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Electrocatalytic nitrogen reduction (eNRR) offers a green pathway for NH3 production from N2 and H2O under ambient conditions. Transition metal oxynitrides (TMOxNy) are among the most promising catalysts but face challenges in achieving high yield and faradaic efficiency (FE). This work develops a hybrid WOxNy/WO3 catalyst with a unique heterogeneous interfacial complexion (HIC) structure. This design enables in situ generation and delivery of highly active hydrogen atoms (H*) in acidic electrolytes, promoting nitrogen hydrogenation and formation of nitrogen vacancies (Nv) on the WOxNy surface. This significantly enhances the selectivity of eNRR for NH3 synthesis while suppressing hydrogen evolution reaction (HER). A simple two-step fabrication process—microwave hydrothermal growth followed by plasma-assisted surface nitridation—was developed to fabricate the designed catalyst electrode, achieving an NH3 yield of 3.2 × 10-10 mol·cm-2·s-1 with 40.1% FE, outperforming most TMN/TMOxNy electrocatalysts. Multiple control experiments confirm that the eNRR follows a HIC-enhanced Mars-van Krevelen (MvK) mechanism. 

Abstract Ultralong afterglow emissions due to room‐temperature phosphorescence (RTP) are of paramount importance in the advancement of smart sensors, bioimaging and light‐emitting devices. We herein present an efficient approach to achieve rarely accessible phosphorescence of heavy atom‐free organoboranes via photochemical switching of sterically tunable fluorescent Lewis pairs (LPs). LPs are widely applied in and well‐known for their outstanding performance in catalysis and supramolecular soft materials but have not thus far been exploited to develop photo‐responsive RTP materials. The intramolecular LPM1BNMnot only shows a dynamic response to thermal treatment due to reversible N→B coordination but crystals ofM1BNMalso undergo rapid photochromic switching. As a result, unusual emission switching from short‐lived fluorescence to long‐lived phosphorescence (rad‐M1BNM,τ_RTP=232 ms) is observed. The reported discoveries in the field of Lewis pairs chemistry offer important insights into their structural dynamics, while also pointing to new opportunities for photoactive materials with implications for fast responsive detectors.