This paper reviews recent progress made in identifying electrocatalysts for carbon dioxide (CO2) reduction to produce low-carbon fuels, including CO, HCOOH/HCOO−, CH2O, CH4, H2C2O4/HC2O4−, C2H4, CH3OH, CH3CH2OH and others. The electrocatalysts are classified into several categories, including metals, metal alloys, metal oxides, metal complexes, polymers/clusters, enzymes and organic molecules. The catalyts' activity, product selectivity, Faradaic efficiency, catalytic stability and reduction mechanisms during CO2 electroreduction have received detailed treatment. In particular, we review the effects of electrode potential, solution–electrolyte type and composition, temperature, pressure, and other conditions on these catalyst properties. The challenges in achieving highly active and stable CO2 reduction electrocatalysts are analyzed, and several research directions for practical applications are proposed, with the aim of mitigating performance degradation, overcoming additional challenges, and facilitating research and development in this area.

A review of catalysts for the electroreduction of carbon dioxide to produce low-carbon fuels

The recent literature on photochemical and photoelectrochemical reductions of CO(2) is reviewed. The different methods of achieving light absorption, electron-hole separation, and electrochemical reduction of CO(2) are considered. Energy gap matching for reduction of CO(2) to different products, including CO, formic acid, and methanol, is used to identify the most promising systems. Different approaches to lowering overpotentials and achieving high chemical selectivities by employing catalysts are described and compared.

https://www.annualreviews.org/doi/pdf/10.1146/annurev-physchem-032511-143759

Photochemical and Photoelectrochemical Reduction of CO2

Synthesis and Applications of Boronic Acid-Containing Polymers: From Materials to Medicine.

With rising levels of CO2 in our atmosphere, technologies capable of converting CO2 into useful products have become more valuable. The field of electrochemical CO2 reduction is reviewed here, with sections on mechanism, formate (formic acid) production, carbon monoxide production, reduction to higher products (methanol, methane, etc.), use of flow cells, high pressure approaches, molecular catalysts, non-aqueous electrolytes, and solid oxide electrolysis cells. These diverse approaches to electrochemical CO2 reduction are compared and contrasted, emphasizing potential processes that would be feasible for large-scale use. Although the focus is on recent reports, highlights of older reports are also included due to their important contributions to the field, particularly for high-rate electrolysis.

Electrochemical CO2 Reduction: Recent Advances and Current Trends

Electrocatalytic CO2 reduction by heterogeneous molecular catalysts is emerging as an important area for CO2 utilization. Unlike commonly used solid heterogeneous catalysts, molecular catalysts possess well-defined structure, which allows the establishment of a precise structural model for better understanding of the CO2 reduction mechanism. The easy modification of molecular catalysts with designated functional fragments through organic synthesis skills also facilitates the development of novel and efficient molecular catalysts. The direct use of molecular catalysts in the homogeneous phase suffers from poor solubility in some common solvents, low utilization and difficulty in recycling. Heterogeneous immobilization of molecular catalysts onto a substrate can potentially solve these problems. This review summarizes the methods that have been developed so far for heterogeneous immobilization of homogeneous molecular catalysts, including covalent/non-covalent bonding, and assembling the molecular catalysts into a periodic skeleton. Challenges and factors affecting the activities of such catalysts in electrochemical CO2 reduction are also discussed.

Electrocatalytic reduction of carbon dioxide: opportunities with heterogeneous molecular catalysts

Electrocatalytic reduction of carbon dioxide by a polymeric film of rhenium tricarbonyl dipyridylamine

