Liquid-Phase Catalytic Exchange of Hydrogen Isotopes over Platinum on Dual-Modified Graphene

Abstract

Although liquid-phase catalytic exchange is an environmentally friendly treatment of hydrogen isotopes in recycled water of a nuclear power station, the successive development of hydrophobic catalysts is still needed to meet much higher catalytic exchange efficiency and stability. Herein, a dual-modified graphene with Pt loading was designed by amination and silanization to anchor Pt nanoparticles uniformly, as well as obtain higher hydrophobicity. After coating the reactor walls with poly­(dimethylsiloxane), the catalytic exchange efficiency of the dual-modified graphene with lower Pt loadings (Pt/200-S-NH2-GR) improved up to 91% at 80 °C, which was higher than 80% of only animated graphene (Pt/NH2-GR) at the same condition. Furthermore, the Pt/200-S-NH2-GR maintained high stability for at least 10 h in the temperature range of 40–80 °C, while the Pt/NH2-GR decreased 17% of catalytic exchange efficiency at 80 °C within 10 h. Using the dual-modified strategy for graphene support, high efficiency and stability was achieved for heavy water dedeuteration.

De Novo Design of a Pt Nanocatalyst on a Conjugated Microporous Polymer-Coated Honeycomb Carrier for Oxidation of Hydrogen Isotopes

“…The valence state of Pt on CMP@Cor was characterized through XPS analysis (Figure S5A), and the results show that the content of metallic Pt is 70.9% on the surface of HisoCat (Table S6). The peaks at 75.7 and 72.3 eV stem from Pt 4f 5/2 and Pt 4f 7/2 of metallic Pt, respectively, which are higher than those of pure Pt (74.4 eV for Pt 4f 5/2 and 71.0 eV for Pt 4f 7/2) . The shift of 1.3 eV to higher binding energy of Pt 4f on HisoCat indicates a strong metal–support interaction between the Pt nanoparticles and the CMP layer. , …”

“…29 The peaks at 75.7 and 72.3 eV stem from Pt 4f 5/2 and Pt 4f 7/2 of metallic Pt, respectively, which are higher than those of pure Pt (74.4 eV for Pt 4f 5/2 and 71.0 eV for Pt 4f 7/2). 30 The shift of 1.3 eV to higher binding energy of Pt 4f on HisoCat indicates a strong metal−support interaction between the Pt nanoparticles and the CMP layer. 31,32 The crystalline form and size of Pt nanoparticles on HisoCat were measured by XRD and high-resolution transmission electron microscopy (HRTEM).…”

Platinum Nanoparticles Anchored on Covalent Triazine Frameworks Modified Cordierite for Efficient Oxidation of Hydrogen Isotopes

“…The Pt (δ+) species accounting for 31.5% of the total platinum probably came from the incomplete reduction of platinum and oxidation by air . Compared with the binding energy of the Pt 4f 5/2 peak (74.4 eV) and Pt 4f 7/2 peak (71.0 eV) on pure Pt, the peaks of Pt(0) 4f 5/2 and Pt(0) 4f 7/2 on HisoNCat were shifted to higher binding energies at 75.3 and 72.0 eV, respectively (Table S3). The Pt 4f peak shifted to a higher binding energy, confirming the interaction of N on the azine ring and Pt. , This interaction can anchor Pt nanoparticles to prevent them from agglomerating and expose more catalytic sites for the reaction gas to enhance the catalytic performance.…”

Liquid‐Phase Catalytic Exchange of Hydrogen Isotopes over Ion Sputtering Platinum on Superhydrophobic Coatings

“…The evaluation of catalyst coatings is done in a cylindrical glass reactor, [12] as shown in Figure 4a. The 50‐Pt/SSNs/PDMS coating is shown in Figure 4b.…”

“…Firstly, due to the existence of support pores and hydrophobic polymer, the utilization of Pt will inevitably decrease. Secondly, the above‐mentioned porous supports cause severe internal diffusion, [9a,12] thus making the stability and efficiency of catalysts decrease. Therefore, eliminating the diffusion in the catalysts and increasing the utilization of Pt remain a challenge for LPCE.…”