Large scale synthesis of high-efficiency bifunctional electrocatalyst based on cost-effective and earth-abundant transition metal for overall water splitting in the alkaline environment is indispensable for renewable energy conversion. In this regard, meticulous design of active sites and probing their catalytic mechanism on both cathode and anode with different reaction environment at molecular-scale are vitally necessary. Herein, a coordination environment inheriting strategy is presented for designing low-coordination Ni2+ octahedra (L-Ni-8) atomic interface at a high concentration (4.6 at.%). Advanced spectroscopic techniques and theoretical calculations reveal that the self-matching electron delocalization and localization state at L-Ni-8 atomic interface enable an ideal reaction environment at both cathode and anode. To improve the efficiency of using the self-modification reaction environment at L-Ni-8, all of the structural features, including high atom economy, mass transfer, and electron transfer, are integrated together from atomic-scale to macro-scale. At high current density of 500 mA/cm2, the samples synthesized at gram-scale can deliver low hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) overpotentials of 262 and 348 mV, respectively.
Lower charge overpotential of sodium–oxygen (Na–O2) batteries makes them a promising electrical storage technology. However, they have an undesirable discharge product, sodium carbonate (Na2CO3), which has widely been found in many previous studies. Whether and how the carbon components in the cathode are involved in the formation of Na2CO3 is still not well understood. Herein, an all solid-state Na–O2 battery was constructed and its charge and discharge cycles were studied using ambient pressure X-ray photoelectron spectroscopy. The operando XPS results clearly demonstrate the formation of Na2CO3 on the cathode during the discharge cycle. A fraction of the carbonate formed can be cycled while charging the battery. Transformation of the carbon-based cathode to Na2CO3 is a potential cause of capacity fading of the Na–O2 battery. 相似文献