Nitrogen fixation under ambient conditions remains a significant challenge. Here, we report nitrogen fixation by Ru single-atom electrocatalytic reduction at room temperature and pressure. In contrast to Ru nanoparticles, single Ru sites supported on N-doped porous carbon greatly promoted electroreduction of aqueous N 2 selectively to NH 3 , affording an NH 3 formation rate of 3.665 mg NH 3 h À1 mg À1Ru at À0.21 V versus the reversible hydrogen electrode. Importantly, the addition of ZrO 2 was found to significantly suppress the competitive hydrogen evolution reaction. An NH 3 faradic efficiency of about 21% was achieved at a low overpotential (0.17 V), surpassing many other reported catalysts. Experiments combined with density functional theory calculations showed that the Ru sites with oxygen vacancies were major active centers that permitted stabilization of *NNH, destabilization of *H, and enhanced N 2 adsorption. We envision that optimization of ZrO 2 loading could further facilitate electroreduction of N 2 at both high NH 3 synthesis rate and faradic efficiency.
Tackling the huge volume expansion of silicon (Si) anode desires a stable solid electrolyte interphase (SEI) to prohibit the interfacial side reactions. Here, a layered conductive polyaniline (LCP) coating is built on Si nanoparticles to achieve high areal capacity and long lifespan. The conformal LCP coating stores electrolyte in interlamination spaces and directs an in situ formation of LCP‐integrated hybrid SEI skin with uniform distribution of organic and inorganic components, enhancing the flexibility of the SEI to buffer the volume changes and maintaining homogeneous ion transport during cycling. As a result, the Si anode shows a remarkable cycling stability under high areal capacity (≈3 mAh cm−2) after 150 cycles and good rate performance of 942 mAh g−1 at 5 A g−1. This work demonstrates the great potential of regulating the SEI properties by a layered polymer‐directing SEI formation for the mechanical and electrochemical stabilization of Si anodes.
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