Single atomic copper doping in ultrathin nitrogenated carbon nanosheets over 20.9 wt% was achieved, greatly boosting the oxygen reduction catalysis.

Developing efficient and stable electrocatalysts is crucial for the electrochemical production of pure and clean hydrogen. For practical applications, an economical and facile method of producing catalysts for the hydrogen evolution reaction (HER) is essential. Here, we report ruthenium (Ru) nanoparticles uniformly deposited on multi-walled carbon nanotubes (MWCNTs) as an efficient HER catalyst. The catalyst exhibits the small overpotentials of 13 and 17 mV at a current density of 10 mA cm-2 in 0.5 M aq. H 2 SO 4 and 1.0 M aq. KOH, respectively, surpassing the commercial Pt/C (16 mV and 33 mV). Moreover, the catalyst has excellent stability in both media, showing almost "zeroloss" during cycling. In a real device, the catalyst produces 15.4% more hydrogen per power consumed, and shows a higher Faradaic efficiency (92.28%) than the benchmark Pt/C (85.97%). Density functional theory calculations suggest that Ru-C bonding is the most plausible active site for the HER.

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There have been extensive efforts to synthesize crystalline covalent triazine-based frameworks (CTFs) for practical applications and to realize their potential. The phosphorus pentoxide (P O )-catalyzed direct condensation of aromatic amide instead of aromatic nitrile to form triazine rings. P O -catalyzed condensation was applied on terephthalamide to construct a covalent triazine-based framework (pCTF-1). This approach yielded highly crystalline pCTF-1 with high specific surface area (2034.1 m g ). At low pressure, the pCTF-1 showed high CO (21.9 wt % at 273 K) and H (1.75 wt % at 77 K) uptake capacities. The direct formation of a triazine-based COF was also confirmed by model reactions, with the P O -catalyzed condensation reaction of both benzamide and benzonitrile to form 1,3,5-triphenyl-2,4,6-triazine in high yield.

Catalysts are at the heart of the hydrogen evolution reaction (HER) for the production of pure and clean hydrogen. For practical applications, the scalable synthesis of efficient HER catalysts, which work in both acidic and alkaline media, is highly desired. In this work, the mechanochemically assisted synthesis of a Ru catalyst with HER performance surpassing Pt in both acidic and alkaline media is reported. Mass production of this Ru catalyst can be achieved via a two-step procedure: the mechanochemical reaction between graphite and dry ice produces edge-carboxylic-acid-functionalized graphene nanoplatelets (CGnP); mixing a Ru precursor and the CGnP in an aqueous medium introduces Ru ions, which coordinate on the CGnP. Subsequent annealing results in uniform Ru nanoparticles (≈2 nm) anchored on the GnP matrix (Ru@GnP). The efficient Ru@GnP catalyst can be easily powered by a single silicon solar cell using a wireless integration device. The self-powered device exhibits robust hydrogen evolution under the irradiation of standard AM 1.5 solar light. This work provides a new opportunity for the low-cost mass production of efficient and stable catalysts for practical applications.

Hydrogen adsorption/desorption behavior plays a key role in hydrogen evolution reaction (HER) catalysis. The HER reaction rate is a trade-off between hydrogen adsorption and desorption on the catalyst surface. Herein, we report the rational balancing of hydrogen adsorption/desorption by orbital modulation using introduced environmental electronegative carbon/nitrogen (C/N) atoms. Theoretical calculations reveal that the empty d orbitals of iridium (Ir) sites can be reduced by interactions between the environmental electronegative C/N and Ir atoms. This balances the hydrogen adsorption/desorption around the Ir sites, accelerating the related HER process. Remarkably, by anchoring a small amount of Ir nanoparticles (7.16 wt%) in nitrogenated carbon matrixes, the resulting catalyst exhibits significantly enhanced HER performance. This includs the smallest reported overpotential at 10 mA cm −2 (4.5 mV), the highest mass activity at 10 mV (1.12 A mg Ir −1 ) and turnover frequency at 25 mV (4.21 H 2 s −1 ) by far, outperforming Ir nanoparticles and commercial Pt/C.

Efficiently converting unstable linkages into stable linkages is an important objective in the chemistry of covalent organic frameworks (COFs), because it enhances stability and preserves crystallinity. Here, an unstable imine-linked COF was converted into a stable aromatic benzoxazole-linked COF (BO-COF) via post-oxidative cyclization, based on chemistry used to form fused-aromatic ladder-like rigid-rod polymers. The structure of the porous BO-COF was confirmed by transmission electron microscopy, infrared and solid-state nuclear magnetic resonance spectroscopies, powder X-ray diffraction patterns, and nitrogen adsorption–desorption isotherms. The efficient post-treatment of an unstable reversible COF converted it into a stable irreversible COF, which had significantly improved thermal and chemical stabilities as well as high crystallinity. This strategy can be universally applied for the synthesis of stable fused-aromatic COFs, expanding their practical applications.

Developing efficient and durable electrocatalysts is key to optimizing the electrocatalytic hydrogen evolution reaction (HER), currently one of the cleanest and most sustainable routes for producing hydrogen. Here, a unique and efficient approach to fabricate and embed uniformly dispersed Ir nanoparticles in a 3D cage‐like organic network (CON) structure is reported. These uniformly trapped Ir nanoparticles within the 3D CON (Ir@CON) effectively catalyze the HER process. The Ir@CON electrocatalyst exhibits high turnover frequencies of 0.66 and 0.20 H2 s−1 at 25 mV and small overpotentials of 13.6 and 13.5 mV while generating a current density of 10 mA cm−2 in 0.5 m H2SO4 and 1.0 m KOH aqueous solutions, respectively, as compared to commercial Pt/C (18 and 23 mV) and Ir/C (20.7 and 28.3 mV). More importantly, the catalyst shows superior stability in both acidic and alkaline media. These results highlight a potentially powerful approach for the design and synthesis of efficient and durable electrocatalysts for HER.