Journal Home > Volume 16 , Issue 4
Nano Research 2023, 16(4): 4625-4633 https://doi.org/10.1007/s12274-022-5085-9
Research Article | Issue | Published: 26 October 2022

Upcycling PET in parallel with energy-saving H2 production via bifunctional nickel-cobalt nitride nanosheets

Show Author's Information Xuan Liu1,  Zhongying Fang2,  Dengke Xiong1,  Shuaiqi Gong1,  Yanli Niu1,  Wei Chen2,  Zuofeng Chen1 ( )
Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, Shanghai 200092, China
State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China
Keywords:
hydrogen evolution reaction, formic acid, nickel-cobalt nitride, polyethylene terephthalate upcycling, ethylene glycol oxidation
Topics:
Catalytic
Cite this article:
Liu X, Fang Z, Xiong D, et al. Upcycling PET in parallel with energy-saving H2 production via bifunctional nickel-cobalt nitride nanosheets. Nano Research, 2023, 16(4): 4625-4633. https://doi.org/10.1007/s12274-022-5085-9
Download citation
EndNote(RIS)
BibTeX

1047

Views

90

Downloads

Citations

29

Crossref

30

WoS

31

Scopus

1

CSCD

Abstract Full text Electronic supplementary material About this article

We describe here an electro-reforming strategy to upcycle polyethylene terephthalate (PET) waste with simultaneous hydrogen production by a bifunctional nickel-cobalt nitride nanosheets electrocatalyst. PET plastics are digested in alkaline solution giving an electrochemically active monomer ethylene glycol (EG). The introduction of Co in Co-Ni3N/carbon cloth (CC) promotes the redox behavior of Ni2+/Ni3+, which is beneficial for EG oxidation at an ultra-low potential (1.15 V vs. reversible hydrogen electrode (RHE)) and breaks through the limitation of high catalytic potentials of simple Ni-based electrocatalysts (1.30 V). In PET hydrolysate with Co-Ni3N/CC couples, an integrated EG oxidation-hydrogen production system achieves a current density of 50 mA·cm−2 at a cell voltage of 1.46 V, which is 370 mV lower than the conventional water splitting. The in-situ Raman and Fourier transform infrared (FTIR) spectroscopies and density functional theory (DFT) calculations identify the catalytic mechanism and point to advantages of heterostructure engineering in optimizing adsorption energies and promoting catalytic activities for EG oxidation.


menu
Abstract
Full text
Outline
Electronic supplementary material
About this article

Upcycling PET in parallel with energy-saving H2 production via bifunctional nickel-cobalt nitride nanosheets

Show Author's information Xuan Liu1, Zhongying Fang2, Dengke Xiong1, Shuaiqi Gong1, Yanli Niu1, Wei Chen2, Zuofeng Chen1 ( )
Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, Shanghai 200092, China
State Key Laboratory of Electroanalytical Chemistry, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China

Abstract

We describe here an electro-reforming strategy to upcycle polyethylene terephthalate (PET) waste with simultaneous hydrogen production by a bifunctional nickel-cobalt nitride nanosheets electrocatalyst. PET plastics are digested in alkaline solution giving an electrochemically active monomer ethylene glycol (EG). The introduction of Co in Co-Ni3N/carbon cloth (CC) promotes the redox behavior of Ni2+/Ni3+, which is beneficial for EG oxidation at an ultra-low potential (1.15 V vs. reversible hydrogen electrode (RHE)) and breaks through the limitation of high catalytic potentials of simple Ni-based electrocatalysts (1.30 V). In PET hydrolysate with Co-Ni3N/CC couples, an integrated EG oxidation-hydrogen production system achieves a current density of 50 mA·cm−2 at a cell voltage of 1.46 V, which is 370 mV lower than the conventional water splitting. The in-situ Raman and Fourier transform infrared (FTIR) spectroscopies and density functional theory (DFT) calculations identify the catalytic mechanism and point to advantages of heterostructure engineering in optimizing adsorption energies and promoting catalytic activities for EG oxidation.

