Because of their high theoretical energy density and low cost, lithium–sulfur (Li–S) batteries are promising next-generation energy storage devices. The electrochemical performance of Li–S batteries largely depends on the efficient reversible conversion of Li polysulfides to Li2S in discharge and to elemental S during charging. Here, we report on our discovery that monodisperse cobalt atoms embedded in nitrogen-doped graphene (Co–N/G) can trigger the surface-mediated reaction of Li polysulfides. Using a combination of operando X-ray absorption spectroscopy and first-principles calculation, we reveal that the Co–N–C coordination center serves as a bifunctional electrocatalyst to facilitate both the formation and the decomposition of Li2S in discharge and charge processes, respectively. The S@Co–N/G composite, with a high S mass ratio of 90 wt %, can deliver a gravimetric capacity of 1210 mAh g–1, and it exhibits an areal capacity of 5.1 mAh cm–2 with capacity fading rate of 0.029% per cycle over 100 cycles at 0.2 C at S loading of 6.0 mg cm–2 on the electrode disk.

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Electrochemical reduction of carbon dioxide (CO) to value-added carbon products is a promising approach to reduce CO levels and mitigate the energy crisis. However, poor product selectivity is still a major obstacle to the development of CO reduction. Here we demonstrate exclusive Ni-N sites through a topo-chemical transformation strategy, bringing unprecedentedly high activity and selectivity for CO reduction. Topo-chemical transformation by carbon layer coating successfully ensures preservation of the Ni-N structure to a maximum extent and avoids the agglomeration of Ni atoms to particles, providing abundant active sites for the catalytic reaction. The Ni-N structure exhibits excellent activity for electrochemical reduction of CO with particularly high selectivity, achieving high faradaic efficiency over 90% for CO in the potential range from -0.5 to -0.9 V and gives a maximum faradaic efficiency of 99% at -0.81 V with a current density of 28.6 mA cm. We anticipate exclusive catalytic sites will shed new light on the design of high-efficiency electrocatalysts for CO reduction.