Efficient electrocatalytic conversion of CO₂ to CO using Ag nanoparticles via high temperature thermal shock

Abstract

Exploring catalysts with high catalytic activity and low cost is crucial for promoting the electrocatalytic reduction of CO₂. In this study, Ag nanoparticle catalysts were synthesized on GS carbon and vapor grown carbon fiber (VGCF) carbon carriers using different silver precursors (AgAc, AgNO₃) through the ultrafast high temperature thermal shock method. The experimental results demonstrated that the performance of Ag catalysts for the electrocatalytic reduction of CO₂ to CO could be significantly enhanced by modulating the nanostructure, carrier, and metal loading. The VGCF-AgNO₃-HT nanoparticles exhibited a relatively regular spherical morphology, with smaller particle sizes and uniform distribution. Furthermore, the intricate and overlapping arrangement of VGCF carbon nanofibers contributed to increasing the active area for electrochemical reactions, making it an excellent catalyst carrier. Catalysts with varying Ag loadings were prepared using the thermal shock method, and it was observed that the nanoparticles maintained their superior nanostructures even with increased Ag loading. The Ag-HT-65 catalyst exhibited outstanding catalytic performance, achieving a CO Faradaic efficiency of 93.03% at a potential of −0.8 V (vs. RHE). After 12 h of testing, the CO Faradaic efficiency remained 90%, exhibiting an excellent stability.

References

[1] Mikkelsen M, Jørgensen M, Krebs F C. The teraton challenge. A review of fixation and transformation of carbon dioxide [J]. Energy & Environmental Science, 2010, 3(1): 43-81.

[2] Lv F, Han N, Qiu Y, et al.. Transition metal macrocycles for heterogeneous electrochemical CO₂ reduction [J]. Coordination Chemistry Reviews, 2020, 422: 213435.

[3] Zhao Y-f, He Liang. Electron distribution regulating of nonmetal doped monolayer g-GaN for enhanced electrocatalytic CO₂ reduction [J]. Applied Surface Science, 2024, 670: 160683.

[4] Wang C, He A, Zhang N-b, et al.. Zn-Bi bimetallic catalyst for electrochemical synthesis of C1 products by highly selective CO₂ reduction [J]. Journal of Catalysis, 2023, 428: 115128.

[5] Ross M B, De Luna P, Li Y-f, et al.. Designing materials for electrochemical carbon dioxide recycling [J]. Nature Catalysis, 2019, 2: 648-658.

[6] Birdja Y Y, Pérez-Gallent E, Figueiredo M C, et al.. Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels [J]. Nature Energy, 2019, 4: 732-745.

[7] Roy A, Jadhav H S, Park S J, et al.. Recent advances in the possible electrocatalysts for the electrochemical reduction of carbon dioxide into methanol [J]. Journal of Alloys and Compounds, 2021, 887: 161449.

[8] Usman M, Humayun M, Garba M D, et al.. Electrochemical reduction of CO₂: A review of cobalt based catalysts for carbon dioxide conversion to fuels [J]. Nanomaterials, 2021, 11(8): 2029.

[9] He J-f, Li Y-l, Huang A-x, et al.. Electrolyzer and catalysts design from carbon dioxide to carbon monoxide electrochemical reduction [J]. Electrochemical Energy Reviews, 2021, 4(4): 680-717.

[10] Yu X-h, Wu J, Yu J-y, et al.. Fabrication of Fe₃C nanoparticles encapsulated in undoped graphite carbon and their catalysis for oxygen reduction [J]. Journal of Central South University, 2023, 30(1): 35-48.

[11] Dang R, Xu X-f, Xie M-meng. Fabrication of triangular Cu₃P nanorods on Cu nanosheets as electrocatalyst for boosted electrocatalytic water splitting [J]. Journal of Central South University, 2022, 29(12): 3870-3883.

[12] Zhang Y-b, Wang P, Yu D, et al.. Evolution mechanism of active sites for selective catalytic reduction of NO_x with NH₃ over Fe-ZSM-5 catalysts doped by Ce/Cu [J]. Journal of Central South University, 2022, 29(7): 2239-2252.

