Efficient water electrolyzers are constrained by the lack of low-cost and earth-abundant hydrogen evolution reaction (HER) catalysts that can operate at industry-level conditions and be prepared with a facile process. Here we report a self-standing MoC–Mo2C catalytic electrode prepared via a one-step electro-carbiding approach using CO2 as the feedstock. The outstanding HER performances of the MoC–Mo2C electrode with low overpotentials at 500 mA cm−2 in both acidic (256 mV) and alkaline electrolytes (292 mV), long-lasting lifetime of over 2400 h (100 d), and high-temperature performance (70 oC) are due to the self-standing hydrophilic porous surface, intrinsic mechanical strength and self-grown MoC (001)–Mo2C (101) heterojunctions that have a ΔGH* value of −0.13 eV in acidic condition, and the energy barrier of 1.15 eV for water dissociation in alkaline solution. The preparation of a large electrode (3 cm × 11.5 cm) demonstrates the possibility of scaling up this process to prepare various carbide electrodes with rationally designed structures, tunable compositions, and favorable properties.
25 February 2013 in Energy & Environmental Science
A molten salt electrochemical system comprising a eutectic mixture of Li–Na–K carbonates, a Ni cathode, and a SnO2 inert anode is proposed for the capture and electrochemical conversion of CO2. It is demonstrated that CO2 can be effectively captured by molten carbonates, and subsequently electrochemically split into amorphous carbon on the cathode, and oxygen gas at the anode. The carbon materials generated at the cathode exhibit high BET surface areas of more than 400 m2 g−1 and as such, represent value-added products for a variety of applications such as energy storage and pollutant adsorption. In the carbonate eutectic (500 °C), the presence of Li2CO3 is shown to be required for the deposition of carbon from the melt, wherein O2− or Li2O serves as the intermediate for CO2 capture and electrochemical conversion. SnO2 proved to be an effective anode for the electrochemical evolution of oxygen. Electrochemical reactions were found to proceed at relatively high current efficiencies, even though the current densities exceed 50 mA cm−2. The intrinsic nature of alkaline oxides for CO2 capture, the conversion of CO2 to value-added products, and the ability to drive the process with renewable energy sources such as solar power, enables the technology to be engineered for high flux capture and utilization of CO2.