Gold Nanoparticles on Polymer-Wrapped Carbon Nanotubes: An Efficient and Selective Catalyst for the Electroreduction of CO2.

Multiple approaches will be needed to reduce the atmospheric CO2 levels, which have been linked to the undesirable effects of global climate change. The electroreduction of CO2 driven by renewable energy is one approach to reduce CO2 emissions while producing chemical building blocks, but current electrocatalysts exhibit low activity and selectivity. Here, we report the structural and electrochemical characterization of a promising catalyst for the electroreduction of CO2 to CO: Au nanoparticles supported on polymer-wrapped multiwall carbon nanotubes. This catalyst exhibits high selectivity for CO over H2 : 80-92 % CO, as well as high activity: partial current density for CO as high as 160 mA cm-2 . The observed high activity, originating from a high electrochemically active surface area (23 m2 g-1 Au), in combination with the low loading (0.17 mg cm-2 ) of the highly dispersed Au nanoparticles underscores the promise of this catalyst for efficient electroreduction of CO2 .

Aqueous transfer of colloidal metal oxide nanocrystals via base-driven ligand exchange.

A general method is developed for removal of native nonpolar oleate ligands from colloidal metal oxide nanocrystals of varying morphologies and compositions. Ligand stripping occurs by phase transfer into potassium hydroxide solution, yielding stable aqueous dispersions with little nanocrystal aggregation and without significant changes to the nanomaterials' physical or chemical properties. This method enables facile fabrication of conductive films of ligand-free nanocrystals.

A carbon-supported copper complex of 3,5-diamino-1,2,4-triazole as a cathode catalyst for alkaline fuel cell applications.

The performance of a novel carbon-supported copper complex of 3,5-diamino-1,2,4-triazole (Cu-tri/C) is investigated as a cathode material using an alkaline microfluidic H(2)/O(2) fuel cell. The absolute Cu-tri/C cathode performance is comparable to that of a Pt/C cathode. Furthermore, at a commercially relevant potential, the measured mass activity of an unoptimized Cu-tri/C-based cathode was significantly greater than that of similar Pt/C- and Ag/C-based cathodes. Accelerated cathode durability studies suggested multiple degradation regimes at various time scales. Further enhancements in performance and durability may be realized by optimizing catalyst and electrode preparation procedures.

A Nitrogen-Doped Carbon Catalyst for Electrochemical CO2 Conversion to CO with High Selectivity and Current Density.

We report characterization of a non-precious metal-free catalyst for the electrochemical reduction of CO2 to CO; namely, a pyrolyzed carbon nitride and multiwall carbon nanotube composite. This catalyst exhibits a high selectivity for production of CO over H2 (approximately 98 % CO and 2 % H2 ), as well as high activity in an electrochemical flow cell. The CO partial current density at intermediate cathode potentials (V=-1.46 V vs. Ag/AgCl) is up to 3.5× higher than state-of-the-art Ag nanoparticle-based catalysts, and the maximum current density is 90 mA cm-2 . The mass activity and energy efficiency (up to 48 %) were also higher than the Ag nanoparticle reference. Moving away from precious metal catalysts without sacrificing activity or selectivity may significantly enhance the prospects of electrochemical CO2 reduction as an approach to reduce atmospheric CO2 emissions or as a method for load-leveling in relation to the use of intermittent renewable energy sources.

A Gross-Margin Model for Defining Technoeconomic Benchmarks in the Electroreduction of CO2.

We introduce a gross-margin model to evaluate the technoeconomic feasibility of producing different C1 -C2 chemicals such as carbon monoxide, formic acid, methanol, methane, ethanol, and ethylene through the electroreduction of CO2 . Key performance benchmarks including the maximum operating cell potential (Vmax ), minimum operating current density (jmin ), Faradaic efficiency (FE), and catalyst durability (tcatdur ) are derived. The Vmax values obtained for the different chemicals indicate that CO and HCOOH are the most economically viable products. Selectivity requirements suggest that the coproduction of an economically less feasible chemical (CH3 OH, CH4 , C2 H5 OH, C2 H4 ) with a more feasible chemical (CO, HCOOH) can be a strategy to offset the Vmax requirements for individual products. Other performance requirements such as jmin and tcatdur are also derived, and the feasibility of alternative process designs and operating conditions are evaluated.