RESUMEN
Ni-Ti intercalated bentonite catalysts (Ni-Ti-bentonite) and Ni-TiO2 supported bentonite catalysts (Ni-TiO2 /bentonite) were prepared, and the effects of Ni-Ti supported and intercalated bentonite on the selective hydrogenation of cinnamaldehyde were investigated. Ni-Ti intercalated bentonite enhanced the Brønsted acid sites strength, decreased the acid amount and Lewis's acid sites strength, which inhibited the activation of the C=O bond and contributed to selective hydrogenation of the C=C bond. When Ni-TiO2 was supported on bentonite, the acid amount and Lewis's acid strength of the catalyst increased, providing additional adsorption sites and increased the acetals byproducts. Due to the higher surface area, mesoporous volume, and suitable acidity, compared with Ni-TiO2 /bentonite in methanol solvent, 2â MPa, 120 °C for 1â h, Ni-Ti-bentonite exhibited a higher cinnamaldehyde (CAL) conversion of 98.8 %, as well as a higher hydrocinnamaldehyde (HCAL) selectivity of 95 %, and no acetals were found in the product.
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Two-dimensional (2D) photocatalysts have attracted considerable research interest in the past decades due to their unique optical, physical and chemical properties. Constructing 2D/2D heterojunctions with large interface area has been considered as an effective approach to enhance the transfer rate and the separation efficiency of the charge carriers, leading to dramatic increase in the photocatalytic performance of the photocatalysts. Here, the state-of-the-art progress on heterojunctions based on 2D materials is reviewed, including the photocatalysis principles using 2D heterojunctions, the categories of 2D heterojunctions and their application in different photocatalytic reactions, and the theoretical studies of the 2D heterojunctions. Moreover, the advantages and disadvantages of the 2D heterojunctions are also discussed. Finally, the ongoing challenges and opportunities for the future development of 2D photocatalysts with built-in heterojunctions are proposed.
RESUMEN
CO2 is activated in a plasma reactor followed by hydrogenation over a Cu-Fe-Ce/HZSM-5 catalyst, and the intrinsic kinetics of the plasma catalytic process are studied. Compared with CO2 hydrogenation using Cu-Fe-Ce/HZSM-5 alone, the CO2 conversion and the dimethyl ether selectivity for the plasma catalytic process are increased by 16.3 %, and 10.1 %, respectively, indicating that the CO2 was activated by the plasma to promote hydrogenation. A study of the intrinsic kinetics shows that the activation energies of methanol formation, the reverse water-gas shift reaction, and methanol dehydration to dimethyl ether are 149.34, 75.47, and 73.18â kJ mol-1 , respectively, which are lower than if Cu-Fe-Ce/HZSM-5 is used without plasma, indicating that the activation of CO2 in the plasma reduces the activation energy of the hydrogenation reaction and improves the yield of dimethyl ether.
RESUMEN
Two-component catalysts have garnered significant attention in the field of catalysis due to their ability to inhibit Ni sintering. In the present work, honeycomb-structuralstructured Al2O3-supported Ni and B were prepared to enhance coke tolerance during dry reforming of methane (DRM). Transmission electron microscopy (TEM) results revealed that the average particle sizes on Ni/Al2O3 and Ni-0.16B/Al2O3 were 7.6â nm and 4.2â nm, respectively, indicating that B can effectively inhibit Ni sintering. After a 100-hour reaction, the conversion of CH4 and CO2 on Ni/Al2O3 decreased by approximately 5 %, whereas on Ni-0.16B/Al2O3, there was no significant decrease in CH4 and CO2 conversion, with values of approximately 81.6 % and 87.2 %, respectively. In situ DRIFT spectra demonstrated that Ni-0.16B/Al2O3 enhanced the activation of CO2, thus improving the catalyst's stability. A Langmuir-Hinshelwood-Hougen-Watson (LHHW) model was developed for intrinsic kinetics, and the resulting kinetic expressions were well-fitted fit to the experimental data, with R2 values exceeding 0.9. ActivationThe activation energies were also calculated. The outstanding stability of Ni-0.16B/Al2O3 can be attributed to its stable honeycomb structure and B's ability to significantly inhibit Ni sintering, reduce catalyst particle size, and enhance coke tolerance.