Keywords: hydrogen evolution reaction, formic acid, nickel-cobalt nitride, polyethylene terephthalate upcycling, ethylene glycol oxidation

References(50)

[1]

Geyer, R.; Jambeck, J. R.; Law, K. L. Production, use, and fate of all plastics ever made. Sci. Adv. 2017, 3, e1700782.
DOI Google Scholar
[2]

Kakadellis, S.; Rosetto, G. Achieving a circular bioeconomy for plastics: Designing plastics for assembly and disassembly is essential to closing the resource loop. Science 2021, 373, 49–50.
DOI Google Scholar
[3]

Rahimi, A.; García, J. M. Chemical recycling of waste plastics for new materials production. Nat. Rev. Chem. 2017, 1, 0046.
DOI Google Scholar
[4]

Huerta Lwanga, E.; Gertsen, H.; Gooren, H.; Peters, P.; Salánki, T.; van der Ploeg, M.; Besseling, E.; Koelmans, A. A.; Geissen, V. Incorporation of microplastics from litter into burrows of Lumbricus terrestris. Environ. Pollut. 2017, 220, 523–531.
DOI Google Scholar
[5]

Nuelle, M. T.; Dekiff, J. H.; Remy, D.; Fries, E. A new analytical approach for monitoring microplastics in marine sediments. Environ. Pollut. 2014, 184, 161–169.
DOI Google Scholar
[6]

Achilias, D. S.; Tsintzou, G. P.; Nikolaidis, A. K.; Bikiaris, D. N.; Karayannidis, G. P. Aminolytic depolymerization of poly(ethylene terephthalate) waste in a microwave reactor. Polym. Int. 2011, 60, 500–506.
DOI Google Scholar
[7]

Thiounn, T.; Smith, R. C. Advances and approaches for chemical recycling of plastic waste. J. Polym. Sci. 2020, 58, 1347–1364.
DOI Google Scholar
[8]

Kim, H. T.; Hee Ryu, M.; Jung, Y. J.; Lim, S.; Song, H. M.; Park, J.; Hwang, S. Y.; Lee, H. S.; Yeon, Y. J.; Sung, B. H. et al. Chemo-biological upcycling of poly(ethylene terephthalate) to multifunctional coating materials. ChemSusChem 2021, 14, 4251–4259.
DOI Google Scholar
[9]

Rorrer, N. A.; Nicholson, S.; Carpenter, A.; Biddy, M. J.; Grundl, N. J.; Beckham, G. T. Combining reclaimed PET with bio-based monomers enables plastics upcycling. Joule 2019, 3, 1006–1027.
DOI Google Scholar
[10]

Kim, H. T.; Kim, J. K.; Cha, H. G.; Kang, M. J.; Lee, H. S.; Khang, T. U.; Yun, E. J.; Lee, D. H.; Song, B. K.; Park, S. J. et al. Biological valorization of poly(ethylene terephthalate) monomers for upcycling waste PET. ACS Sustainable Chem. Eng. 2019, 7, 19396–19406.
DOI Google Scholar
[11]

Zhang, F.; Wang, F.; Wei, X. Y.; Yang, Y.; Xu, S. M.; Deng, D. H.; Wang, Y. Z. From trash to treasure: Chemical recycling and upcycling of commodity plastic waste to fuels, high-valued chemicals and advanced materials. J. Energy Chem. 2022, 69, 369–388.
DOI Google Scholar
[12]

Ügdüler, S.; Van Geem, K. M.; Denolf, R.; Roosen, M.; Mys, N.; Ragaert, K.; De Meester, S. Towards closed-loop recycling of multilayer and coloured PET plastic waste by alkaline hydrolysis. Green Chem. 2020, 22, 5376–5394.
DOI Google Scholar
[13]

Karayannidis, G. P.; Chatziavgoustis, A. P.; Achilias, D. S. Poly(ethylene terephthalate) recycling and recovery of pure terephthalic acid by alkaline hydrolysis. Adv. Polym. Technol. 2002, 21, 250–259.
DOI Google Scholar
[14]

Kao, C. Y.; Cheng, W. H.; Wan, B. Z. Investigation of alkaline hydrolysis of polyethylene terephthalate by differential scanning calorimetry and thermogravimetric analysis. J. Appl. Polym. Sci. 1998, 70, 1939–1945.
DOI Google Scholar
[15]

Uekert, T.; Kuehnel, M. F.; Wakerley, D. W.; Reisner, E. Plastic waste as a feedstock for solar-driven H2 generation. Energy Environ. Sci. 2018, 11, 2853–2857.
DOI Google Scholar
[16]

Uekert, T.; Kasap, H.; Reisner, E. Photoreforming of nonrecyclable plastic waste over a carbon nitride/nickel phosphide catalyst. J. Am. Chem. Soc. 2019, 141, 15201–15210.
DOI Google Scholar
[17]

