Electrocatalytically Activating and Reducing N Molecule by Tuning Activity of Local Hydrogen Radical.

Decarbonizing N conversion is particularly challenging, but essential for sustainable development of industry and agriculture. Herein, we achieve electrocatalytic activation/reduction of N on X/Fe-N-C (X=Pd, Ir and Pt) dual-atom catalysts under ambient condition. We provide solid experimental evidence that local hydrogen radical (H*) generated on the X site of the X/Fe-N-C catalysts can participate in the activation/reduction of N adsorbed on the Fe site.

Tuning Fe Spin Moment in Fe-N-C Catalysts to Climb the Activity Volcano via a Local Geometric Distortion Strategy.

As the most promising alternative to platinum-based catalysts for cathodic oxygen reduction reaction (ORR) in proton exchange membrane fuel cells, further performance enhancement of Fe-N-C catalysts is highly expected to promote their wide application. In Fe-N-C catalysts, the single Fe atom forms a square-planar configuration with four adjacent N atoms (D symmetry). Breaking the D symmetry of the FeN active center provides a new route to boost the activity of Fe-N-C catalysts.

Two dimensional electrocatalyst engineering via heteroatom doping for electrocatalytic nitrogen reduction.

The electrocatalytic N reduction reaction (eNRR) - which can occur under ambient conditions with renewable energy input - became a promising synthetic pathway for ammonia (NH) and has attracted growing attention in the past few years. Some achievements have been made in the eNRR; however, there remain significant challenges to realize satisfactory NH production. Therefore, the rational design of highly efficient and durable eNRR catalysts with N[triple bond, length as m-dash]N bond activating and breaking ability is highly desirable.

The Crucial Role of Charge Accumulation and Spin Polarization in Activating Carbon-Based Catalysts for Electrocatalytic Nitrogen Reduction.

Cost-effective carbon-based catalysts are promising for catalyzing the electrochemical N reduction reaction (NRR). However, the activity origin of carbon-based catalysts towards NRR remains unclear, and regularities and rules for the rational design of carbon-based NRR electrocatalysts are still lacking. Based on a combination of theoretical calculations and experimental observations, chalcogen/oxygen group element (O, S, Se, Te) doped carbon materials were systematically evaluated as potential NRR catalysts.