Electrolytic Reduction of Carbon Dioxide at Mercury Electrode in Aqueous Solution

Hori, Yoshio; Suzuki, Shin

doi:10.1246/bcsj.55.660

Cited by 140CO2 Reduction Techniques and CatalystsElectrocatalysts for Energy ConversionElectrochemical Analysis and Applications

Electrolytic Reduction of Carbon Dioxide at Mercury Electrode in Aqueous Solution

Hori, Yoshio, Suzuki, Shin·1982·Bulletin of the Chemical Society of Japan

DOI 10.1246/bcsj.55.660

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Abstract

Cathodic reduction of carbon dioxide at a mercury pool electrode was investigated in aqueous solutions of NaHCO3, NaH2PO4–Na2HPO4, NaCl, NaClO4, Na2SO4, LiHCO3, and KHCO3 as well as their combinations. The reaction product was confirmed to be HCOO− by a qualitative spot test. HCOO− was quantitatively analyzed by a permanganate titration. The partial current densities of HCOO− formation (ic) and H2 evolution (iH) were calculated. In the present paper, relationships between electrode behavior and solution properties, some of which have been qualitatively described in previous papers, are quantitatively clarified as follows. The electrode potential Ec for constant ic (0.5 mA/cm2) remains constant irrespective of pH and anions in the pH region of 2.4 to 7.8, whereas the potential EH for constant iH (0.5 mA/cm2) varies linearly with a slope of 125 mV/pH. The present experimental results verify Eyring et al.’s presumption that in a relatively high overvoltage region (region 2) the cathodic reduction of CO2 at Hg proceeds with the charge transfer to CO2 as the rate determining step. CO2 reduction and H2 evolution are concluded to proceed independently at the Hg electrode. The dependence of Ec on electrolyte concentration is interpreted in terms of the diffuse double layer theory. The effect of cation species on Ec also is discussed.

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To produce hydrocarbons on pressurized Cu, the current density must be increased.
“To produce hydrocarbons on pressurized Cu, the current density must be increased.[206,222]”
From Electrochemical CO 2 Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [222]
The primary benefit of elevated pressure is enhanced CO2 solubility in aqueous electrolytes, which allows for higher CO2RR current densities.
“The primary benefit of elevated pressure is well-evidenced in H cell reactors, the enhanced CO2 solubility in aqueous electrolytes, which allows for higher CO2RR current densities [221,222] .”
From Electrochemical CO 2 Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [222]
For Cu catalysts, increasing pressure typically results in increased CO production at the same applied potential due to stimulated desorption of intermediates from the surface.
“For Cu catalysts, increasing pressure typically results in increased CO production at the same applied potential [222,231] due to stimulated desorption of intermediates from the surface.[232,233]”
From Electrochemical CO 2 Reduction into Chemical Feedstocks: From Mechanistic Electrocatalysis Models to System Design (2019) · cites this paper as [222]

