stability and corrosion resistance of the composite coatings were also verified, and it was found that the composite coatings exhibited good antimicrobial stability and corrosion resistance characteristics. The results of this study provide a new possibility for the development of bactericidal coatings of simulated enzyme catalyst and a new solution for green antifouling.

Key words:  Co3O4-Zn coating      ultrasound assistance      simulated enzyme-catalyzed antimicrobial      electrodeposition      sodium oleate     
Received:  21 November 2023      32134.14.1005.4537.2023.371
ZTFLH:  TG174  
Fund: National Natural Science Foundation of China(42376204);Shandong Provincial Natural Science Foundation(ZR2022MD023);Wenhai Program of the S&T Fund of Shandong Province for Pilot National Laboratory for Marine Science and Technology(2021WHZZB2303);the Young Elite Scientists Sponsorship Program by CAST(YESS20210201)
Corresponding Authors:  ZHAI Xiaofan, E-mail: zhaixf@qdio.ac.cnDUAN Jizhou, E-mail: duanjz@qdio.ac.cn
About author:  First author contact:WANG Youqiang, E-mail: wyq1970301@126.com

URL: 

https://www.jcscp.org/EN/10.11902/1005.4537.2023.371     OR     https://www.jcscp.org/EN/Y2024/V44/I5/1164

