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Chemical utilization of vast fossil and renewable feedstocks of methane remains one of the most important challenges of modern chemistry. Herein, we report direct and selective methane photocatalytic oxidation at ambient conditions into carbon monoxide, which is an important chemical intermediate and a platform molecule. The composite catalysts on the basis of zinc, tungstophosphoric acid and titania exhibit exceptional performance in this reaction, high carbon monoxide selectivity and quantum efficiency of 7.1% at 362 nm. In-situ Fourier transform infrared and X-ray photoelectron spectroscopy suggest that the catalytic performance can be attributed to zinc species highly dispersed on tungstophosphoric acid /titania, which undergo reduction and oxidation cycles during the reaction according to the Mars–van Krevelen sequence. The reaction proceeds via intermediate formation of surface methyl carbonates. While methane has become an increasingly important chemical feedstock, its selective conversion to other chemicals has proven challenging. Here, authors demonstrate a photocatalyst based on earth-abundant elements that selectively converts methane to carbon monoxide under mild conditions.

CuM and AgM (M = Cr, Fe) catalysts were synthesized, characterized, and evaluated in methane reforming with CO2 with and without pretreatment under a H2 atmosphere. Their textural and structural characteristics were evaluated using various physicochemical methods, including XRD, B.E.T., SEM-EDS, XPS, and H2-TPR. It was shown that the nature of the species has a significant effect on these structural, textural, and reactivity properties. AgCr catalysts, presenting several oxidation states (Ag0, Ag+1, Cr3+, and Cr6+ in Ag, AgCrO2, and AgCr2O4), showed the most interesting catalytic performance in their composition. The intermediate Cr2O3 phase, formed during the catalytic reaction, played an important role as a catalytic precursor in the in situ production of highly dispersed nanoparticles, being less prone to coke formation in spite of the severe reaction conditions. In contrast, the AgFe catalyst showed low activity and a low selectivity for DRM in the explored temperature range, due to a significant contribution of the reverse water–gas shift reaction, which accounted for the low H2/CO ratios.

The development of the future French and European bioeconomies will involve developing new green chemical processes in which catalytic transformations are key. The VAALBIO team (valorization of alkanes and biomass) of the UCCS laboratory (Unité de Catalyse et Chimie du Solide) are working on various catalytic processes, either developing new catalysts and/or designing the whole catalytic processes. Our research is focused on both the fundamental and applied aspects of the processes. Through this review paper, we demonstrate the main topics developed by our team focusing mostly on oxygen- and hydrogen-related processes as well as on green hydrogen production and hybrid catalysis. The social impacts of the bioeconomy are also discussed applying the concept of the institutional compass.

To investigate the influence of Ag and the loading of Ni species, Ni-Ag type catalysts were synthesized with varying Ni/Ag ratios (1, 1.5 and 2) using the coprecipitation method. The catalysts were extensively characterized using various techniques such as TG-DSC-SM, XRD, ICP, BET, SEM-EDX and TPR and subsequently tested in the CH4/CO2 reaction without any pretreatment. Regardless of the ratio employed, a phase mixture containing NiO and Ag was observed after calcination under air between 600 °C and 1200 °C. SEM analysis confirmed the presence of a close interface between Ag and NiO. The specific surface area was found to be significantly higher for the catalyst with lower Ni content (R = 1). TPR analysis demonstrated that the inclusion of Ag facilitated the reduction of Ni at lower temperatures. XRD analyses of the spent catalyst confirmed catalyst reduction during the reaction. Among the samples, a catalyst with Ni/Ag = 1 exhibited superior catalytic activity without any pretreatment under a reduction atmosphere, in which case the conversions of methane and CO2 at 650 °C amounted to 38 and 45 mol%, respectively, with H2/CO = 0.7 and 71 mol% of H2. The presence of Ag species enhances the stability of the Ni catalyst and improves catalytic performance in the dry reforming of methane.

Bimetallic layered double oxide (LDO) NiM (M = Cr, Fe) catalysts with nominal compositions of Ni/M = 2 or 3 were tailored from layered double hydroxides (LDH) using a coprecipitation method to investigate the effects of the trivalent metal (Cr or Fe) and the amount of Ni species on the structural, textural, reducibility, and catalytic properties for CH4/CO2 reforming. The solids before (LDH) and after (LDO) thermal treatment at 500 °C were characterized using TGA-TD-SM, HT-XRD, XRD, Raman, and IR-ATR spectroscopies; N2 physical adsorption; XPS; and H2-TPR. According to the XRD and Raman analysis, a hydrotalcite structure was present at room temperature and stable up to 250 °C. The interlayer space decreased when the temperature increased, with a lattice parameter and interlayer space of 3.018 Å and 7.017 Å, respectively. The solids fully decomposed into oxide after calcination at 500 °C. NiO and spinel phases (NiM2O4, M = Cr or Fe) were observed in the NiM (M = Cr, Fe) catalysts, and Cr2O3 was detected in the case of NiCr. The NiFe catalysts show low activity and selectivity for DRM in the temperature range explored. In contrast, the chromium compound demonstrated interesting CH4 and CO2 conversions and generally excellent H2 selectivity at low reaction temperatures. CH4 and CO2 conversions of 18–20% with H2/CO of approx. 0.7 could be reached at temperatures as low as 500 °C, but transient behavior and deactivation were observed at higher temperatures or long reaction times. The excellent activity observed during this transient sequence was attributed to the stabilization of the metallic Ni particles formed during the reduction of the NiO phase due to the presence of NiCr2O4, opening the path for the use of these materials in periodic or looping processes for methane reforming at low temperature.