[13] Bushuyev O S, de Luna P, Dinh C T, et al.. What should we make with CO₂ and how can we make it? [J]. Joule, 2018, 2(5): 825-832.

[14] Zhang W-j, Hu Y, Ma L-b, et al.. Progress and perspective of electrocatalytic CO₂ reduction for renewable carbonaceous fuels and chemicals [J]. Advanced Science, 2017, 5(1): 1700275.

[15] Choi J, Kim J, Wagner P, et al.. Highly ordered mesoporous carbon/iron porphyrin nanoreactor for the electrochemical reduction of CO₂ [J]. Journal of Materials Chemistry A, 2020, 8(30): 14966-14974.

[16] Kwon T, Prabhakaran S, Kim D H, et al.. Engineering hydrophobicity and high-index planes of gold nanostructures for highly selective electrochemical CO₂ reduction to CO and efficient CO₂ capture [J]. Chemical Engineering Journal, 2024, 485: 150045.

[17] Han L-l, Song S-j, Liu M-j, et al.. Stable and efficient single-atom Zn catalyst for CO₂ reduction to CH₄ [J]. Journal of the American Chemical Society, 2020, 142(29): 12563-12567.

[18] Shen S-b, Peng X-y, Song L-d, et al.. AuCu alloy nanoparticle embedded Cu submicrocone arrays for selective conversion of CO₂ to ethanol [J]. Small, 2019, 15(37): e1902229.

[19] Foit S R, Vinke I C, de Haart L G J, et al.. Power-to-syngas: An enabling technology for the transition of the energy system? [J]. Angewandte Chemie International Edition, 2017, 56(20): 5402-5411.

[20] Wang R, Peng Y, Chung J, et al.. Understanding of C=O bonding activation during CO₂ electroreduction: A case study of CO₂ reduction to CO on ZnO [J]. Chem Catalysis, 2023, 3(11): 100792.

[21] Zhou Q-c, Tang X-n, Qiu S-h, et al.. Stable CuIn alloy for electrochemical CO₂ reduction to CO with high-selectivity [J]. Materials Today Physics, 2023, 33: 101050.

[22] Wang Y-x, Cao L, Libretto N J, et al.. Ensemble effect in bimetallic electrocatalysts for CO₂ reduction [J]. Journal of the American Chemical Society, 2019, 141(42): 16635-16642.

[23] Chen Y-h, Li C W, Kanan M W. Aqueous CO₂ reduction at very low overpotential on oxide-derived Au nanoparticles [J]. Journal of the American Chemical Society, 2012, 134(49): 19969-19972.

[24] Yuan X-l, Wu Y-s, Jiang B, et al.. Interface engineering of silver-based heterostructures for CO₂ reduction reaction [J]. ACS Applied Materials & Interfaces, 2020, 12(50): 56642-56649.

[25] Zhu Z, Huang W-r, Chen C Y, et al.. Preparation of Pd-Au/TiO₂-WO₃ to enhance photoreduction of CO₂ to CH₄ and CO [J]. Journal of CO2 Utilization, 2018, 28: 247-254.

[26] Ding J, Bu Y-f, Ou M, et al.. Facile decoration of carbon fibers with Ag nanoparticles for adsorption and photocatalytic reduction of CO₂ [J]. Applied Catalysis B: Environmental, 2017, 202: 314-325.

[27] Zhang F, Li Y-h, Qi M-y, et al.. Boosting the activity and stability of Ag-Cu₂O/ZnO nanorods for photocatalytic CO₂ reduction [J]. Applied Catalysis B: Environmental, 2020, 268: 118380.

[28] Watmanee S, Klinaubol T, Nganglumpoon R, et al.. Origin of surface-bonded oxygen on dendritic Ag particles towards 3D-nanocrystalline carbon formation during CO₂ electrochemical reduction reaction [J]. Chemical Engineering Journal, 2024, 480: 148182.

[29] Zeng M, Wu Y-t, Wang Y, et al.. Silver nanoparticle-enhanced photocatalytic CO₂ reduction over Ag/Nb₂O₅ under UV-vis light irradiation [J]. Applied Catalysis A: General, 2023, 666: 119412.