Ruthenium(II) terpyridine complexes containing the pyrrole-tagged 2,2′-dipyridylamine ligand PPP (where PPP stands for N-(3-bis(2-pyridyl)aminopropyl)pyrrole with the general formula [Ru(tpy)(PPP)X]n+ (1, X = Cl–; 2, X = H2O; 3, X = CH3CN; tpy = 2,2′:6′,2″-terpyridine) have been synthesized and characterized by 1H NMR, IR, UV–vis, mass spectrometry, and elemental analysis. 1 and 2 have been structurally characterized by X-ray crystallography. Both 1 and 2 were successfully immobilized onto glassy carbon electrode via anodic oxidation of the pyrrole moiety on the PPP ligand to give stable and highly electroactive polymer films. Cyclic voltammetric studies of 1 in acetonitrile revealed a RuIII/RuII couple at 0.4 V vs Cp2Fe+/0 initially, but another redox couple resulting from chloride substitution by acetonitrile developed at E1/2 = 0.82 V upon repetitive potential scan. This ligand substitution was induced by the acidic local environment caused by the release of protons during pyrrole polymerization. The e...

Ruthenium terpyridine complexes containing a pyrrole-tagged 2,2'-dipyridylamine ligand-synthesis, crystal structure, and electrochemistry.

The Mn 2+ /HCO 3 − /H 2 O 2 catalytic system exhibits excellent aldehyde selectivity in the oxidation of various benzylic and allyic alcohols under mild conditions and short reaction time when the reactions are carried out in a biphasic dicationic pyrrolidinium ionic liquid/ n -heptane medium. The dicationic pyrrolidinium ionic liquid shows differential solubility towards alcohols and their aldehydes whereas the immiscible n -heptane instantaneously extracted and separated aldehydes from the reaction phase. This design of biphasic ionic liquid/ n -heptane catalytic system prevents the over-oxidation of aldehydes to carboxylic acids effectively. Separation and recycling can also be easily done by decantation of the n -heptane layer after reaction. With the biphasic system, high conversion of benzyl alcohol to benzaldehyde was achieved with very low loadings of H 2 O 2 and Mn(OAc) 2 catalyst at room temperature and within short reaction time. Throughout 10 reaction cycles, a total turnover number (TON) of 37,600 was achieved and excellent catalytic reactivity and selectivity were maintained with an average yield of 94%.

Controlling the selectivity of the manganese/bicarbonate/hydrogen peroxide catalytic system by a biphasic pyrrolidinium ionic liquid/n-heptane medium

Molecularly imprinted polymeric films were prepared on the surface of a gold electrode by reductive electrochemical co-polymerization of 3-acrylamidophenylboronic acid (AABA), acrylamide (as spacer monomer), and N,N′-methylenebisacrylamide (as crosslinker monomer) in the presence of dopamine in water. The analytical determination of dopamine was investigated with this molecularly imprinted poly(AABA) film-modified gold electrode using cyclic voltammetry, electrochemical quartz crystal balance, and differential pulse voltammetry. The covalent nature of dopamine-boronic acid interaction as well as the negative charge on the molecularly imprinted polymeric film at physiological pH allowed excellent selectivity against ascorbic acid and other structurally similar interferents. The sensitivity of molecularly imprinted poly(AABA)-modified electrode was further improved by depositing a thin layer of multiwalled carbon nanotubes on the gold electrode surface prior to electropolymerization. The increased surface area due to the presence of carbon nanotubes improved the dopamine sensor’s detection limit to ∼20 nM as determined by differential pulse voltammetry. A linear dependence of peak current in the differential pulse voltammograms was obtained over the dopamine concentration range from 50 nM to 2 µM.

A dopamine electrochemical sensor based on molecularly imprinted poly(acrylamidophenylboronic acid) film

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Electrocatalytic reduction of carbon dioxide by a polymeric film of rhenium tricarbonyl dipyridylamine

Ruthenium terpyridine complexes containing a pyrrole-tagged 2,2'-dipyridylamine ligand-synthesis, crystal structure, and electrochemistry.

Controlling the selectivity of the manganese/bicarbonate/hydrogen peroxide catalytic system by a biphasic pyrrolidinium ionic liquid/n-heptane medium

A dopamine electrochemical sensor based on molecularly imprinted poly(acrylamidophenylboronic acid) film