Defect-rich and ultrathin N doped carbon nanosheets exhibited low overpotentials and robust stability for simultaneous ORR, OER and HER.

Electrochemical CO 2 reduction is a promising way to mitigate CO 2 emissions and close the anthropogenic carbon cycle. Among products from CO 2 RR, multicarbon chemicals, such as ethylene and ethanol with high energy density, are more valuable. However, the selectivity and reaction rate of C 2 production are unsatisfactory due to the sluggish thermodynamics and kinetics of C−C coupling. The electric field and thermal field have been studied and utilized to promote catalytic reactions, as they can regulate the thermodynamic and kinetic barriers of reactions. Either raising the potential or heating the electrolyte can enhance C−C coupling, but these come at the cost of increasing side reactions, such as the hydrogen evolution reaction. Here, we present a generic strategy to enhance the local electric field and temperature simultaneously and dramatically improve the electric−thermal synergy desired in electrocatalysis. A conformal coating of ∼5 nm of polytetrafluoroethylene significantly improves the catalytic ability of copper nanoneedles (∼7-fold electric field and ∼40 K temperature enhancement at the tips compared with bare copper nanoneedles experimentally), resulting in an improved C 2 Faradaic efficiency of over 86% at a partial current density of more than 250 mA cm −2 and a record-high C 2 turnover frequency of 11.5 ± 0.3 s −1 Cu site −1 . Combined with its low cost and scalability, the electric−thermal strategy for a state-of-the-art catalyst not only offers new insight into improving activity and selectivity of value-added C 2 products as we demonstrated but also inspires advances in efficiency and/or selectivity of other valuable electro-/photocatalysis such as hydrogen evolution, nitrogen reduction, and hydrogen peroxide electrosynthesis.

Atomically dispersed FeN 4 catalysts have been considered as potential materials to replace Pt-based catalysts for the oxygen reduction reaction (ORR), but they often suffer from sluggish O 2 activation kinetics due to the symmetrical charge distribution. Herein, we introduce external N, including pyrrolic-N (PN) and graphitic-N (GN), as an electron acceptor near FeN 4 to regulate its charge distribution and improve its ORR activity. Theoretical calculations reveal that introduction of PN evokes much enhanced electron redistribution and local electrical field on the Fe site compared with those observed with GN introduction and the pristine one. Synchrotron X-ray absorption spectroscopy and X-ray photoelectron spectroscopy validate the positive charge accumulation of Fe in the FeN 4 site induced by introducing PN. Thus, the obtained FeN 4 -PN exhibits a great performance for ORR in 0.1 M KOH with a remarkable half-wave potential of 0.91 V versus reversible hydrogen electrode, as well as a Tafel slope of 58 mV decade −1 . This work provides a guide to improve the catalytic performances of single-atom catalysts by introducing chargeredistribution sites.

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A steady sulfur cathode is central to realizing stable room temperature sodium–sulfur (RT Na–S) batteries.