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Ohmori, T., Nakayama, A., Mametsuka, H., & Suzuki, E. (2001) · Journal of Electroanalytical Chemistry · doi:10.1016/s0022-0728(01)00624-6 · Cited by 39 · see citing works
Photoelectrochemical reduction of carbon dioxide on a p+/p-Si photocathode in aqueous electrolyte
Junfu, L., & Baozhu, C. (1992) · Journal of Electroanalytical Chemistry · doi:10.1016/0022-0728(92)80045-6 · Cited by 39 · see citing works
Mechanistic Insights Into H 2 O Dissociation in Overall Photo‐/Electro‐Catalytic CO 2 Reduction
Ma, M., Fang, Y., Huang, Z., Wu, S., He, W., Ge, S., Zheng, Z. G., Zhou, Y., Fa, W., & Wang, X. (2025) · Angewandte Chemie International Edition · doi:10.1002/anie.202425195 · Cited by 36 · see citing works
The influence of electrolyte identity upon the electro-reduction of CO2
Setterfield-Price, B. M., & Dryfe, R. A. W. (2014) · Journal of Electroanalytical Chemistry · doi:10.1016/j.jelechem.2014.07.009 · Cited by 36 · see citing works
Comparing the electrocatalytic reduction of CO2 to CO on gold cathodes in batch and continuous flow electrochemical cells
Ahangari, H. T., Portail, T., & Marshall, A. T. (2019) · Electrochemistry Communications · doi:10.1016/j.elecom.2019.03.005 · Cited by 36 · see citing works
Recent Advances in the Electroreduction of CO2 over Heteroatom-Doped Carbon Materials
Pérez-Sequera, A. C., Díaz-Pérez, M., & Serrano-Ruiz, J. C. (2020) · Catalysts · doi:10.3390/catal10101179 · Cited by 25 · see citing works
Modeling electrochemical CO 2 reduction at silver gas diffusion electrodes using a TFFA approach
Löffelholz, M., Osiewacz, J., Lüken, A., Perrey, K., Bulan, A., & Turek, T. (2022) · Chemical Engineering Journal · doi:10.1016/j.cej.2022.134920 · Cited by 36 · see citing works
Alkali Metal Cations Induce Structural Evolution on Au(111) During Cathodic Polarization
Wang, Y., Fu, J., Feng, Y., Zhao, K., Wang, L., Cai, J.-Y., Wang, X., Chen, T., Yang, F., Hu, J., et al. (2024) · Journal of the American Chemical Society · doi:10.1021/jacs.4c09404 · Cited by 35 · see citing works
The adsorption of CO2, H2CO3, HCO3− and CO32− on Cu2O (111) surface: First‐principles study
Wu, H., Zhang, N., Cao, Z., Wang, H., & Hong, S. (2011) · International Journal of Quantum Chemistry · doi:10.1002/qua.23250 · Cited by 34 · see citing works
Reactivity of Copper Electrodes towards Functional Groups and Small Molecules in the Context of CO2 Electro-Reductions
Schmid, B., Reller, C., Neubauer, S., Fleischer, M., Dorta, R., & Schmid, G. (2017) · Catalysts · doi:10.3390/catal7050161 · Cited by 33 · see citing works
“Pioneering work in CO2 reduction was done by Hori [8] and Paik [9] on mercury electrodes.”
Background
Decision tree analysis for efficient CO2 utilization in electrochemical systems
Günay, M. E., Türker, L., & Tapan, N. A. (2018) · Journal of CO2 Utilization · doi:10.1016/j.jcou.2018.09.011 · Cited by 33 · see citing works
Towards understanding of CO 2 electroreduction to C 2+ products on copper‐based catalysts
Liu, T., Sang, J., Li, H., Wei, P., Zang, Y., & Wang, G. (2022) · Battery energy · doi:10.1002/bte2.20220012 · Cited by 33 · see citing works
“The first one proposed by Hori et al.(76,77) argued that the potential was charged by cations in the electric double layer through specific adsorption.”
Background
Modeling mass transfer limitations driven by electrowetting in electrochemical CO2 reduction at silver gas diffusion electrodes
Osiewacz, J., Löffelholz, M., Ellendorff, B., & Turek, T. (2024) · Journal of Power Sources · doi:10.1016/j.jpowsour.2024.234430 · Cited by 28 · see citing works
CO2 Reduction Using Electrochemical Approach
Hori, Y. (2016) · Lecture notes in energy · doi:10.1007/978-3-319-25400-5_12 · Cited by 27 · see citing works
Self-citation
Interfaced Ag/Cu nanostructures derived from metal thiolate nanoplates: A highly selective catalyst for electrochemical reduction of CO2 to ethanol
Abeyweera, S. C., Simukaitis, M., Wei, Q., & Sun, Y. (2022) · SmartMat · doi:10.1002/smm2.1096 · Cited by 27 · see citing works
“1–14 Metallic nanostructures have been studied as a class of exciting catalysts since Hori et al.(15,16) pioneeringly explored the possibility of eCO2RR on metals (e.”
Background
Mechanism of nickel-catalysed electron transfer activation of aromatic halides
Amatore, C. A., & Jutand, A. (1991) · Journal of Electroanalytical Chemistry · doi:10.1016/0022-0728(91)85227-g · Cited by 27 · see citing works
Perspective on the interfacial engineering for electrocatalytic N2 to NH3 conversion from catalysts to systems
Choe, S., Kim, N., & Jang, Y. J. (2023) · EcoEnergy · doi:10.1002/ece2.10 · Cited by 24 · see citing works
Electrochemical reduction of CO2 to formic acid on Bi2O2CO3/carbon fiber electrodes
Puppin, L. G., Khalid, M., da Silva, G. T. S. T., Ribeiro, C., Varela, H., & Lopes, O. F. (2020) · Journal of materials research/Pratt's guide to venture capital sources · doi:10.1557/jmr.2020.16 · Cited by 25 · see citing works
Mechanism of electrochemical carbon dioxide reduction to formate on tin electrode
Naikkath, A., Mohan, N. G., Ramanujam, K., & Srinivasan, R. (2024) · Chemical Engineering Journal · doi:10.1016/j.cej.2024.148972 · Cited by 23 · see citing works
Electrochemical reduction of carbon dioxide on hydrogen-storing materials: Part 4. Electrochemical behavior of the Pd electrode in aqueous and nonaqueous electrolyte
Ohkawa, K., Noguchi, Y., Nakayama, S., Hashimoto, K., & Fujishima, A. (1994) · Journal of Electroanalytical Chemistry · doi:10.1016/0022-0728(94)87105-1 · Cited by 23 · see citing works
The role of malachite nanorods for the electrochemical reduction of CO2 to C2 hydrocarbons
Spodaryk, M., Zhao, K., Zhang, J., Oveisi, E., & Züttel, A. (2018) · Electrochimica Acta · doi:10.1016/j.electacta.2018.11.124 · Cited by 22 · see citing works
Voltammetry of carbon dioxide. Part 2. Voltammetry in aqueous solutions on glassy carbon
Eggins, B. R., Bennett, E. M., & McMullan, E. A. (1996) · Journal of Electroanalytical Chemistry · doi:10.1016/0022-0728(96)04590-1 · Cited by 21 · see citing works
Unraveling the Simultaneous Enhancement of Selectivity and Durability on Single‐Crystalline Gold Particles for Electrochemical CO2 Reduction
Lim, Y. J., Seo, D., Abbas, S. A., Jung, H., Ma, A., Lee, K., Lee, G., Lee, H., & Nam, K. M. (2022) · Advanced Science · doi:10.1002/advs.202201491 · Cited by 20 · see citing works
Electrochemical reduction of CO2 to liquid products: Factors influencing production and selectivity
Khan, R. R. M., Saleem, R., Batool, S. S., Rasheed, S., Saeed, Z., Pervaiz, M. A., Younas, U., Summer, M., & Liaqat, M. (2025) · International Journal of Hydrogen Energy · doi:10.1016/j.ijhydene.2025.04.077 · Cited by 19 · see citing works
Mechanistic Insights Into H 2 O Dissociation in Overall Photo‐/Electro‐Catalytic CO 2 Reduction
Ma, M., Fang, Y., Huang, Z., Wu, S., He, W., Ge, S., Zheng, Z., Zhou, Y., Fa, W., & Wang, X. (2025) · Angewandte Chemie · doi:10.1002/ange.202425195 · Cited by 20 · see citing works

