The selective deposition of Fe species inside ZSM-5 for the oxidation of cyclohexane to cyclohexanone

The design of efficient iron-based catalysts remains a great challenge for selective cyclohexane oxidation to cyclohexanone under mild conditions.Because of the complex distribution of iron location on the support,the selectivity is always low.Here,we report a general strategy to selectively deposit highly-dispersed FeO_(x) into the micropore of ZSM-5 by atomic layer deposition(ALD).The framework of ZSM-5 and the Bronsted acid sites are intact during ALD,and the Fe species are selectively deposited onto the defect and Lewis acid sites of ZSM-5.Besides,more Fe–O–Si bonds are formed over FeO_(x)/ZSM-5 with a low loading of Fe,while FeO_(x) nanoparticles are generated at high Fe loading.They cannot be realized by the traditional solution method.The obtained FeO_(x)/ZSM-5 catalysts perform high selectivity of cyclohexanone(92%–97%),and ALD cycle numbers of FeO_(x) control the activity.Compared with the Fe nanoparticles,the Fe–O–Si species performs higher turnover frequency and stability in the oxidation reaction.

Distance Effect of Ni-Pt Dual Sites for Active Hydrogen Transfer in Tandem Reaction

Unveiling the distance effect between different sites in multifunctional catalysts remains a major challenge.Herein,we investigate the distance effect by constructing a dual-site distance-controlled tandem catalyst with a five-layered TiO2/Pt/TiO2/Ni/TiO2 tubular nanostructure by template-assisted atomic layer deposition.In this catalyst,the Ni and Pt sites are separated by a porous TiO2 interlayer,and the distance between them can be precisely controlled on the subnanometer scale by altering the thickness of the interlayer,while the inner and outer porous TiO2 layers are designed for structural stability.The catalyst exhibits superior performance for the tandem hydrazine hydrate decomposition to hydrogen and subsequent nitrobenzene hydrogenation when the Ni and Pt site distance is on the subnanometer level.The performance increases with the decrease of the distance and is better than the catalyst without the TiO2 interlayer.Isotopic and kinetic experiments reveal that the distance effect controls the transfer of active hydrogen,which is the rate-determining step of the tandem reaction in a water solvent.Reduced Ti species with oxygen vacancies on the TiO2 interlayer provide the active sites for hydrogen transfer with-Ti-OH surface intermediates via the continuous chemisorption/desorption of water.A smaller distance induces the generation of more active sites for hydrogen transfer and thus higher efficiency in the synergy of Ni and Pt sites.Our work provides new insight for the distance effect of different active sites and the mechanism of intermediate transfer in tandem reactions.

Fast Carrier Selection of JPEG Steganography Appropriate for Application

In recent years,the improvement of the security of steganography mainly involves not only carrier security but also distortion function.In the actual environment,the existing method of carrier selection is limited by its complex algorithm and slow running speed,making it not appropriate for rapid communication.This study proposes a method for selecting carriers and improving the security of steganography.JPEG images are decompressed to spatial domain.Then correlation coefficients between two adjacent pixels in the horizontal,vertical,counter diagonal,and major diagonal directions are calculated.The mean value of the four correlation coefficients is used to evaluate the security of each JPEG image.The images with low correlation coefficients are considered safe carriers and used for embedding in our scheme.The experimental results indicate that the stego images generated from the selected carriers exhibit a higher anti-steganalysis capability than those generated from the randomly selected carriers.Under the premise of the same security level,the images with low correlation coefficients have a high capacity.Our algorithm has a very fast running speed,and the running time of a 2048×2048 image is less than 1 s.