Zhu, J.; Hu, L. S.; Zhao, P. X.; Lee, L. Y. S.; Wong, K. Y. Recent advances in electrocatalytic hydrogen evolution using nanoparticles. Chem. Rev. 2020, 120, 851–918.
DOI Google Scholar
[18]

Yu, Z. Y.; Duan, Y.; Feng, X. Y.; Yu, X. X.; Gao, M. R.; Yu, S. H. Clean and affordable hydrogen fuel from alkaline water splitting: Past, recent progress, and future prospects. Adv. Mater. 2021, 33, 2007100.
DOI Google Scholar
[19]

Niu, Y. L.; Teng, X.; Gong, S. Q.; Xu, M. Z.; Sun, S. G.; Chen, Z. F. Engineering two-phase bifunctional oxygen electrocatalysts with tunable and synergetic components for flexible Zn-air batteries. Nano-Micro Lett. 2021, 13, 126.
DOI Google Scholar
[20]

Gong, S. Q.; Niu, Y. L.; Teng, X.; Liu, X.; Xu, M. Z.; Xu, C.; Meyer, T. J.; Chen, Z. F. Visible light-driven, selective CO2 reduction in water by In-doped Mo2C based on defect engineering. Appl. Catal. B: Environ. 2022, 310, 121333.
DOI Google Scholar
[21]

Han, C.; Li, W. J.; Wang, J. Z.; Huang, Z. G. Boron leaching: Creating vacancy-rich Ni for enhanced hydrogen evolution. Nano Res. 2022, 15, 1868–1873.
DOI Google Scholar
[22]

Zhang, Y. C.; Han, C. D.; Gao, J.; Pan, L.; Wu, J. T.; Zhu, X. D.; Zou, J. J. NiCo-based electrocatalysts for the alkaline oxygen evolution reaction: A review. ACS Catal. 2021, 11, 12485–12509.
DOI Google Scholar
[23]

Lei, Y. T.; Zhang, L. L.; Xu, W. J.; Xiong, C. L.; Chen, W. X.; Xiang, X.; Zhang, B.; Shang, H. S. Carbon-supported high-entropy Co-Zn-Cd-Cu-Mn sulfide nanoarrays promise high-performance overall water splitting. Nano Res. 2022, 15, 6054–6061.
DOI Google Scholar
[24]

Wang, S. C.; Liu, B. Y.; Wang, X.; Zhang, Y. J.; Huang, W. Nanoporous MoO3–x/BiVO4 photoanodes promoting charge separation for efficient photoelectrochemical water splitting. Nano Res. 2022, 15, 7026–7033.
DOI Google Scholar
[25]

Wang, Z. Y.; Xu, L.; Huang, F. Z.; Qu, L. B.; Li, J. T.; Owusu, K. A.; Liu, Z. A.; Lin, Z. F.; Xiang, B. H.; Liu, X. et al. Copper-nickel nitride nanosheets as efficient bifunctional catalysts for hydrazine-assisted electrolytic hydrogen production. Adv. Energy Mater. 2019, 9, 1900390.
DOI Google Scholar
[26]

Zheng, S. Y.; Qin, H. Y.; Cao, X. J.; Wang, T. Z.; Lu, W. B.; Jiao, L. F. Electron modulation of cobalt carbonate hydroxide by Mo doping for urea-assisted hydrogen production. J. Energy Chem. 2022, 70, 258–265.
DOI Google Scholar
[27]

Li, M.; Deng, X. H.; Liang, Y.; Xiang, K.; Wu, D.; Zhao, B.; Yang, H. P.; Luo, J. L.; Fu, X. Z. CoxP@NiCo-LDH heteronanosheet arrays as efficient bifunctional electrocatalysts for co-generation of value-added formate and hydrogen with less-energy consumption. J. Energy Chem. 2020, 50, 314–323.
DOI Google Scholar
[28]

Gao, L. F.; Liu, Z. B.; Ma, J. L.; Zhong, L. J.; Song, Z. Q.; Xu, J. N.; Gan, S. Y.; Han, D. X.; Niu, L. NiSe@NiOx core–shell nanowires as a non-precious electrocatalyst for upgrading 5-hydroxymethylfurfural into 2,5-furandicarboxylic acid. Appl. Catal. B: Environ. 2020, 261, 118235.
DOI Google Scholar
[29]

