Preparation and catalytic properties of honeycomb catalyst for hydrogen isotope oxidation

Wu, Quanwen; Zheng, Zhenhua; Huang, Zhiyong; Luo, Wenhua

doi:10.1016/j.fusengdes.2015.01.013

Cited by 9 publications

(5 citation statements)

References 19 publications

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“…The properties of the catalyst significantly affect the hydrogen isotope enrichment and removal in the catalytic oxidation . Precious metals (Pt and Pd) and some metal oxides, metal complexes such as copper, silver, rhenium, and hopcalite, have been reported to be efficient catalysts for the oxidation of hydrogen isotopes. − Among them, the precious metals are capable of catalyzing the oxidation reaction at lower temperatures, even at room temperature, which has attracted intense research interest in the past decades . However, the aggregation of Pt during high-temperature annealing, deactivation effect of water vapor on Pt active sites, and deuterium/tritium isotope effect caused low and unsustainable catalytic activity in long-running operation …”

Section: Introductionmentioning

confidence: 99%

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

Zhang

Wang

et al. 2022

ACS Appl. Mater. Interfaces

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A booming demand for energy highlights the importance of an emergency cleanup system in the nuclear industry or hydrogen-energy sector to reduce the risk of hydrogen explosion and decrease tritium emission. The properties of the catalyst determine the efficiency of hydrogen isotope enrichment and removal in the emergency cleanup system. However, the aggregation behavior of Pt, deactivation effect of water vapor, and isotope effect induce a continuous decrease in the catalytic activity of the Pt catalyst. Herein, a de novo design of a Pt nanocatalyst is proposed for catalytic oxidation of the hydrogen isotope via modification of a conjugated microporous polymer onto honeycomb cordierite as a Pt support. The conjugated microporous polymer creates a microporous and hydrophobic environment to attenuate the deactivation effect of water vapor and shape Pt nanoparticles with a diameter of around 2.4 nm. Thus, the as-prepared catalysts exhibit excellent catalytic performance in the range of 25−65 °C and high space velocity (≤30 000 h −1 ) and a stable and high catalytic activity during 487 h of continuous and intermittent operation. Importantly, the charge of the Pt nanoparticles is redistributed by the conjugated skeletons, leading to a decreased energy barrier in the rate-limiting step of hydrogen isotope oxidation and a reduced isotope effect.

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Section: Introductionmentioning

confidence: 99%

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

Zhang

Wang

et al. 2022

ACS Appl. Mater. Interfaces

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“…Precious metals and some metal oxides − have been applied in hydrogen isotope oxidation reactions. Among them, platinum-loaded catalysts have attracted intense attention in recent decades due to their low working temperature and deep removal. ,, Sandeep et al prepared a Pt-loaded stainless steel Dixon ring as a catalyst to reduce the concentration of hydrogen isotopes in pressurized heavy water reactors . The catalyst can reduce the concentration of deuterium in the mixing vessel at 35 °C.…”

Section: Introductionmentioning

confidence: 99%

“…The catalyst can reduce the concentration of deuterium in the mixing vessel at 35 °C. Wu et al developed a Pt/Al 2 O 3 –HC catalyst through loading Pt on honeycomb substrates coated with γ-Al 2 O 3 for the catalytic oxidation of hydrogen . Pt/Al 2 O 3 –HC showed good catalytic performance for H 2 oxidation at room temperature and high space velocity.…”

Section: Introductionmentioning

confidence: 99%

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

Chen

Wang

et al. 2023

ACS Appl. Nano Mater.

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Catalytic oxidation is frequently employed to remove hydrogen isotopes to diminish the risk from tritium leakage and hydrogen explosion. However, Pt particle aggregation and deactivation from water are the major challenges for traditional catalysts. Herein, we design hydrophobic anchoring sites to bind Pt nanoparticles through constructing covalent triazine frameworks on cordierite for the efficient oxidation of hydrogen isotopes. The Pt nanoparticles were uniformly dispersed with a diameter of 1.8–2.4 nm on the catalyst. The catalyst has a high catalytic activity for H2/D2 oxidation at 25–65 °C and high space velocity (≤30,000 h–1). It retains stable catalytic activity in 246 h continuous and intermittent operations and exhibits a lower isotope effect (K F,H/K F,D = 1:0.7) than most of the reported Pt catalysts, indicating good catalytic activity for tritium oxidation. This work provides a Pt-anchoring nanocatalyst with high hydrophobicity for the oxidation of hydrogen isotopes, which can be an effective strategy for designing catalysts.

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“…Honeycomb substrate can dramatically reduce the pressure drop and enhance gas handling capacity. 31,32 The silica nanoparticles can modulate the surface roughness of the carrier to enhance the surface area and hydrophobicity of the substrate. 33,34 The modification of PTS and FAS-17 can decrease the surface free energy and endow the substrate with good amphiphobicity and irradiation resistance.…”

Section: ■ Introductionmentioning

confidence: 99%

“…Then, phenyltriethoxysilane (PTS) and 1 H ,1 H ,2 H ,2 H -perfluorodecyltriethoxysilane (FAS-17) were modified on the honeycomb cordierite (Scheme ). Honeycomb substrate can dramatically reduce the pressure drop and enhance gas handling capacity. , The silica nanoparticles can modulate the surface roughness of the carrier to enhance the surface area and hydrophobicity of the substrate. , The modification of PTS and FAS-17 can decrease the surface free energy and endow the substrate with good amphiphobicity and irradiation resistance. ,, The physicochemical characteristics and catalytic performance of the catalyst were investigated systematically. This work is a pioneering example of creating an amphiphobic environment for the catalytic oxidation of hydrogen isotopes by surface microstructure modulation and is also a solution for the simultaneous attenuation of the inactivation effect of water and VOCs.…”

Section: Introductionmentioning

confidence: 99%

Surface Microstructure Modulation Strategy to Design an Amphiphobic Platinum Nanocatalyst for Efficient Catalytic Oxidation of Hydrogen Isotopes

Chen

Zhou

et al. 2022

ACS Sustainable Chem. Eng.

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Security risks of hydrogen isotopes in hydrogen energy sections and nuclear projects require systems to remove hydrogen isotopes. The oxidation of hydrogen isotopes in a system depends on the efficiency of the catalyst. However, the performance of the catalyst is often reduced by water and volatile organic compounds (VOCs) present in the air. In this study, a surface microstructure modulation strategy is adopted to prepare honeycomb Pt catalysts with an amphiphobic surface (Pt@CDM) for the efficient oxidation of hydrogen isotopes. The surface microstructure of the honeycomb carrier is modulated by surface roughening and postfluorination. The optimized substrate shows a water contact angle of 138.9°and a contact angle of 125.4°with n-hexadecane. Pt@CDM exhibits a much higher H 2 /D 2 conversion than commercial catalysts in a wet environment with VOCs. Additionally, Pt@CDM can retain a catalytic efficiency of more than 95% after 83.5 h of continuous working and intermittent operation. The isotope effect on the oxidation of H 2 and D 2 (K F,H2 /K F,D2 ) is 1:0.88, which is much lower than that of most of the other catalysts and indicates the good catalytic performance of tritium oxidation. This work demonstrates a surface microstructure modulation technology to improve catalytic performance and will also be a strategy for designing efficient catalysts in a practical environment.

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Preparation and catalytic properties of honeycomb catalyst for hydrogen isotope oxidation

Cited by 9 publications

References 19 publications

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

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

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

Surface Microstructure Modulation Strategy to Design an Amphiphobic Platinum Nanocatalyst for Efficient Catalytic Oxidation of Hydrogen Isotopes

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