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.
MXene-reinforced composite coatings have recently shown promise for metal anticorrosion due to their large aspect ratio and antipermeability; however, the challenges of the poor dispersion, oxidation, and sedimentation of MXene nanofillers in a resin matrix that are often encountered in the existing curing methods have greatly limited practical applications. Herein, we reported an efficient, ambient, and solvent-free electron beam (EB) curing technology to fabricate PDMS@MXene filled acrylatepolyurethane (APU) coatings for anticorrosion of 2024 Al alloy, a common aerospace structural material. We showed that the dispersion of MXene nanoflakes modified by PDMS-OH was dramatically improved in EB-cured resin and enhanced the water resistance through the additional water-repellent groups of PDMS-OH. Moreover, the controllable irradiation-induced polymerization enabled a unique high-density cross-linked network, presenting a large physical barrier against corrosive media. The newly developed APU-PDMS@MX 1 coatings achieved excellent corrosionresistance with the highest protection efficiency of 99.9957%. The coating filled with uniformly distributed PDMS@MXene promoted the corrosion potential, corrosion current density, and corrosion rate to be −0.14 V, 1.49 × 10 −9 A/cm 2 , and 0.0004 mm/ year, respectively, and the impedance modulus was increased by 1−2 orders of magnitude compared to that of APU-PDMS coating. This work combining 2D material with EB curing technology broadens the avenue for designing and fabricating composite coatings for metal corrosion protection.
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