Zn

composite

coating

Co3O4

concentration in electrolyte

g·L-1

NaOI

concentration in electrolyte

mol·L-1

Time

min

Ultrasonic

intensity

W

Stirring

rate

r·min-1

pH

Current density

mA·cm-2

ZB--30306003-420
ZY-0.00530306003-420
ZC5-30306003-420
ZCY50.00530306003-420
Table 1  Electrodeposition parameters of Co3O4-Zn composite coatings
Fig.1  SEM images of ZB (a), ZY (b), ZC (c) and ZCY (d) composite coatings
Fig.2  SEM images of Co3O4 powders (a) and ZCY coating (b), and corresponding EDS element mappings of ZCY coating (c-f)
Fig.3  Cross-sectional morphology of ZCY coating (a) and elemental mappings in the region 1 (b), and SEM image of the region 2 in Fig.3b (c) and EDS line scannings along the line in Fig.3c (d)
Composite coatingCo / atomic fraction, %Zn / atomic fraction, %Co / Zn atomic ratio
ZB098.909/
ZY099.325/
ZC1.16197.4050.012
ZCY2.99793.0770.032
Table 2  EDS determined contents of Co and Zn in the composite coatings
Fig.4  XRD patterns of the coatings, showing the exitance of Co3O4 (a) and Zn (b)
Fig.5  Electrochemical analysis results of ZB, ZY, ZC and ZCY coatings during electrodeposition (a-e), and equivalent circuit for fitting EIS data (f)
Fig.6  Fluorescence microscope images of ZB, ZY, ZC and ZCY coatings after immersion for 2 h in Escherichia coli solutions with and without the addition of H2O2 (a), and the corresponding histograms of bacterial coverage on the coatings (b)
Fig.7  Fluorescence microscopy images of ZB and ZCY coatings after immersion for 2 h in Escherichia coli, Staphylococcus aureus and Pseudomonas aeruginosa solutions with the addition of hydrogen peroxide (a), and corresponding histograms of bacterial coverage (b)
Fig.8  Fluorescence microscopy images (a) and bacterial coverages (b) of ZB and ZCY composite coatings in Escherichia coli solution during cyclic immersion for 8 cycles
Fig.9  Nyqusit plots (a), Rct values (b), Tafel curves (c) of ZB and ZCY coatings in seawater, and corresponding equivalent circuit diagram (d)
GroupEcorr / V vs SCEIcorr / A·cm-2
ZB + Nacl-1.223350313.46 × 10-5
ZCY + Nacl-1.137499291.51 × 10-5
ZB + NaCl + H2O2-1.303865317.34 × 10-5
ZCY + NaCl + H2O2-1.243350314.17 × 10-5
Table 3  Calculated self-etching potentials and self-etching current densities of ZB and ZCY coatings in seawater based on Tafel curves in Fig.9c
Fig.10  Fluorescence microscopy images of ZB and ZCY coatings after adding scavenger in the absence and addition of H2O2 (a), and corresponding histograms of bacterial coverage (b), and EPR spectra of O2-, h+, and OH for ZCY coating (c-e)
Fig.11  Schematic diagram of bactericidal mechanism of Co3O4-Zn composite coatings
Fig.12  Bactericidal conditions of cobalt tetroxide powders in various bacteria solutions without and with H2O2 after the addition of scavenger
1 Al-Saadi S, Singh Raman R K. Silane coatings for corrosion and microbiologically influenced corrosion resistance of mild steel: a review [J]. Materials (Basel), 2022, 15: 7809
2 Bharatiya U, Gal P, Agrawal A, et al. Effect of corrosion on crude oil and natural gas pipeline with emphasis on prevention by ecofriendly corrosion inhibitors: a comprehensive review [J]. J. Bio- Tribo-Corros., 2019, 5: 35
3 Heyer A, D'Souza F, Leon Morales C F, et al. Ship ballast tanks a review from microbial corrosion and electrochemical point of view [J]. Ocean Eng., 2013, 70: 188
4 Loto C A. Microbiological corrosion: mechanism, control and impact—a review [J]. Int. J. Adv. Manuf. Technol., 2017, 92: 4241
5 Abioye O P, Loto C A, Fayomi O S I. Evaluation of anti-biofouling progresses in marine application [J]. J. Bio- Tribo-Corros., 2019, 5: 22
6 Saleem Khan M, Liang T, Liu Y Z, et al. Microbiologically influenced corrosion mechanism of ferrous alloys in marine environment [J]. Metals, 2022, 12: 1458
7 Punith Kumar M K, Rekha M Y, Srivastava C. Electrogalvanization using new generation coatings with carbonaceous additives: progress and challenges [J]. Corros. Rev., 2021, 39: 15
8 Oluwole O O, Oloruntoba D T, Awheme O. Effect of zinc plating of low carbon steel on corrosion resistance in cocoa fluid environment [J]. Mater. Des., 2008, 29: 1266
9 Klekotka M, Zielińska K, Stankiewicz A, et al. Tribological and anticorrosion performance of electroplated zinc based nanocomposite coatings [J]. Coatings, 2020, 10: 594
10 Zhai X F, Sun C T, Li K, et al. Synthesis and characterization of chitosan-zinc composite electrodeposits with enhanced antibacterial properties [J]. RSC Adv., 2016, 6: 46081
11 Zhai X F, Sun C T, Li K, et al. Composite deposition mechanism of 4,5-dichloro-2-n-octyl-4-isothiazolin-3-one in zinc films for enhanced corrosion resistant properties [J]. J. Ind. Eng. Chem., 2016, 36: 147
