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Hierarchically porous P substituted HZSM‐5 (H[P, Al]‐ZSM‐5‐AT‐0.05 M) was successfully synthesized by isomorphous substitution method with introduced P atoms into ZSM‐5 zeolite frameworks followed by alkali treatment. H[P, Al]‐ZSM‐5‐AT‐0.05 M was characterized by XRD, ICP‐OES, SEM, FT‐IR, N2 adsorption‐desorption, NH3‐TPD, XPS, Py‐IR, and TG‐DTA, respectively. The surface area, pore volume, particle size and P/Al (molar ratio) are 328 m2.g−1, 0.23 cm3.g−1, 563 nm and 0.027, respectively. The catalytic performance of H[P, Al]‐ZSM‐5‐AT‐0.05 M in coupling reaction of methanol with 1‐butene was investigated in the fixed‐bed reactor. On the condition of reaction temperature at 500°C under atmosphere pressure, the main product is propylene with the selectivity and yield of 33.7% and 31.0%, respectively. Hydrogen transfer index was calculated to 0.24. Moreover, its diffusion limitation was investigated with the self‐etherification of benzyl alcohol reaction. The value of Thiele modulus (η) and effectiveness factor (ϕ) are 0.08 and 16.9, respectively. The scheme of isomorphously substituted method of introducing P into ZSM‐5 framework and catalytic performance over H[P, Al]‐ZSM‐5 and H[P, Al]‐ZSM‐5‐AT‐0.05 M in coupling methanol with 1‐butene. P substituted HZSM‐5 is treated with NaOH solution to form mesoporous zeolites. The result shows that H[P, Al]‐ZSM‐5‐AT‐0.05 M exhibited higher catalytic stability, higher apparent reaction rate, effectiveness factor and lower content of diffusion limitation in coupling of methanol with 1‐butene to propylene reaction. [ABSTRACT FROM AUTHOR]

We prepared ZnZr 7 O/HZ-1.5NH 4 F tandem catalyst with high catalytic activity for the direct conversion of CO 2 hydrogenation to aromatics by combining theoretical calculations and experiments. [Display omitted] • It was simulated that the (0 1 0) plane of the sheet HZSM-5 had the strongest adsorption capacity for CH 3 O* and CHOO*. • We prepared catalysts with high catalytic activity and stability by combining theoretical calculations and experiments. • The thickness can be precisely adjusted to prepare a series of sheet HZSM-5 by adding urea and NH 4 F. • Urea inhibits the generation of defective sites in HZSM-5, while NH 4 F promotes the generation of defective sites. • The thickness of the sheet HZSM-5 is also a factor affecting the catalytic activity. The adsorption properties of CH 3 O* and CHOO* adsorbed on the three crystal planes (0 0 1, 0 1 0, 1 0 1) of HZSM-5 were simulated by the generalized gradient approximation (GGA) of density functional theory (DFT), it was found that the (0 1 0) plane corresponding to the b-axis of the sheet HZSM-5 had the strongest adsorption energy for CH 3 O* and CHOO*. Therefore, we successfully synthesized sheet HZSM-5 with different thicknesses by adding the inhibitor (urea) and mineralizer (F−) to the synthesis system based on the theoretical calculations. The physicochemical properties of HZSM-5 were investigated by the characterization methods of SEM, TEM, Py-IR, OH-IR, CO 2 -TPD and so on. The results showed the thickness of HZSM-5 can be precisely adjusted by adding urea and NH 4 F and changing the ratio of urea/NH 4 F or TPAOH/NH 4 F. Then, the sheet HZSM-5 and ZnZr 7 O were connected in tandem to investigate the reaction conditions and catalytic performance for the direct conversion of CO 2 hydrogenation to aromatics. It was found that the HZ-1.5NH 4 F had a large specific surface area, suitable B acid content and more defect sites. These advantages resulted in a high aromatic selectivity of 77.5% and CO 2 conversion of 17.6% over ZnZr 7 O/HZ-1.5NH 4 F. Meanwhile, it exhibits stable performance and no significant deactivation after 80 h of operation. [ABSTRACT FROM AUTHOR]

