Electrocatalytic or photocatalytic N2 reduction holds great promise for green and sustainable NH3 production under ambient conditions, where an efficient catalyst plays a crucial role but remains a long‐standing challenge. Here, a high‐throughput screening of catalysts for N2 reduction among (nitrogen‐doped) graphene‐supported single atom catalysts is performed based on a general two‐step strategy. 10 promising candidates with excellent performance are extracted from 540 systems. Most strikingly, a single W atom embedded in graphene with three C atom coordination (W1C3) exhibits the best performance with an extremely low onset potential of 0.25 V. This study not only provides a series of promising catalysts for N2 fixation, but also paves a new way for the rational design of catalysts for N2 fixation under ambient conditions.

Monolayer C2N supported heteronuclear dual-atom catalysts are designed for efficient CO2 electrochemical reduction.

Oxygen reduction reaction towards hydrogen peroxide (H2O2) provides a green alternative route for H2O2 production, but it lacks efficient catalysts to achieve high selectivity and activity simultaneously under industrial-relevant production rates. Here we report a boron-doped carbon (B-C) catalyst which can overcome this activity-selectivity dilemma. Compared to the state-of-the-art oxidized carbon catalyst, B-C catalyst presents enhanced activity (saving more than 210 mV overpotential) under industrial-relevant currents (up to 300 mA cm−2) while maintaining high H2O2 selectivity (85–90%). Density-functional theory calculations reveal that the boron dopant site is responsible for high H2O2 activity and selectivity due to low thermodynamic and kinetic barriers. Employed in our porous solid electrolyte reactor, the B-C catalyst demonstrates a direct and continuous generation of pure H2O2 solutions with high selectivity (up to 95%) and high H2O2 partial currents (up to ~400 mA cm−2), illustrating the catalyst’s great potential for practical applications in the future.

The photo-/electrocatalytic nitrogen reduction reaction (NRR) is an up and coming method for sustainable NH 3 production; however, its practical application is impeded by poor Faradaic efficiency originating from the competing hydrogen evolution reaction (HER) and the inert N≡N triple bond activation. In this work, we put forth a method to boost NRR through construction of donor–acceptor couples of dual-metal sites. The synergistic effect of dual active sites can potentially break the metal-based activity benchmark toward efficient NRR. By systematically evaluating the stability, activity, and selectivity of 28 heteronuclear dual-atom catalysts (DACs) of M1M2/g-C 3 N 4 candidates, FeMo/g-C 3 N 4 is screened out as an effective electrocatalyst for NRR with a particularly low limiting potential of −0.23 V for NRR and a rather high potential of −0.79 V for HER. Meanwhile, TiMo/g-C 3 N 4 , NiMo/g-C 3 N 4 , and MoW/g-C 3 N 4 with suitable band edge positions and visible light absorption can be applied to NRR as photocatalysts. The excellent catalytic activity is attributed to the tunable composition of metal dimers, which play an important role in modulating the binding strength of the target intermediates. This work may pave a new way for the rational design of heteronuclear DACs with high activity and stability for NRR, which may also apply to other reactions.

Ammonia (NH 3 ) is one of the most important industrial chemicals owing to its wide applications in various fields. However, the synthesis of NH 3 at ambient conditions remains a coveted goal for chemists. In this work, we study the potential of the newly synthesized single-atom catalysts, i.e., single metal atoms (Cu, Pd, Pt, and Mo) supported on N-doped carbon for N 2 reduction reaction (NRR) by employing first-principles calculations. It is found that Mo 1 -N 1 C 2 can catalyze NRR through the enzymatic mechanism with an ultralow overpotential of 0.24 V. Most importantly, the removal of the produced NH 3 is rapid with a free-energy uphill of only 0.47 eV for the Mo 1 -N 1 C 2 catalyst, which is much lower than that for everreported catalysts with low overpotentials and endows Mo 1 -N 1 C 2 with excellent durability. The coordination effect on activity is further evaluated, showing that the experimentally realized active site, single Mo atom coordinated by one N atom and two C atoms (Mo-N 1 C 2 ), possesses the highest catalytic performance. Our study offers new opportunities for advancing electrochemical conversion of N 2 into NH 3 at ambient conditions.