Kinetic studies of the electrolytic reduction of carbon dioxide on the mercury electrode
Paik, W., Andersen, T. N., & Eyring, H. B. (1969) · Electrochimica Acta · doi:10.1016/0013-4686(69)87019-2 · Cited by 192 · see citing works
Product Selectivity Affected by Cationic Species in Electrochemical Reduction of CO2 and CO at a Cu Electrode
Murata, A., & Hori, Y. (1991) · Bulletin of the Chemical Society of Japan · doi:10.1246/bcsj.64.123 · Cited by 544 · see citing works
Self-citation
Photocurrent kinetics at the electron emission from a metal into electrolyte solution Part VII. Absolute rate constants of CO2 electrochemical reduction on mercury
Babenko, S. D. (1983) · Journal of Electroanalytical Chemistry (1959) · doi:10.1016/0368-1874(83)80523-1
Electrolytic Reduction of Bicarbonate Ion at a Mercury Electrode
Hori, Y., & Suzuki, S. (1983) · Journal of The Electrochemical Society · doi:10.1149/1.2119593 · Cited by 85 · see citing works
Self-citation
Effect of Electrolyte on the Electrochemical Reduction of CO2
Salazar-Villalpando, M. D. (2011) · ECS Transactions · doi:10.1149/1.3565504 · Cited by 23 · see citing works

Authors: Hori, Y., & Suzuki, S.
Affiliations: Chiba University (JP)
ORCID: Suzuki, Shin
Venue: Bulletin of the Chemical Society of Japan
Publisher: Oxford University Press (OUP)
Published: 1982-03-01
Volume: 55
Issue: 3
Pages: 660-665
ISSN: 0009-2673 (ISSN-L)
1348-0634
DOI: 10.1246/bcsj.55.660
OpenAlex: W2082327469
Cited by: 140
References: 8
Citations by year: 2026: 3 · 2025: 12 · 2024: 9 · 2023: 7 · 2022: 6 · 2021: 15 · 2020: 8 · 2019: 9 · 2018: 6 · 2017: 9 · 2016: 11 · 2015: 4 · 2014: 4 · 2013: 3 · 2012: 4
FWCI: 3.39
Type: journal article
Language: en
Open access: closed
Licence: academic.oup.com/pages/standard-publication-reuse-rights (vor)
Locations: Bulletin of the Chemical Society of Japan (publishedVersion)
Topics: Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › CO2 Reduction Techniques and Catalysts
Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
Physical Sciences › Chemistry › Electrochemistry › Electrochemical Analysis and Applications
Keywords: electrochemical CO2 reduction, mercury electrode, formate formation, hydrogen evolution reaction, electrode potential, pH dependence, anion effects, electrolyte concentration, diffuse double layer, cation effects, rate-determining step, sodium bicarbonate, sodium phosphate, sodium perchlorate, sodium sulfate, potassium bicarbonate

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Electrolytic Reduction of Carbon Dioxide at Mercury Electrode in Aqueous Solution

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