Liu, W. J.; Xu, Z. R.; Zhao, D. T.; Pan, X. Q.; Li, H. C.; Hu, X.; Fan, Z. Y.; Wang, W. K.; Zhao, G. H.; Jin, S. et al. Efficient electrochemical production of glucaric acid and H2 via glucose electrolysis. Nat. Commun. 2020, 11, 265.
DOI Google Scholar
[30]

Li, Y.; Wei, X. F.; Chen, L. S.; Shi, J. L. Electrocatalytic hydrogen production trilogy. Angew. Chem., Int. Ed. 2021, 60, 19550–19571.
DOI Google Scholar
[31]

Li, L. G.; Wang, P. T.; Shao, Q.; Huang, X. Q. Metallic nanostructures with low dimensionality for electrochemical water splitting. Chem. Soc. Rev. 2020, 49, 3072–3106.
DOI Google Scholar
[32]

Liu, X.; Wang, K. K.; Zhou, L. M.; Pu, H. K.; Zhang, T.; Jia, J.; Deng, Y. J. Shape-controlled synthesis of concave pt and willow-like Pt nanocatalysts via electrodeposition with hydrogen adsorption/desorption and investigation of their electrocatalytic performances toward ethanol oxidation reaction. ACS Sustainable Chem. Eng. 2020, 8, 6449–6457.
DOI Google Scholar
[33]

Ji, L. L.; Wang, J. Y.; Teng, X.; Meyer, T. J.; Chen, Z. F. CoP nanoframes as bifunctional electrocatalysts for efficient overall water splitting. ACS Catal. 2020, 10, 412–419.
DOI Google Scholar
[34]

Mondal, B.; Karjule, N.; Singh, C.; Shimoni, R.; Volokh, M.; Hod, I.; Shalom, M. Unraveling the mechanisms of electrocatalytic oxygenation and dehydrogenation of organic molecules to value-added chemicals over a Ni-Fe oxide catalyst. Adv. Energy Mater. 2021, 11, 2101858.
DOI Google Scholar
[35]

Li, J. N.; Li, J. L.; Liu, T.; Chen, L.; Li, Y. F.; Wang, H. L.; Chen, X. R.; Gong, M.; Liu, Z. P.; Yang, X. J. Deciphering and suppressing over-oxidized nitrogen in nickel-catalyzed urea electrolysis. Angew. Chem., Int. Ed. 2021, 60, 26656–26662.
DOI Google Scholar
[36]

Ni, S.; Qu, H. N.; Xu, Z. H.; Zhu, X. Y.; Xing, H. F.; Wang, L.; Yu, J. M.; Liu, H. Z.; Chen, C. M.; Yang, L. R. Interfacial engineering of the NiSe2/FeSe2 p–p heterojunction for promoting oxygen evolution reaction and electrocatalytic urea oxidation. Appl. Catal. B: Environ. 2021, 299, 120638.
DOI Google Scholar
[37]

Geng, S. K.; Zheng, Y.; Li, S. Q.; Su, H.; Zhao, X.; Hu, J.; Shu, H. B.; Jaroniec, M.; Chen, P.; Liu, Q. H. et al. Nickel ferrocyanide as a high-performance urea oxidation electrocatalyst. Nat. Energy 2021, 6, 904–912.
DOI Google Scholar
[38]

Wang, L. P.; Zhu, Y. J.; Wen, Y. Z.; Li, S. Y.; Cui, C. Y.; Ni, F. L.; Liu, Y. X.; Lin, H. P.; Li, Y. Y.; Peng, H. S. et al. Regulating the local charge distribution of Ni active sites for the urea oxidation reaction. Angew. Chem., Int. Ed. 2021, 60, 10577–10582.
DOI Google Scholar
[39]

Liu, X.; Fang, Z. Y.; Teng, X.; Niu, Y. L.; Gong, S. Q.; Chen, W.; Meyer, T. J.; Chen, Z. Paired formate and H2 productions via efficient bifunctional Ni-Mo nitride nanowire electrocatalysts. J. Energy Chem. 2022, 72, 432–441.
DOI Google Scholar
[40]

Barwe, S.; Weidner, J.; Cychy, S.; Morales, D. M.; Dieckhöfer, S.; Hiltrop, D.; Masa, J.; Muhler, M.; Schuhmann, W. Electrocatalytic oxidation of 5-(hydroxymethyl)furfural using high-surface-area nickel boride. Angew. Chem., Int. Ed. 2018, 57, 11460–11464.
DOI Google Scholar
[41]

