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      Stand-alone asymmetric hollow fiber gas-diffusion electrodes with distinguished bronze phases for high-efficiency CO2 electrochemical reduction

      , , , , , , , ,
      Applied Catalysis B: Environmental
      Elsevier BV

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          Enhanced electrocatalytic CO2 reduction via field-induced reagent concentration.

          Electrochemical reduction of carbon dioxide (CO2) to carbon monoxide (CO) is the first step in the synthesis of more complex carbon-based fuels and feedstocks using renewable electricity. Unfortunately, the reaction suffers from slow kinetics owing to the low local concentration of CO2 surrounding typical CO2 reduction reaction catalysts. Alkali metal cations are known to overcome this limitation through non-covalent interactions with adsorbed reagent species, but the effect is restricted by the solubility of relevant salts. Large applied electrode potentials can also enhance CO2 adsorption, but this comes at the cost of increased hydrogen (H2) evolution. Here we report that nanostructured electrodes produce, at low applied overpotentials, local high electric fields that concentrate electrolyte cations, which in turn leads to a high local concentration of CO2 close to the active CO2 reduction reaction surface. Simulations reveal tenfold higher electric fields associated with metallic nanometre-sized tips compared to quasi-planar electrode regions, and measurements using gold nanoneedles confirm a field-induced reagent concentration that enables the CO2 reduction reaction to proceed with a geometric current density for CO of 22 milliamperes per square centimetre at -0.35 volts (overpotential of 0.24 volts). This performance surpasses by an order of magnitude the performance of the best gold nanorods, nanoparticles and oxide-derived noble metal catalysts. Similarly designed palladium nanoneedle electrocatalysts produce formate with a Faradaic efficiency of more than 90 per cent and an unprecedented geometric current density for formate of 10 milliamperes per square centimetre at -0.2 volts, demonstrating the wider applicability of the field-induced reagent concentration concept.
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            Frontiers, opportunities, and challenges in biochemical and chemical catalysis of CO2 fixation.

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              CO2 electrolysis to multicarbon products at activities greater than 1 A cm−2

              Electrolysis offers an attractive route to upgrade greenhouse gases such as carbon dioxide (CO 2 ) to valuable fuels and feedstocks; however, productivity is often limited by gas diffusion through a liquid electrolyte to the surface of the catalyst. Here, we present a catalyst:ionomer bulk heterojunction (CIBH) architecture that decouples gas, ion, and electron transport. The CIBH comprises a metal and a superfine ionomer layer with hydrophobic and hydrophilic functionalities that extend gas and ion transport from tens of nanometers to the micrometer scale. By applying this design strategy, we achieved CO 2 electroreduction on copper in 7 M potassium hydroxide electrolyte (pH ≈ 15) with an ethylene partial current density of 1.3 amperes per square centimeter at 45% cathodic energy efficiency.
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                Author and article information

                Contributors
                Journal
                Applied Catalysis B: Environmental
                Applied Catalysis B: Environmental
                Elsevier BV
                09263373
                December 2021
                December 2021
                : 298
                : 120538
                Article
                10.1016/j.apcatb.2021.120538
                ae5312fa-3059-4e99-bf79-d847f3715348
                © 2021

                https://www.elsevier.com/tdm/userlicense/1.0/

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