[30] Hatsukade T, Kuhl K P, Cave E R, et al.. Insights into the electrocatalytic reduction of CO₂ on metallic silver surfaces [J]. Physical Chemistry Chemical Physics, 2014, 16(27): 13814-13819.

[31] Rosen J, Hutchings G S, Lu Q, et al.. Mechanistic insights into the electrochemical reduction of CO₂ to CO on nanostructured Ag surfaces [J]. ACS Catalysis, 2015, 5(7): 4293-4299.

[32] Back S, Yeom M S, Jung Y. Active sites of Au and Ag nanoparticle catalysts for CO₂ electroreduction to CO [J]. ACS Catalysis, 2015, 5(9): 5089-5096.

[33] Woldu A R. From low to high-index facets of noble metal nanocrystals: A way forward to enhance the performance of electrochemical CO₂ reduction [J]. Nanoscale, 2020, 12(16): 8626-8635.

[34] Zhang N-q, Zhang X-x, Tao L, et al.. Silver single-atom catalyst for efficient electrochemical CO₂ reduction synthesized from thermal transformation and surface reconstruction [J]. Angewandte Chemie, 2021, 133(11): 6235-6241.

[35] Deng W-y, Zhang L, Dong H, et al.. Achieving convenient CO₂ electroreduction and photovoltage in tandem using potential-insensitive disordered Ag nanoparticles [J]. Chemical Science, 2018, 9(32): 6599-6604.

[36] Liu S-b, Tao H-b, Zeng L, et al.. Shape-dependent electrocatalytic reduction of CO₂ to CO on triangular silver nanoplates [J]. Journal of the American Chemical Society, 2017, 139(6): 2160-2163.

[37] Fan T-t, Wu Q-l, Yang Z, et al.. Electrochemically driven formation of sponge-like porous silver nanocubes toward efficient CO₂ electroreduction to CO [J]. ChemSusChem, 2020, 13(10): 2677-2683.

[38] Ham Y S, Choe S, Kim M J, et al.. Electrodeposited Ag catalysts for the electrochemical reduction of CO₂ to CO [J]. Applied Catalysis B: Environmental, 2017, 208: 35-43.

[39] Kim C, Eom T, Jee M S, et al.. Insight into electrochemicalc CO₂ reduction on surface-molecule-mediated Ag nanoparticles [J]. ACS Catalysis, 2017, 7(1): 779-785.

[40] Hsieh Y C, Betancourt L E, Senanayake S D, et al.. Modification of CO₂ reduction activity of nanostructured silver electrocatalysts by surface halide anions [J]. ACS Applied Energy Materials, 2019, 2(1): 102-109.

[41] Gustavsen K R, Huang H, Johannessen E A, et al.. Boron-induced growth of highly textured Ag (111) films with nano-tentacle structures for the electrochemical reduction of CO₂ to CO [J]. Electrochemistry Communications, 2023, 156: 107600.

[42] Zhang T, Lu X-y, Qi W, et al.. Efficient electroreduction of CO₂ to CO on silver single-atom catalysts: Activity enhancement through coordinated modulation of polyaniline [J]. Applied Catalysis B: Environment and Energy, 2024, 349: 123896.

[43] Gengzang D-j, Chen W-j, Chen Q, et al.. Optimized ZnSn(OH)₆ porous hollow microspheres via doping Ag for detecting formaldehyde [J]. Journal of Alloys and Compounds, 2023, 967: 171623.

[44] Yang M, Zhang J-z, Cao Y-y, et al.. Facet sensitivity of capping ligand-free Ag crystals in CO₂ electrochemical reduction to CO [J]. ChemCatChem, 2018, 10(22): 5128-5134.

[45] Wang G-y, Liang Y, Song J, et al.. Study on high activity and outstanding stability of hollow-NiPt@SiO₂ core-shell structure catalyst for DRM reaction [J]. Frontiers in Chemistry, 2020, 8: 220.

RIGHTS & PERMISSIONS

Central South University