The present study proposes a new approach for direct CO2 conversion using primary radicals from water irradiation. In order to ensure reduction of CO2 into CO2 -• by all the hydrated electrons, we use formate ions to scavenge simultaneously the parent oxidizing radicals H • and OH • producing the same transient CO2 -• radicals. Conditions are optimized to obtain the highest conversion yield of CO2. The goal is achieved under mild conditions of room temperature, neutral pH and 1 atm of CO2 pressure. All the available radicals are exploited for selectively converting CO2 into oxalate that is accompanied by H2 evolution. The mechanism presented accounts for the results and also sheds light on the data in the literature. The radiolytic approach is a mild and scalable route of direct CO2 capture at the source in industry and the products, oxalate salt and H2, can be easily separated.
High-energy radiation that is compatible with renewable energy sources enables direct H 2 production from water for fuels; however, the challenge is to convert it as efficiently as possible, and the existing strategies have limited success. Herein, we report the use of Zr/Hf-based nanoscale UiO-66 metal− organic frameworks as highly effective and stable radiation sensitizers for purified and natural water splitting under γ-ray irradiation. Scavenging and pulse radiolysis experiments with Monte Carlo simulations show that the combination of 3D arrays of ultrasmall metal-oxo clusters and high porosity affords unprecedented effective scattering between secondary electrons and confined water, generating increased precursors of solvated electrons and excited states of water, which are the main species responsible for H 2 production enhancement. The use of a small quantity (<80 mmol/L) of UiO-66-Hf-OH can achieve a γ-rays-to-hydrogen conversion efficiency exceeding 10% that significantly outperforms Zr-/Hf-oxide nanoparticles and the existing radiolytic H 2 promoters. Our work highlights the feasibility and merit of MOF-assisted radiolytic water splitting and promises a competitive method for creating a green H 2 economy.
A deuteron radio-frequency quadrupole (RFQ) is being built by the RFQ group at Peking University. It is a very compact high-current RFQ, operating at 162.5 MHz in continuous-wave mode. By optimizing the beam dynamics design, our simulations reached 98% transmission efficiency for acceleration of the 50-mA deuteron beam from 50 keV to 1 MeV, with an intervane voltage of 60 kV and a length of 1.809 m. This RFQ adopts a window-type structure, with low power consumption and sufficient mode separation, with no stabilizing rods required. Its magnetic coupling windows have been optimized by both electromagnetic simulation and the construction of an equivalent circuit model. The empirical equation based on the circuit model provides a new way to evaluate the effect of the window size on the frequency. In addition, an aluminum model of the full-length RFQ has been built and tested, and the results show good agreement with the simulations. During the tuning process, the magnetic coupling effect between quadrants was found to be unique to the window-type RFQ. We also propose a method to estimate the effects of different degrees of electric field unflatness on the beam transmission. For the cooling system design, the results of thermostructural analysis, verified by comparing results from ANSYS and CST, show that the special cooling channels provide a high cooling efficiency around the magnetic coupling windows. The maximal deformation of the structure was approximately 75 μm. The beam-loading effect caused by a high current, and the coupler design, are also discussed.
The radio-frequency quadrupole (RFQ) group at Peking University has built a window-type RFQ, operating at 162.5 MHz in continuous-wave (cw) mode. It is designed to accelerate a 50 mA deuteron beam from 50 keV to 1 MeV with a vane length of 1.809 m. The cavity was fabricated in two segments using 100% oxygen-free electronic (OFE) copper. Using an iterative assembly and measurement procedure for the precise alignment of the two segments, we reduced the assembly errors to within AE0.05 mm. The radio frequency (rf) measurements of the whole cavity show excellent rf properties, with the measured intrinsic Q-value of 8962, which equates to 96% of the simulated value for OFE copper. We also investigated field fluctuations caused by misalignment between the two segments, and studied their impact on the beam transmission using beam dynamics simulations. During field tuning, we compiled a set of unique tuning rules for the window-type RFQ. After tuning, the maximal field unflatness of the single quadrant is within AE2%, and the asymmetry of the four quadrants is within AE1%. During rf conditioning, the cw power of the cavity reached 55 kW within 32 hours, and we have recorded nearly seven hours of stable running at a cw power of 50 kW. The measured bremsstrahlung spectrum shows that the accelerator needs 49.9 kW to generate the intervane voltage of 60 kV, with a specific shunt impedance of 130.5 kΩ m. An H þ 2 ion beam extracted from an electron cyclotron resonance ion source was used for the beam commissioning, because deuteron beam acceleration will bring a serious radiation field. We achieved stable and robust acceleration of about 1.5 mA cw H þ 2 beam for one hour.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.
hi@scite.ai
10624 S. Eastern Ave., Ste. A-614
Henderson, NV 89052, USA
Copyright © 2024 scite LLC. All rights reserved.
Made with 💙 for researchers
Part of the Research Solutions Family.