[Display omitted] • The right amount of cobalt ions could induce the formation of Fe 1-x S. • 100 mL orange II solution (30 mg/L) was degraded to 99.9% within 15 min. • OH and h+ played an important role in the photo-Fenton-like process. • FeS 2 -Fe 1-x S exhibited excellent stability and high catalytic degradation activity for other dyes. It is a challenge to develop heterogeneous Fenton-like catalysts with excellent performance and stability in the field of wastewater treatment. In this work, the FeS 2 -Fe 1-x S heterostructure catalyst was prepared by solvothermal method through adding cobalt element to change the particle nucleation process and inhibit the transformation process of pyrrhotite (Fe 1-x S) phase to pyrite (FeS 2) phase. Then, a series of experiments were devised to clarify the catalytic activity of FeS 2 -Fe 1-x S heterostructure. The degradation experiments exhibited that 99.9% degradation efficiency was achieved for 30 mg/L orange II solution within 15 min at the conditions of 0.2 g/L FeS 2 -Fe 1-x S, 2 mM H 2 O 2 and pH = 3.0. In addition, the reusability of the FeS 2 -Fe 1-x S catalyst was also investigated and the result displayed that degradation efficiency of orange II can reach 95.2% after eight cycles. The degradation of orange II was enhanced by Fenton reaction between FeS 2 -Fe 1-x S and dissolved oxygen, which could smoothly release Fe2+ and Fe3+ for the activation of H 2 O 2 to produce more hydroxyl radicals. Finally, the degradation pathway of orange II was proposed by detecting intermediates produced in FeS 2 -Fe 1-x S/H 2 O 2 photo-Fenton-like system by liquid chromatography-mass spectrometry (LC-MS). In short, FeS 2 -Fe 1-x S is a promising catalyst for removing the organic pollutants from solutions. [ABSTRACT FROM AUTHOR]

Elemental doping has been proven to be an effective strategy for increasing the catalytic activity and structural stability of Fenton catalysts. Therefore, this work reports that Mn-doped FeS 2 /Fe 2 O 3 (Mn 3 O 4 –FeS 2 /Fe 2 O 3) has excellent catalytic performance for the degradation of Orange II under simulated solar energy. Degradation experiment results showed that the sample with a manganese-iron molar ratio of 1:2 exhibited higher activity than others. The degradation rate of 20 mg/L OII reached 99.0% in 18 min under the conditions of 0.3 g/L Mn 3 O 4 –FeS 2 /Fe 2 O 3 , 5 mM H 2 O 2 and pH = 2.8. In addition to, the Mn 3 O 4 –FeS 2 /Fe 2 O 3 catalyst shows good reusability for Orange II and high activity for other dyes (MB, MG, Rh B and MO) under optimal conditions. Degradation mechanism study indicated that the heterogeneous Fenton reaction was promoted by retarding the recombination of photogenerated charge carriers and accelerating the cycle between Fe3+/Mn2+ and Fe2+/Mn3+, which improved photo-Fenton-like catalytic performance, resulting in the enhanced degradation of organic pollutant. Finally, a possible degradation pathway was proposed according to the results of liquid chromatography-mass spectrometry (LC-MS). In short, the catalyst has potential application value in wastewater treatment. • The degradation of Orange II by Mn 3 O 4 –FeS 2 /Fe 2 O 3 attained to 99.0% in 18 min. • Both.•OH and •O 2 − played important roles in the degradation process. • The photo-Fenton-like catalytic performance of the Mn 3 O 4 –FeS 2 /Fe 2 O 3 catalyst was enhanced. • The catalyst maintained excellent reusability for Orange II and high activity for other dyes. [ABSTRACT FROM AUTHOR]