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Paired electrolysis offers an auspicious strategy for the generation of high‐value chemicals, at both the anode and cathode, in an integrated electrochemical reactor. Through efficient electron utilization, routine product misuse at overlooked electrodes can be prevented. Here, an original paired electrosynthetic system is reported that can convert CO2 to ethylene (C2H4) at the cathode, and water to hydrogen peroxide (H2O2) at the anode under a single pass of electric charge. Amongst various investigated copper (Cu) nanomorphologies, the bespoke mixed Cu nanowire/nanoparticle catalyst recorded a peak C2H4 Faraday efficiency (FE) of 60% following 370 h of electrolysis at 200 mA cm−2, while the tailored boron‐doped diamond (BDD) anode accumulated an unprecedented ≈1% w/w of H2O2 in 4 m K2CO3 upon applying 300 mA cm−2 for 10 h. When paired, the dual C2H4‐H2O2 electrochemical cell attains a combined FE of 120% for 50 h at 200 mA cm−2, a combined energy efficiency (EE) of 69%, and a 50% decrease in the overall electrical energy consumption (EEC) compared to the individual electrosynthesis of C2H4 and H2O2. [ABSTRACT FROM AUTHOR]

Electrochemical synthesis of hydrogen peroxide (H2O2), via the two‐electron water oxidation reaction (2e− WOR), is an attractive method for the sustainable production of valuable chemicals in place of oxygen during water electrolysis. While the majority of 2e− WOR studies have focussed on electrocatalyst design, little research has been carried out on the selection of the supporting electrolyte. In this work, we investigate the impact of potassium carbonate (K2CO3) electrolytes, and their key properties, on H2O2 production. We found that at electrolyte pH values (>9.5) where the carbonate anion (CO32−) was prevalent in the mixture, a 26.5 % increase in the Faraday efficiency (%FE) for H2O2 production was achieved, compared to bicarbonate (HCO3−) dominant solutions. Utilising boron‐doped diamond (BDD) in highly concentrated K2CO3 solutions, current densities of up to 511 mA cm−2 (in 4 m) and %FEs of 91.5 % (in 5 m) could be attained. The results presented in this work highlight the influence of CO32− on electrochemical H2O2 generation via the 2e− WOR and provide novel pathways to produce desirable commodities at the anode during electrochemical water splitting. [ABSTRACT FROM AUTHOR]

The electrochemical reduction of CO2 continues to see significant interest as a viable means of both producing important chemical materials and lowering carbon emissions. The primary challenge to making this process economically viable is the design of catalyst, electrode and reactor components that can selectively produce just one of the many possible CO2 reduction products. In this work, we report the use of hydrophobic 1-octadecanethiol coatings at copper coated gas diffusion electrodes to enhance the production of ethylene. This thiol coating gives a substantial increase in the production of ethylene at low current densities as well as a change in the rate determining step, as indicated by the substantial reduction in the Tafel slope. The observed changes to the CO2 reduction reaction indicate that the thiol layer provides a triphasic interface within the gas diffusion electrode catalyst layer. [ABSTRACT FROM AUTHOR]