•  
  •  
 

Corresponding Author

Ming-Yan Wang(mingyanlyg@hotmail.com)

Abstract

The worldwide extensive release of carbon dioxide (CO2) has caused serious environmental pollution and unprecedented climate change problems. Thus, for the sustainable development of human society, it is very necessary to convert CO2 to renewable fuels through clean and economical processes. The electrochemical CO2 reduction reaction (CO2RR) is regarded as a promising approach for the recycling of carbon resource and the generation of sustainable fuels. However, the slow kinetics and formation of multiple products in CO2RR hinder its large-scale application. Hence, great research efforts are made to develop electrocatalysts with high product selectivity at low overpotential. Recently, nanostructured transition metal oxide based electrocatalysts have displayed quite exciting performances for the CO2RR, in terms of fast kinetics, selectivity and durability. Among the various metal oxides, cobalt oxides show high CO2RR activity, and selective for the formation of formic acid. In this paper, a hybrid of CoO nanoflowers grown onto three-dimensional (3D) reduced graphene oxide (RGO)@Ni foam (CoO/RGO@NF) was synthesized by a facile hydrothermal method. The composite electrode of CoO/RGO@NF was characterized by XRD and SEM. It is found that the CoO nanoflowers grew uniformly on the 3D network of RGO@NF electrode. The CoO nanoflowers were formed by a large number of nanorods around a center. The length of the nanorods was about 10 ~ 15 μm, and the diameter was about 100 ~ 200 nm. The electrocatalytic performance of CoO/RGO@NF composite electrode for CO2 reduction was studied by cyclic voltammetry and linear scanning voltammetry. The results showed that the current efficiency of CoO/RGO@NF electrode for electrocatalytic reduction of CO2 was 70.9% and the Faraday efficiency for formic acid production was 65.2%. In addition, the yield of formic acid on the electrode was 59.8 μmol·h-1·cm-2 at -0.76 V(vs. SHE) after 4 h of electrolysis. Furthermore, the current density was stable at about 90%. These data indicated that the as-prepared CoO/RGO@NF composite electrode had achieved excellent catalytic activity, selectivity and stability for CO2 electroreduction.

Graphical Abstract

Keywords

CO2 electrocatalysis, hydrothermal method, nickel foam, CoO nanoflowers

Publication Date

2021-08-28

Online Available Date

2020-06-28

Revised Date

2020-06-03

Received Date

2020-05-12

References

[1] Yuvraj Y B, Elena P G, Marta C F, Adrien J G, Federico C V, Marc T M K. Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels[J]. Nat. Energy, 2019, 4(9): 732-745.
doi: 10.1038/s41560-019-0450-y URL

[2] Zhang B H(张宝花), Zhang J T(张进涛). Regulation of copper surface via redox reactions for enhancing carbon dioxide electroreduction[J]. J. Electrochem.(电化学), 2019, 25(4): 497-503.

[3] Zhou T C(周天辰), He C(何川), Zhang Y N(张亚男), Zhao G H(赵国华). Photoelectrocatalytic reduction of CO2[J]. Progress Chem.(化学进展), 2012, 24(10): 1897-1905.

[4] Zhao X Y(赵叙言), Wang X Q(王潇乾), Wu Y E(吴宇恩). Research and development of single site catalyst in electrocatalytic reduction of CO2[J]. Sci. China - Chem.(中国科学: 化学), 2018, 48(9): 1027-1039.

[5] Li C W Kanan W. CO2 reduction at low overpotential on Cu electrodes resulting from the reduction of thick Cu2O films[J]. J. Am. Chem. Soc., 2012(17), 134: 7231-7234.
doi: 10.1021/ja3010978 URL

[6] Chen Y H, Kanan M W. Tin oxide dependence of the CO2 reduction efficiency on tin electrodes and enhanced activity for tin/tin oxide thin-film catalysts[J]. J. Am. Chem. Soc., 2012, 134(4): 1986-1989.
doi: 10.1021/ja2108799 URL

[7] Cao S, Lin Y, Jiao X C, Sun Y F, Luo Q Q, Zhang W H, Li D Q, Yang J L, Xie Y. Partially oxidized atomic cobalt layers for carbon dioxide electroreduction to liquid fuel[J]. Nature, 2016, 529(7584): 68-71.
doi: 10.1038/nature16455 URL

[8] Yang G(杨刚), Yu Z P(余志鹏), Zhang J(张杰), Liang Z X(梁振兴). A highly efficient flower-like cobalt catalyst for electroreduction of carbon dioxide[J]. Chinese J. Catal.(催化学报), 2018, 39(5): 914-919.

