Developing efficient and stable oxygen evolution reaction (OER) electrocatalysts that can work stably in acidic conditions is crucial for advancing proton-exchange membrane water electrolysers commercialization. Here, we prepared a heterostructure-based OER electrocatalyst by in-situ growing RuO2 nanoparticles on metal-organic-framework-derived Co3O4 nanoaggregates that can operate stably in acidic electrolytes. The interface of RuO2/Co3O4 heterostructure, as well as their effect on electronic structure, were examined by various advanced characterizations. The optimized RuO2/Co3O4 electrocatalyst reveals an ultra-low overpotential of 206 and 320 mV at 10 and 100 mA·cm−2, respectively. X-ray photoelectron spectroscopy, differential electrochemical mass spectroscopy measurements and theoretical calculations indicate that the as-constructed RuO2/Co3O4 interfaces could reduce the metal-oxygen covalence and energy barriers of rate-determining step, thereby decreasing the participation of lattice oxygen and preventing excessive oxidation of Ru sites during OER. In practical PEMWE systems, RuO2/Co3O4 achieves 1.63 V at 1 A·cm−2, and maintains remarkable stability for over 500 h with a very small voltage degradation rate of 0.2 mV·h−1. This study provides a promising avenue for developing cost-effective OER electrocatalysts with superior activity and stability for advanced energy conversion.
- Article type
- Year
- Co-author
Open Access
Research Article
Issue
Open Access
Research Article
Just Accepted
Metal halide perovskites (e.g., CsPbBr3) have emerged as highly promising scintillator materials owing to their superior optoelectronic characteristics. However, their practical deployment is constrained by intrinsic structural instability and nonradiative recombination-induced energy loss. Herein, we show that Ni2+ doping constitutes a potent regulatory strategy for synergistically improving the scintillation performance and environmental robustness of CsPbBr3 perovskite. Various characterizations combined with threotecial calculation indicate that the incorporation of Ni2+ dopants triggers lattice contraction, thereby enhancing the resistance to environmental perturbations. Ni-doping also passivates intrinsic defects and traps, leading to marked suppression of nonradiative recombination pathways. This synergy in as-prepared Ni-doped CsPbBr3 leads to an 11-fold enhancement in photoluminescence intensity and a substantial increase in photoluminescence quantum yield from 56.0% to 93.7%. Notably, it delivers an exceptional light yield of 38428.5 photons MeV-1, a low detection limit of 64.9 nGyair s-1, and superior radiation tolerance. Furthermore, a flexible scintillation screen containing Ni-doped CsPbBr3 enables high-resolution X-ray imaging with a spatial resolution of 16.6 lp mm-1, notably surpassing that of the majority of reported perovskite-based scintillators. This study provides profound insights into the pivotal role of metal doping into halide perovskites for enhancing environmental stability in radiation detection technologies.
Open Access
Review Article
Issue
Electrochemical nitrate reduction reaction (NO3RR) emerges as a sustainable approach for converting residual nitrate pollutants into valuable ammonia under ambient conditions, offering a promising alternative to the energy-intensive Haber–Bosch process. Compared to single-metal-site electrocatalysts, dual-metal-site (DMS) electrocatalysts show synergistic effects between adjacent metal sites, effectively regulating the electronic state and enhancing the catalytic activity and selectivity for NO3RR with multi-step proton and electron transfers. Further understanding on NO3RR is of practical significance for design of efficient DMS electrocatalysts. This review aims to systematically investigate the recent advancement of DMS electrocatalysts for NO3RR to ammonia synthesis, providing new understandings and insights into this catalytic process. The NO3RR mechanism, artificial intelligence (AI)-driven DMS synthesis, DMS synthesis/characterization, and design of chemical reaction systems are categorized and discussed. DMS electrocatalysts for NO3RR at the cathode can reduce the energy input for water oxidation, biomass oxidation reactions, and zinc-nitrate batteries, while simultaneously enhancing the yields of anode and cathode products. Finally, the remaining challenges and future perspectives for DMS electrocatalysts in NO3RR are further discussed. This review provides in-depth guidance for rational design of dual-site electrocatalysts, facilitating practical and sustainable electrochemical processes in the near future.
Open Access
Research Article
Issue
Electrocatalytic synthesis of ammonia (NH3) from nitrate (NO3−) is an effective approach for reducing nitrate pollutants in the environment and a promising method for ammonia synthesis under mild conditions. However, current catalyst syntheses are costly, and their application in real wastewater remains underexplored. Herein, we prepared high-efficiency copper-based single-atom-nanoparticle synergistic sites on carbon felt (CuSA/NP@C) from copper-containing wastewater. Trace Cu2+ in wastewater enables efficient nitrate reduction reaction (NO3RR), and the effect of different Cu2+ concentrations was also investigated. The optimized CuSA/NP@C, with synergy between single atoms and nanoparticles, shows excellent activity: a maximum Faradaic efficiency of ~ 100% (at −0.3 V vs. reversible hydrogen electrode (RHE)) and a NH3 yield of ~ 10 mg·cm−2. Theoretical calculations reveal that Cu single-atoms and nanoparticles synergistically act on the NO3* and H* intermediates to promote nitrate hydrogenation to NH3. A membrane electrode assembly with the CuSA/NP@C cathode achieves the NH3 synthesis at an industrial current density of 200 mA·cm−2 for over 90 h. This “treating waste with waste” strategy offers new paths for nitrate wastewater recycling and green NH3 synthesis advancement.
京公网安备11010802044758号