Ambient electrochemical N2 reduction is emerging as a highly promising alternative to the Haber–Bosch process but is typically hampered by a high reaction barrier and competing hydrogen evolution, leading to an extremely low Faradaic efficiency. Here, we demonstrate that under ambient conditions, a single-atom catalyst, iron on nitrogen-doped carbon, could positively shift the ammonia synthesis process to an onset potential of 0.193 V, enabling a dramatically enhanced Faradaic efficiency of 56.55%. The only doublet coupling representing 15NH4+ in an isotopic labeling experiment confirms reliable NH3 production data. Molecular dynamics simulations suggest efficient N2 access to the single-atom iron with only a small energy barrier, which benefits preferential N2 adsorption instead of H adsorption via a strong exothermic process, as further confirmed by first-principle calculations. The released energy helps promote the following process and the reaction bottleneck, which is widely considered to be the first hydrogenation step, is successfully overcome.
Lithium metal, the ideal anode material for rechargeable batteries, suffers from the inherent limitations of sensitivity to the humid atmosphere and dendrite growth. Herein, low-cost fabrication of a metallic-lithium anode that is stable in air and plated dendrite-free from an organic-liquid electrolyte solves four key problems that have plagued the development of large-scale Li-ion batteries for storage of electric power. Replacing the low-capacity carbon anode with a safe, dendrite-free lithium anode provides a fast charge while reducing the cost of fabrication of a lithium battery, and increasing the cycle life of a rechargeable cell by eliminating the liquid-electrolyte ethylene-carbonate additive used to form a solid-electrolyte interphase passivation layer on the anode that is unstable during cycling. This solution is accomplished by formation of a hydrophobic solid-electrolyte interphase on a metallic-lithium anode that allows for handling of the treated lithium anode membrane in a standard dry room during cell fabrication.
An ultrahigh pyridinic N-content-doped porous carbon monolith is reported, and the content of pyridinic N reaches up to 10.1% in overall material (53.4 ± 0.9% out of 18.9 ± 0.4% N content), being higher than most of previously reported N-doping carbonaceous materials, which exhibit greatly improved electrochemical performance for potassium storage, especially in term of the high reversible capacity. Remarkably, the pyridinic N-doped porous carbon monolith (PNCM) electrode exhibits high initial charge capacity of 487 mAh g at a current density of 20 mA g , which is one of the highest reversible capacities among all carbonaceous anodes for K-ion batteries. Moreover, the K-ion full cell is successfully assembled, demonstrating a high practical energy density of 153.5 Wh kg . These results make PNCM promising for practical application in energy storage devices and encourage more investigations on a similar potassium storage system.
The high solubility of long-chain lithium polysulfides and their infamous shuttle effect in lithium sulfur battery lead to rapid capacity fading along with low Coulombic efficiency. To address above issues, we propose a new strategy to suppress the shuttle effect for greatly enhanced lithium sulfur battery performance mainly through the formation of short-chain intermediates during discharging, which allows significant improvements including high capacity retention of 1022 mAh/g with 87% retention for 450 cycles. Without LiNO-containing electrolytes, the excellent Coulombic efficiency of ∼99.5% for more than 500 cycles is obtained, suggesting the greatly suppressed shuttle effect. In situ UV/vis analysis of electrolyte during cycling reveals that the short-chain LiS and LiS polysulfides are detected as main intermediates, which are theoretically verified by density functional theory (DFT) calculations. Our strategy may open up a new avenue for practical application of lithium sulfur battery.
Highly flexible bismuth Hall sensors on polymeric foils are fabricated, and the key optimization steps that are required to boost their sensitivity to the bulk value are identified. The sensor can be bent around the wrist or positioned on the finger to realize an interactive pointing device for wearable electronics. Furthermore, this technology is of great interest for the rapidly developing market of eMobility, for optimization of eMotors and magnetic bearings.
Covalent organic frameworks with abundant active sites are potential metal-free catalysts for the nitrogen reduction reaction. However, the utilization ratio of active sites is restricted in an actual reaction process due to the limited nitrogen transport. Here, we demonstrate that facilitating the N
2
accessibility to boron-rich covalent organic frameworks through electrochemical excitation can achieve highly efficient nitrogen reduction activity. Simulations show that the boron sites are bonded with nitrogenous species under electrochemical condition and the resultant amorphous phase of covalent organic frameworks has much stronger affinity toward N
2
to enhance the molecule collision. Combined with experimental results, the excitation process is confirmed to be a virtuous cycle of more excited sites and stronger N
2
affinity, which continuously proceed until the whole system reaches the optimum reaction status. As expected, the electrochemically excited catalyst delivers significantly enhanced reaction activity, with a high Faradaic efficiency of 45.43%.
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