Li, M.; Deng, X. H.; Xiang, K.; Liang, Y.; Zhao, B.; Hao, J.; Luo, J. L.; Fu, X. Z. Value-added formate production from selective methanol oxidation as anodic reaction to enhance electrochemical hydrogen cogeneration. ChemSusChem 2020, 13, 914–921.
DOI Google Scholar
[42]

Li, Y.; Wei, X. F.; Chen, L. S.; Shi, J. L.; He, M. Y. Nickel-molybdenum nitride nanoplate electrocatalysts for concurrent electrolytic hydrogen and formate productions. Nat. Commun. 2019, 10, 5335.
DOI Google Scholar
[43]

Sha, L. N.; Yin, J. L.; Ye, K.; Wang, G.; Zhu, K.; Cheng, K.; Yan, J.; Wang, G. L.; Cao, D. X. The construction of self-supported thorny leaf-like nickel-cobalt bimetal phosphides as efficient bifunctional electrocatalysts for urea electrolysis. J. Mater. Chem. A 2019, 7, 9078–9085.
DOI Google Scholar
[44]

Gao, X. R.; Yu, Y.; Liang, Q. R.; Pang, Y. J.; Miao, L. Q.; Liu, X. M.; Kou, Z. K.; He, J. Q.; Pennycook, S. J.; Mu, S. C. et al. Surface nitridation of nickel-cobalt alloy nanocactoids raises the performance of water oxidation and splitting. Appl. Catal. B: Environ. 2020, 270, 118889.
DOI Google Scholar
[45]

Zhu, C. R.; Wang, A. L.; Xiao, W.; Chao, D. L.; Zhang, X.; Tiep, N. H.; Chen, S.; Kang, J. N.; Wang, X.; Ding, J. et al. In situ grown epitaxial heterojunction exhibits high-performance electrocatalytic water splitting. Adv. Mater. 2018, 30, 1705516.
DOI Google Scholar
[46]

Chen, W.; Xu, L. T.; Zhu, X. R.; Huang, Y. C.; Zhou, W.; Wang, D. D.; Zhou, Y. Y.; Du, S. Q.; Li, Q. L.; Xie, C. et al. Unveiling the electrooxidation of urea: Intramolecular coupling of the N–N bond. Angew. Chem., Int. Ed. 2021, 60, 7297–7307.
DOI Google Scholar
[47]

Zhao, B.; Liu, J. W.; Wang, X. W.; Xu, C. Y.; Sui, P.; Feng, R. F.; Wang, L.; Zhang, J. J.; Luo, J. L.; Fu, X. Z. CO2-emission-free electrocatalytic CH3OH selective upgrading with high productivity at large current densities for energy saved hydrogen co-generation. Nano Energy 2021, 80, 105530.
DOI Google Scholar
[48]

Antolini, E.; Gonzalez, E. R. Alkaline direct alcohol fuel cells. J. Power Sources 2010, 195, 3431–3450.
DOI Google Scholar
[49]

Li, Y.; Wei, X. F.; Han, S. H.; Chen, L. S.; Shi, J. L. MnO2 electrocatalysts coordinating alcohol oxidation for ultra-durable hydrogen and chemical productions in acidic solutions. Angew. Chem., Int. Ed. 2021, 60, 21464–21472.
DOI Google Scholar
[50]

Gomes, J. F.; Garcia, A. C.; Gasparotto, L. H. S.; de Souza, N. E.; Ferreira, E. B.; Pires, C.; Tremiliosi-Filho, G. Influence of silver on the glycerol electro-oxidation over AuAg/C catalysts in alkaline medium: A cyclic voltammetry and in situ FTIR spectroscopy study. Electrochim. Acta 2014, 144, 361–368.
DOI Google Scholar
File
12274_2022_5085_MOESM1_ESM.pdf (1.3 MB)
Publication history
Copyright
Acknowledgements

Publication history

Received: 12 August 2022
Revised: 20 September 2022
Accepted: 21 September 2022
Published: 26 October 2022
Issue date: April 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 22072107 and 21872105), the Science & Technology Commission of Shanghai Municipality (No. 19DZ2271500), and the Fundamental Research Funds for the Central Universities.

Return