CuM and AgM (M = Cr, Fe) catalysts were synthesized, characterized, and evaluated in methane reforming with CO[sub.2] with and without pretreatment under a H[sub.2] atmosphere. Their textural and structural characteristics were evaluated using various physicochemical methods, including XRD, B.E.T., SEM-EDS, XPS, and H[sub.2]-TPR. It was shown that the nature of the species has a significant effect on these structural, textural, and reactivity properties. AgCr catalysts, presenting several oxidation states (Ag[sup.0], Ag[sup.+1], Cr[sup.3+], and Cr[sup.6+] in Ag, AgCrO[sub.2], and AgCr[sub.2]O[sub.4]), showed the most interesting catalytic performance in their composition. The intermediate Cr[sub.2]O[sub.3] phase, formed during the catalytic reaction, played an important role as a catalytic precursor in the in situ production of highly dispersed nanoparticles, being less prone to coke formation in spite of the severe reaction conditions. In contrast, the AgFe catalyst showed low activity and a low selectivity for DRM in the explored temperature range, due to a significant contribution of the reverse water–gas shift reaction, which accounted for the low H[sub.2]/CO ratios.

The abatement of toluene was studied in a sequential adsorption-plasma catalysis (APC) process. Within this process, Hopcalite was used as bifunctional material: as adsorbent (storage stage) and as catalyst via the oxidation of adsorbed toluene (discharge stage). It was observed that the desorption and oxidation activity of the adsorbed toluene was significantly affected the process variables. In addition, the adsorption time influenced the CO2 selectivity and CO2 yield by changing the interaction between the catalyst and the plasma generated species. At least four APC sequences were performed for each examined condition suggesting that Hopcalite is very stable under plasma exposure during all the sequences. Consequently, these results could contribute to advance the plasma–catalyst system with an optimal VOC oxidation efficiency. The catalytic activity, amount of toluene adsorbed, amount of toluene desorbed and product formation have been quantified by FT-IR. Moreover, the catalyst was characterized by XRD, H2-TPR, N2 adsorption–desorption analysis and XPS. Hopcalite shows a good CO2 selectivity and CO2 yield when the APC process is performed with an adsorption time of 20 min and a plasma treatment with a discharge power of 46 W which leads to a low energy cost of 11.6 kWh·m−3 and energy yields of toluene and CO2 of 0.18 (±0.01) g·kWh−1 and 0.48 (±0.06) g·kWh−1 respectively.

CuM and AgM (M = Cr, Fe) catalysts were synthesized, characterized, and evaluated in methane reforming with CO with and without pretreatment under a H atmosphere. Their textural and structural characteristics were evaluated using various physicochemical methods, including XRD, B.E.T., SEM-EDS, XPS, and H -TPR. It was shown that the nature of the species has a significant effect on these structural, textural, and reactivity properties. AgCr catalysts, presenting several oxidation states (Ag , Ag , Cr , and Cr in Ag, AgCrO , and AgCr O ), showed the most interesting catalytic performance in their composition. The intermediate Cr O phase, formed during the catalytic reaction, played an important role as a catalytic precursor in the in situ production of highly dispersed nanoparticles, being less prone to coke formation in spite of the severe reaction conditions. In contrast, the AgFe catalyst showed low activity and a low selectivity for DRM in the explored temperature range, due to a significant contribution of the reverse water-gas shift reaction, which accounted for the low H /CO ratios.

A novel strategy for toluene abatement was investigated using a sequential adsorption-regeneration process. Commercial Hopcalite (CuMn2Ox, Purelyst101MD), Ceria nanorods, and UiO-66-SO3H, a metal–organic framework (MOF), were selected for this study. Toluene was first adsorbed on the material and a mild thermal activation was performed afterwards in order to oxidize toluene into CO2 and H2O. The materials were characterized by XRD, N2 adsorption-desorption analysis, H2-TPR and TGA/DSC. The best dynamic toluene adsorption capacity was observed for UiO-66-SO3H due to its hierarchical porosity and high specific surface area. However, in terms of balance between storage and catalytic properties, Hopcalite stands out from others owing to its superior textural/chemical properties promoting irreversible toluene adsorption and outstanding redox properties, allowing a high activity and CO2 selectivity in toluene oxidation. The high conversion of toluene into CO2 which easily desorbs from the surface during heating treatment shows that the sequential adsorption-catalytic thermal oxidation can encompass a classical oxidation process in terms of efficiency, CO2 yield, and energy-cost saving, providing that the bifunctional material displays a good stability in repetitive working conditions.

An original process based on cold plasma assisted polymerization of tetramethyldisiloxane (TMDSO) in the presence of O2 was developed to cover substrates showing various shapes (plate and foam). In the frame of catalytic application, this coating has to act as a bonding layer for the deposition of active phase such as VOx/TiO2 well‐known for its properties in NOx and volatile organic compounds abatement and in the production of chemical intermediates. Good results were obtained by the deposition of a 5‐μm thick polysiloxane film followed by a thermal treatment under air at 650°C and by a remote nitrogen plasma post treatment. This procedure led to a silica‐like layer allowing its coating in an aqueous suspension of TiO2. Such a multilayered material can be obtained homogeneously on the whole surface of a sample showing a 3D open geometry like metallic foam. Characterizations of the different steps of the elaborated multilayer material were performed by Fourier transformed infrared spectroscopy, Raman spectrometry, X‐ray photoelectron spectroscopy, and electron probe micro‐analyzer. POLYM. ENG. SCI., 2011. © 2011 Society of Plastics Engineers