[9] Gao S, Jiao X C, Sun Z T, Zhang W H, Sun Y F, Wang C M, Hu Q T, Zu X L, Yang F, Yang S Y, Liang L, Wu J, Xie Y. Ultrathin CO3O4 layers realizing optimized CO2 electroreduction to formate[J]. Angew. Chem. Int. Ed., 2016, 55(2): 698-702.
doi: 10.1002/anie.201509800 URL

[10] Zhu Y W, Murali S, Cai WW, Li X S, Suk J W, Potts J R, Ruoff R S. Graphene and graphene oxide: Synjournal, properties, and applications[J]. Adv. Mater., 2010, 22(35): 3906-3924.
doi: 10.1002/adma.201001068 URL

[11] Geioushy R A, Khaled M M, Hakeem A S, Alhooshani K, Basheer C. High efficiency graphene/Cu2O electrode for the electrochemical reduction of carbon dioxide to ethanol[J]. J. Electroanal. Chem., 2017, 785: 138-143.
doi: 10.1016/j.jelechem.2016.12.029 URL

[12] Wu J J, Liu M J, Sharma P P, Yadav RM, Ma L L, Yang Y C, Zou X L, Zhou X D, Vajtai R, Yakobson B I, Lou J, Ajayan P M. Incorporation of nitrogen defects for efficient reduction of CO2 via two-electron pathway on three-dimensional graphene foam[J]. Nano Lett., 2016, 16(1): 466-470.
doi: 10.1021/acs.nanolett.5b04123 URL

[13] Wang M Y, Zhu W, Ma L, Ma J J, Zhang D E, Tong Z W, Chen J. Enhanced simultaneous detection of ractopamine and salbutamol — Via electrochemical-facial deposition of MnO2 nanoflowers onto 3D RGO/Ni foam templates[J]. Biosens. & Bioelectron., 2016, 78: 259-266.
doi: 10.1016/j.bios.2015.11.062 URL

[14] Hummers W S, Offeman R E. Preparation of graphitic oxide[J]. J. Am. Chem. Soc., 1958, 80(6): 1339-1339.
doi: 10.1021/ja01539a017 URL

[15] Zhuo M N(卓孟宁), Li F(李飞), Jiang H(蒋浩), Chen Q W(陈倩文), Li P(李鹏), Wang L Z(王立章). Preparation of SnO2/GDE cathodes and their electrocatalytic reduction of CO2 to produce formic acid[J]. Chem. J. Chinese U.(高等学校化学学报), 2020, 41(3): 530-537.

[16] Im H J, Jun G H, Lee D J, Ryu H J, Hong S H. Enhanced electromagnetic interference shielding behavior of grap-hene nanoplatelet/Ni/wax nanocomposites[J]. J. Mater. Chem. C, 2017, 5(26): 6471-6479.
doi: 10.1039/C7TC01405H URL

[17] Wang Q, Cai C Y, Wang M Y, Guo Q, Wang B, Luo W N, Wang Y J, Zhang C Y, Zhou L H, Zhang D E, Tong Z W, Liu Y Q, Chen J. Efficient photocatalytic degradation of malachite green in seawater by the hybrid of zinc-oxide nanorods grown on three-dimensional (3D) reduced graphene oxide (RGO)/Ni foam[J]. Materials, 2018, 11(6): 1004-1016.
doi: 10.3390/ma11061004 URL

[18] Zhang Y L, Zhu J, Song X, Zhong X. Controlling the synjournal of CoO nanocrystals with various morphologies[J] J. Phys. Chem. C, 2008, 112(14): 5322-5327.
doi: 10.1021/jp709943x URL

[19] Zhang L N(张莉娜), Wang J Y(王金意), Zhang H X(张涵轩), Cai W B(蔡文斌). A novel fabrication of RuO2/TiO2 nanofilms for electrocatalytic reduction of CO2[J]. Acta Chim. Sinica(化学学报), 2010, 68(6): 590-593.

Share

COinS
 
 

To view the content in your browser, please download Adobe Reader or, alternately,
you may Download the file to your hard drive.

NOTE: The latest versions of Adobe Reader do not support viewing PDF files within Firefox on Mac OS and if you are using a modern (Intel) Mac, there is no official plugin for viewing PDF files within the browser window.