RESUMEN
The photocatalytic CO2 reduction strategy driven by visible light is a practical way to solve the energy crisis. However, limited by the fast recombination of photogenerated electrons and holes in photocatalysts, photocatalytic efficiency is still low. Herein, a WO3/BiOBr S-scheme heterojunction was formed by combining WO3 with BiOBr, which facilitated the transfer and separation of photoinduced electrons and holes and enhanced the photocatalytic CO2 reaction. The optimized WO3/BiOBr heterostructures exhibited best activity for photocatalytic CO2 reduction without any sacrificial reagents, and the CO yield reached 17.14 µmol g-1 after reaction for 4 h, which was 1.56 times greater than that of BiOBr. The photocatalytic stability of WO3/BiOBr was also improved.
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With the development of modern society, environmental pollution and energy shortage have become the focus of worldwide attention [...].
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To improve the water absorbency and water-retention rate of superabsorbent materials, a porous calcium carbonate composite superabsorbent polymer (PCC/PAA) was prepared by copolymerization of acrylic acid and porous calcium carbonate prepared from ground calcium carbonate. The results showed that the binding energies of C-O and C=O in the O 1s profile of PCC/PAA had 0.2 eV and 0.1-0.7 eV redshifts, respectively, and the bonding of -COO- groups on the surface of the porous calcium carbonate led to an increase in the binding energy of O 1s. Furthermore, the porous calcium carbonate chelates with the -COO- group in acrylic acid through the surface Ca2+ site to form multidirectional crosslinking points, which would increase the flexibility of the crosslinking network and promote the formation of pores inside the PCC/PAA to improve the water storage space. The water absorbency of PCC/PAA with 2 wt% porous calcium carbonate in deionized water and 0.9 wt% NaCl water solution increased from 540 g/g and 60 g/g to 935 g/g and 80 g/g, respectively. In addition, since the chemical crosslinker N,N'-methylene bisacrylamide is used in the polymerization process of PCC/PAA, N,N'-methylene bisacrylamide and porous calcium carbonate enhance the stability of the PCC/PAA crosslinking network by double-crosslinking with a polyacrylic acid chain, resulting in the crosslinking network of PCC/PAA not being destroyed after water absorption saturation. Therefore, PCC/PAA with 2 wt% porous calcium carbonate improved the water-retention rate by 244% after 5 h at 60 °C, and the compressive strength was approximately five-times that of the superabsorbent without porous calcium carbonate.
RESUMEN
Photocatalytic CO2 reduction is a tactic for solving the environmental pollution caused by greenhouse gases. Herein, NH4H2PO4 was added as a phosphorus source in the process of the hydrothermal treatment of melamine for the first time, and phosphorus-doped hollow tubular g-C3N4 (x-P-HCN) was fabricated and used for photocatalytic CO2 reduction. Here, 1.0-P-HCN exhibited the largest CO production rate of 9.00 µmol·g-1·h-1, which was 10.22 times higher than that of bulk g-C3N4. After doping with phosphorus, the light absorption range, the CO2 adsorption capacity, and the specific surface area of the 1.0-P-HCN sample were greatly improved. In addition, the separation of photogenerated electron-hole pairs was enhanced. Furthermore, the phosphorus-doped g-C3N4 effectively activated the CO2 adsorbed on the surface of phosphorus-doped g-C3N4 photocatalysts, which greatly enhanced the CO production rate of photocatalytic CO2 reduction over that of g-C3N4.