12 Zhai X F, Myamina M, Duan J Z, et al. Microbial corrosion resistance of galvanized coatings with 4,5-dichloro-2-n-octyl-4-isothiazolin-3-one as a biocidal ingredient in electrolytes [J]. Corros. Sci., 2013, 72: 99
13 Kumar C M P, Lakshmikanthan A, Chandrashekarappa M P G, et al. Electrodeposition based preparation of Zn-Ni alloy and Zn-Ni-WC Nano-composite coatings for corrosion-resistant applications [J]. Coatings, 2021, 11: 712
14 Silva-Ichante M, Reyes-Vidal Y, Bácame-Valenzuela F J, et al. Electrodeposition of antibacterial Zn-Cu/silver nanoparticle (AgNP) composite coatings from an alkaline solution containing glycine and AgNPs [J]. J. Electroanal. Chem., 2018, 823: 328
15 Castro-Rodríguez B, Terán-López A, Reyes-Vidal Y, et al. Zinc/Silver Particle (Zn/AgP) composite coatings: evaluation of corrosion in physiological environments and antibacterial activity against P. aeruginosa [J]. Coatings, 2020, 10: 337
16 García-Lecina E, García-Urrutia I, Díez J A, et al. A comparative study of the effect of mechanical and ultrasound agitation on the properties of electrodeposited Ni/Al2O3 nanocomposite coatings [J]. Surf. Coat. Technol., 2012, 206: 2998
17 Beltowska-Lehman E, Bigos A, Indyka P, et al. Optimisation of the electrodeposition process of Ni-W/ZrO2 nanocomposites [J]. J. Electroanal. Chem., 2018, 813: 39
18 Nath P, Sahu D K, Mallik A. Physicochemical and corrosion properties of sono-electrodeposited Cu-Ni thin films [J]. Surf. Coat. Technol., 2016, 307: 772
19 Zargazi M, Entezari M H. Ultrasound assisted deposition of highly stable self-assembled Bi2MoO6 nanoplates with selective crystal facet engineering as photoanode [J]. Ultrason. Sonochem., 2020, 67: 105145
20 Safavi M S, Walsh F C. Electrodeposited Co-P alloy and composite coatings: A review of progress towards replacement of conventional hard chromium deposits [J]. Surf. Coat. Technol., 2021, 422: 127564
21 Zarebidaki A, Allahkaram S R. Effect of surfactant on the fabrication and characterization of Ni-P-CNT composite coatings [J]. J. Alloy. Compd., 2011, 509: 1836
22 Yuan J C, Shiller A M. Hydrogen peroxide in deep waters of the North Pacific Ocean [J]. Geophys. Res. Lett., 2004, 31: L01310
23 Diaz J M, Plummer S, Tomas C, et al. Production of extracellular superoxide and hydrogen peroxide by five marine species of harmful bloom-forming algae [J]. J. Plankton Res., 2018, 40: 667
doi: 10.1093/plankt/fby043 pmid: 30487659
24 Wu L H, Luo Y, Wang C F, et al. Self-driven electron transfer biomimetic enzymatic catalysis of bismuth-doped PCN-222 MOF for rapid therapy of bacteria-infected wounds [J]. ACS Nano, 2023, 17: 1448
25 Mu J S, Wang Y, Zhao M, et al. Intrinsic peroxidase-like activity and catalase-like activity of Co3O4 nanoparticles [J]. Chem. Commun., 2012, 48: 2540
26 Dong J L, Song L N, Yin J J, et al. Co3O4 nanoparticles with multi-enzyme activities and their application in immunohistochemical assay [J]. ACS Appl. Mater. Interfaces, 2014, 6: 1959
27 Yang H G, Yang R T, Zhang P, et al. A bimetallic (Co/2Fe) metal-organic framework with oxidase and peroxidase mimicking activity for colorimetric detection of hydrogen peroxide [J]. Microchim. Acta, 2017, 184: 4629
28 Zhuang Y X, Zhang X D, Chen Q M, et al. Co3O4/CuO hollow nanocage hybrids with high oxidase-like activity for biosensing of dopamine [J]. Mater. Sci. Eng., 2019, 94C: 858
29 Alizadeh N, Salimi A, Hallaj R. Mimicking peroxidase-like activity of Co3O4-CeO2 nanosheets integrated paper-based analytical devices for detection of glucose with smartphone [J]. Sens. Actuators, 2019, 288B: 44
30 Chen J, Shan M D, Zhu H J, et al. Antimicrobial properties of heterojunction BiSnSbO6-ZnO composites in wastewater treatment [J]. Environ. Sci. Pollut. Res., 2023, 30: 55498
31 Polyakov N A, Botryakova I G, Glukhov V G, et al. Formation and anticorrosion properties of superhydrophobic zinc coatings on steel [J]. Chem. Eng. J., 2021, 421: 127775
32 Otani T, Fukunaka Y, Homma T. Effect of lead and tin additives on surface morphology evolution of electrodeposited zinc [J]. Electrochim. Acta, 2017, 242: 364
33 Nanda B, Mallik M. Production of copper powder by electrodeposition with different equilibrium crystal shape [J]. Trans. Indian Inst. Met., 2020, 73: 2113
34 Li H Y, Liu Y C, Liu J, et al. A Wulff-type boronate for boronate affinity capture of cis-diol compounds at medium acidic pH condition [J]. Chem. Commun., 2011, 47: 8169
35 Nayana K O, Venkatesha T V. Bright zinc electrodeposition and study of influence of synergistic interaction of additives on coating properties [J]. J. Ind. Eng. Chem., 2015, 26: 107
