Atomically dispersed transition metal active sites have emerged as one of the most important fields of study because they display promising performance in catalysis and have the potential to serve as ideal models for fundamental understanding. However, both the preparation and determination of such active sites remain a challenge. The structural engineering of carbon-and nitrogencoordinated metal sites (M−N−C, M = Fe, Co, Ni, Mn, Cu, etc.) via employing new heteroatoms, e.g., P and S, remains challenging. In this study, carbon nanosheets embedded with nitrogen and phosphorus dual-coordinated iron active sites (denoted as Fe-N/P-C) were developed and determined using cutting edge techniques. Both experimental and theoretical results suggested that the N and P dual-coordinated iron sites were favorable for oxygen intermediate adsorption/desorption, resulting in accelerated reaction kinetics and promising catalytic oxygen reduction activity. This work not only provides efficient way to prepare well-defined single-atom active sites to boost catalytic performance but also paves the way to identify the dual-coordinated single metal atom sites.
Hydrogen evolution reaction (HER) on earth-abundant molybdenum disulfide (MoS 2) in acidic media is a robust process, but is kinetically retarded in alkaline media. Thus, improving the sluggish kinetics for HER in alkaline media is crucial for advancing the performance of water-alkali electrolyzers. Here, we demonstrate a dramatic enhancement of HER kinetics in base by judiciously hybridizing vertical MoS 2 sheets with another earth-abundant material, layered double hydroxide (LDH). The resultant MoS 2 /NiCo-LDH hybrid exhibits an extremely low HER overpotential of 78 mV at 10 mA/cm 2 and a low Tafel slope of 76.6 mV/dec in 1 M KOH solution. At the current density of 20 mA/cm 2 or even higher, the MoS 2 /NiCo-LDH composite can operate without degradation for 48 hr. This work not only brought forth a cost-effective and robust electrocatalyst, but more generally opened up new vistas for developing high-performance electrocatalysts in unfavorable media recalcitrant to conventional catalyst design.
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