RESUMEN
Constructing an efficient photoelectron transfer channel to promote the charge carrier separation is a great challenge for enhancing photocatalytic hydrogen evolution from water. In this work, an ultrathin 2D/2D Ti3 C2 Tx /ZnIn2 S4 heterostructure is rationally designed by coupling the ultrathin ZnIn2 S4 with few-layered Ti3 C2 Tx via the electrostatic self-assembly strategy. The 2D/2D Ti3 C2 Tx /ZnIn2 S4 heterostructure possesses larger contact area and strong electronic interaction to promote the charge carrier transfer at the interface, and the sulfur vacancy on the ZnIn2 S4 acting as the electron trap further enhances the separation of the photoinduced electrons and holes. As a consequence, the optimal 2D/2D Ti3 C2 Tx /ZnIn2 S4 composite exhibits a high photocatalytic hydrogen evolution rate of 148.4 µmol h-1 , which is 3.6 times and 9.2 times higher than that of ZnIn2 S4 nanosheet and flower-like ZnIn2 S4 , respectively. Moreover, the stability of the ZnIn2 S4 is significantly improved after coupling with the few-layered Ti3 C2 Tx . The characterizations and density functional theory calculation demonstrate that the synergistic effect of the sulfur vacancy and Ti3 C2 Tx cocatalyst can greatly promote the electrons transfer from ZnIn2 S4 to Ti3 C2 Tx and the separation of photogenerated charge carriers, thus enhancing the photocatalytic hydrogen evolution from water.
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Two-dimensional (2D)-structured photocatalysts with atomically thin layers not only have the potential to enhance hydrogen generation efficiency but also allow more direct investigations of the effects of surface terminations on photocatalytic activity. Taking 2D Bi2WO6 as a model, we found that the configuration of bilayer Bi2O2 sandwiched by alternating WO4 layers enabled the thermodynamic driving potential for photocatalytic hydrogen evolution. Without Pt deposition, the H2 generation efficiency can reach to 56.9 µmol/g/h by 2D Bi2WO6 as compared with no activity of Bi2WO6 nanocrystals under simulated solar light. This configuration is easily functionalized by adsorption of Cl-/Br- to form Bi-Cl/Bi-Br bonds, which leads to the decrease of recombination in photogenerated charge carriers and narrower band gaps. This work highlights an effective way to design photocatalysts with efficient hydrogen evolution by tuning the surface terminations.
RESUMEN
Photocatalytic hydrogen evolution from water has received enormous attention due to its ability to address a number of global environmental and energy-related issues. Here, we synthesize 2D/2D Ti3C2/g-C3N4 composites by electrostatic self-assembly technique and demonstrate their use as photocatalysts for hydrogen evolution under visible light irradiation. The optimized Ti3C2/g-C3N4 composite exhibited a 10 times higher photocatalytic hydrogen evolution performance (72.3 µmol h-1 gcat-1) than that of pristine g-C3N4 (7.1 µmol h-1 gcat-1). Such enhanced photocatalytic performance was due to the formation of 2D/2D heterojunctions in the Ti3C2/g-C3N4 composites. The intimate contact between the monolayer Ti3C2 and g-C3N4 nanosheets promotes the separation of photogenerated charge carriers at the Ti3C2/g-C3N4 interface. Furthermore, the ultrahigh conductivity of Ti3C2 and the Schottky junction formed between g-C3N4/MXene interfaces facilitate the photoinduced electron transfer and suppress the recombination with photogenerated holes. This work demonstrates that the 2D/2D Ti3C2/g-C3N4 composites are promising photocatalysts thanks to the ultrathin MXenes as efficient co-catalysts for photocatalytic hydrogen production.
RESUMEN
Hydrogen production through facile photocatalytic water splitting is regarded as a promising strategy to solve global energy problems. Transition-metal carbides (MXenes) have recently drawn attention as potential co-catalyst candidates for photocatalysts. Here, we report niobium pentoxide/carbon/niobium carbide (MXene) hybrid materials (Nb2 O5 /C/Nb2 C) as photocatalysts for hydrogen evolution from water splitting. The Nb2 O5 /C/Nb2 C composites were synthesized by one-step CO2 oxidation of Nb2 CTx . Nb2 O5 grew homogeneously on Nb2 C after mild oxidation, during which some amorphous carbon was also formed. With an optimized oxidation time of 1.0â h, Nb2 O5 /C/Nb2 C showed the highest hydrogen generation rate (7.81â µmol h-1 gcat-1 ), a value that was four times higher than that of pure Nb2 O5 . The enhanced performance of Nb2 O5 /C/Nb2 C was attributed to intimate contact between Nb2 O5 and conductive Nb2 C and the separation of photogenerated charge carriers at the Nb2 O5 /Nb2 C interface; the results presented herein show that transition-metal carbide are promising co-catalysts for photocatalytic hydrogen production.