36 Mackinnon D J, Brannen J M, Fenn P L. Characterization of impurity effects in zinc electrowinning from industrial acid sulphate electrolyte [J]. J. Appl. Electrochem., 1987, 17: 1129
37 Sun K E K, Hoang T K A, Doan T N L, et al. Suppression of dendrite formation and corrosion on zinc anode of secondary aqueous batteries [J]. ACS Appl. Mater. Interfaces, 2017, 9: 9681
38 Gunawardena G, Hills G, Montenegro I. Electrochemical nucleation: Part II. The electrodeposition of silver on vitreous carbon [J]. J. Electroanal. Chem. Interfacial Electrochem., 1982, 138: 241
39 Zhai X F, Ju P, Guan F, et al. Electrodeposition of capsaicin-induced ZnO/Zn nanopillar films for marine antifouling and antimicrobial corrosion [J]. Surf. Coat. Technol., 2020, 397: 125959
40 Wang J, Wang Y, Zhang D. Exploring the bactericidal performance and application of novel mimic enzyme Co4S3 [J]. J. Colloid Interface Sci., 2020, 561: 327
41 Liu T J, Zhang X Y, Fu K, et al. Fabrication of Co3O4/NiCo2O4 nanocomposite for detection of H2O2 and dopamine [J]. Biosensors (Basel), 2021, 11: 452
42 Jiang D, Cui H Z, Chen H, et al. Wear and corrosion properties of B4C-added CoCrNiMo high-entropy alloy coatings with in-situ coherent ceramic [J]. Mater. Des., 2021, 210: 110068
43 Liu H, Ding Y N, Yang B C, et al. Colorimetric and ultrasensitive detection of H2O2 based on Au/Co3O4-CeO x nanocomposites with enhanced peroxidase-like performance [J]. Sens. Actuators, 2018, 271B: 336
44 Liu Q Y, Zhu R R, Du H, et al. Higher catalytic activity of porphyrin functionalized Co3O4 nanostructures for visual and colorimetric detection of H2O2 and glucose [J]. Mater. Sci. Eng., 2014, 43C: 321
[1] HUANG Zhifeng, YONG Qiwen, FANG Rui, XIE Zhihui. Superhydrophobic and Corrosion-resistant Nickel-based Composite Coating on Magnesium Alloy[J]. 中国腐蚀与防护学报, 2023, 43(4): 755-764.
[2] CHEN Huimin, WANG Shuaixing, ZHANG Qi, ZHAN Zhongwei, DU Nan. Electrodeposition Behavior of Silver in an Alkaline DMH Plating Bath with 5,5-Dimethylhydantoin as Complexing Agent[J]. 中国腐蚀与防护学报, 2023, 43(4): 896-902.
[3] LIU Yongqiang, LIU Guangming, FAN Wenxue, GAN Hongyu, TANG Rongmao, SHI Chao. Effect of Polyethylene Glycol-600 on Acidic Zn-Ni Alloy Electroplating and Its Corrosion Resistance[J]. 中国腐蚀与防护学报, 2022, 42(2): 235-242.
[4] DOU Jianye, QU Shaopeng, XUAN Xingyu. Service Behavior of Cerium Ion Modified SiO2 Film Prepared by Different Methods in Artificial Deep Sea Environments[J]. 中国腐蚀与防护学报, 2022, 42(2): 258-266.
[5] ZHANG Chenyang, LIU Huicong, HAN Dongxiao, ZHU Liqun, LI Weiping. Preparation of Micron SiC/Ni-Co-P Composite Coatings and Influencing Factors[J]. 中国腐蚀与防护学报, 2021, 41(5): 579-584.
[6] BAO Ren, ZHOU Genshu, LI Hongwei. Preparation of High-tin Bronze Corrosion-resistant Coating by Potentiostatic Pulse Electrodeposition[J]. 中国腐蚀与防护学报, 2020, 40(6): 585-591.
[7] YANG Yinchu,FU Xiuqing,LIU Lin,MA Wenke,SHEN Moqi. Electrochemical Corrosion of Ni-P-BN(h)-Al2O3 Composite Coating Deposited by Spray Electrodeposition[J]. 中国腐蚀与防护学报, 2020, 40(1): 57-62.
[8] Bin JIANG, Lilan ZENG, Tao LIANG, Haobo PAN, Yanxin QIAO, Jing ZHANG, Ying ZHAO. Directional Electrodeposition of Micro-nano Superhyd-rophobic Coating on 316L Stainless Steel[J]. 中国腐蚀与防护学报, 2018, 38(5): 438-446.
[9] Shibing DING,Tengfei XIANG,Cheng LI,Shunli ZHENG,Qi WANG,Mengping DU. A Simple Two-step Process for Fabrication of Super-hydrophobic Nickel Film by Electro-deposition Technique[J]. 中国腐蚀与防护学报, 2016, 36(5): 450-456.
[10] Qiongyu ZHOU,Xiaofen WANG,Qingdong ZHONG,Cao WANG,Yifeng HU. Effect of pH Value on Structure and Corrosion Resistance of Electrodeposited Ni-W Alloy Coating[J]. 中国腐蚀与防护学报, 2016, 36(5): 457-462.
[11] LUO Lili, FEI Jingyin, WANG Lei, LIN Xihua, WANG Shaolan. Alloying of Compositionally Modulated Cu/Ni Multilayer Films and Corrosion Performance of Cu-Ni Alloy Coatings[J]. 中国腐蚀与防护学报, 2014, 34(6): 523-531.
[12] LI Yuanyuan, DU Nan, SHU Weifa, WANG Shuaixing, ZHAO Qing. Electrodeposition Behavior of Zinc in Alkaline Zincate Electrolyte[J]. 中国腐蚀与防护学报, 2014, 34(1): 89-94.
[13] ZHANG Wuhua,FEI Jingyin,LUO Lili,LIN Xihua. High Speed Pulse Electro Plating Process of Nickel[J]. 中国腐蚀与防护学报, 2013, 33(4): 317-324.
[14] CHEN Ye, FEI Jingyin, WANG Lei, WAN Binghua. PULSE ELECTRODEPOSITION OF NICKEL MATRIX ALLOY COATINGS WITH HIGH CONTENT OF PHOSPHORUS[J]. 中国腐蚀与防护学报, 2012, 32(6): 501-506.
[15] WAN Binghua, FEI Jingyin, FENG Guangyong, ZHANG Wuhua, WANG Shaolan. PHOTOGENERATED CATHODE PROTECTION PROPERTIES OF Zn-Co-TiO2 NANOCOMPOSITE COATINGS[J]. 中国腐蚀与防护学报, 2012, 32(4): 327-332.
No Suggested Reading articles found!