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1.
Phys Chem Chem Phys ; 26(26): 18285-18301, 2024 Jul 03.
Artículo en Inglés | MEDLINE | ID: mdl-38910560

RESUMEN

The electrochemical CO2 reduction reaction (eCO2RR) driven by renewable electricity offers a green and sustainable technology for synthesizing chemicals and managing global carbon balance. However, developing electrocatalysts with high activity and selectivity for producing C1 products (CO, HCOOH, CH3OH, and CH4) remains a daunting task. In this study, we conducted comprehensive first-principles calculations to investigate the eCO2RR mechanism using B-defective BC3-supported transition metal single-atom catalysts (TM@BC3 SACs). Initially, we evaluated the thermodynamic and electrochemical stability of the designed 26 TM@BC3 SACs by calculating the binding energy and dissolution potential of the anchored TM atoms. Subsequently, the selectivity of the eCO2RR and hydrogen evolution reaction (HER) on stable SACs was determined by comparing the free energy change (ΔG) for the first protonation of CO2 with the ΔG of *H formation. The stability and selectivity screening processes enabled us to narrow down the pool of SACs to the 14 promising ones. Finally, volcano plots for the eCO2RR towards different C1 products were established by using the adsorption energy descriptors of key intermediates, and three SACs were predicted to exhibit high activity and selectivity. The limiting potentials (UL) for HCOOH production on Pd@BC3 and Ag@BC3 are -0.11 V and -0.14 V. CH4 is a preferred product on Re@BC3 with UL of -0.22 V. Elaborate electronic structure calculations elucidate that the activity and selectivity originate from the sufficient activation of the C-O bond and the strong orbital hybridization between crucial intermediates and metal atoms. The proposed catalyst screening criteria, constructed volcano plots and predicted SACs may provide a theoretical foundation for the development of computationally guided catalyst designs for electrochemical CO2 conversion to C1 products.

2.
Micromachines (Basel) ; 15(3)2024 Mar 13.
Artículo en Inglés | MEDLINE | ID: mdl-38542635

RESUMEN

This paper introduces the structure and characteristics of an internal-matching high-power Doherty power amplifier based on GaN HEMT devices with 0.25 µm process platforms from the Nanjing Electronic Devices Institute. Through parameter extraction and load-pull testing of the model transistor, an EE_HEMT model for the 1.2 mm gate-width GaN HEMT device was established. This model serves as the foundation for designing a high-power three-stage Doherty power amplifier. The amplifier achieved a saturated power gain exceeding 9 dB in continuous wave mode, with a saturated power output of 49.7 dBm. The drain efficiency was greater than 65% at 2.6 GHz. At 9 dB power back-off point, corresponding to an output power of 40.5 dBm, the drain efficiency remained above 55%. The performance of the amplifier remains consistent within the 2.55-2.62 GHz frequency range. The measured power, efficiency, and gain of the designed Doherty power amplifier align closely with the simulation results based on the EE_HEMT model, validating the accuracy of the established model. Furthermore, the in-band matching design reduces the size and weight of the amplifier. The amplifier maintains normal operation even after high and low-temperature testing, demonstrating its reliability. In conjunction with DPD (digital pre-distortion) for the modulated signal test, the amplifier exhibits extremely high linearity (ACLR < -50.93 dBc). This Doherty power amplifier holds potential applications in modern wireless communication scenarios.

3.
J Colloid Interface Sci ; 666: 66-75, 2024 Jul 15.
Artículo en Inglés | MEDLINE | ID: mdl-38583211

RESUMEN

Perovskite CsPbBr3 quantum dot shows great potential in artificial photosynthesis, attributed to its outstanding optoelectronic properties. Nevertheless, its photocatalytic activity is hindered by insufficient catalytic active sites and severe charge recombination. In this work, a CsPbBr3@Ag-C3N4 ternary heterojunction photocatalyst is designed and synthesized for high-efficiency CO2 reduction. The CsPbBr3 quantum dots and Ag nanoparticles are chemically anchored on the surface of g-C3N4 sheets, forming an electron transfer tunnel from CsPbBr3 quantum dots to Ag nanoparticles via g-C3N4 sheets. The resulting CsPbBr3@Ag-C3N4 ternary photocatalyst, with spatial separation of photogenerated carriers, achieves a remarkable conversion rate of 19.49 µmol·g-1·h-1 with almost 100 % CO selectivity, a 3.13-fold enhancement in photocatalytic activity as compared to CsPbBr3 quantum dots. Density functional theory calculations reveal the rapid CO2 adsorption/activation and the decreased free energy (0.66 eV) of *COOH formation at the interface of Ag nanoparticles and g-C3N4 in contrast to the g-C3N4, leading to the excellent photocatalytic activity, while the thermodynamically favored CO desorption contributes to the high CO selectivity. This work presents an innovative strategy of constructing perovskite-based photocatalyst by modulating catalyst structure and offers profound insights for efficient CO2 conversion.

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