Hydrodechlorination of trifluoro-trichloroethane to chlorotrifluoroethylene:Revealing the deactivation mechanism and regeneration strategy of Pd-Cu/AC catalyst

Chlorotrifluoroethylene(CTFE)is a vital fluorinated olefinic monomer produced through the catalytic hydrodechlorination of trichlorotrifluoroethane(CFC-113),an eco-friendly process.However,hydrodechlorination catalysts for olefin production often suffer from poor stability.The Pd/AC catalyst and Pd-Cu/AC catalyst prepared by co-impregnation method exhibited poor stability,Pd-Cu/AC catalyst with CFC-113 conversion dropping to around 37%after 50 h of hydrodechlorination reaction.Brunauer-Emmett-Teller,transmission electron microscopy,X-ray photoelectron spectroscopy,and X-ray diffraction of fresh and deactivated Pd/AC catalysts indicate that the deactivation of Pd/AC catalysts is due to high-temperature agglomeration of Pd.Comparative analysis of fresh and deactivated Pd-Cu/AC catalysts using Brunauer-Emmett-Teller,transmission electron microscopy,and thermogravimetric analysis techniques revealed decreased dispersion of active sites,reduced surface area,catalyst aggregation deactivation,and a significant decrease in Cu content.Furthermore,the results of NH3-TPD revealed that the acid sites of the catalyst increased significantly.X-ray diffraction spectra indicated the formation of new species,basic copper chloride(Cu_(2)(OH)_(3)Cl),during the reaction.As the reaction progressed,these new species agglomerated,leading to a gradual loss of catalyst activity.Moreover,the deactivated catalyst was successfully reactivated using a simple alkaline washing method.

Metasurface-based nanoprinting: principle, design and advances

Metasurface-based nanoprinting(meta-nanoprinting)has fully demonstrated its advantages in ultrahigh-density gray-scale/color image recording and display.A typical meta-nanoprinting device usually has image resolutions reaching 80 k dots per inch(dpi),far exceeding conventional technology such as gravure printing(typ.5 k dpi).Besides,by fully exploit-ing the design degrees of freedom of nanostructured metasurfaces,meta-nanoprinting has been developed from previ-ous single-channel to multiple-channels,to current multifunctional integration or even dynamic display.In this review,we overview the development of meta-nanoprinting,including the physics of nanoprinting to manipulate optical amplitude and spectrum,single-functional meta-nanoprinting,multichannel meta-nanoprinting,dynamic meta-nanoprinting and mul-tifunctional metasurface integrating nanoprinting with holography or metalens,etc.Applications of meta-nanoprinting such as image display,vortex beam generation,information decoding and hiding,information encryption,high-density optical storage and optical anti-counterfeiting have also been discussed.Finally,we conclude the opportunities and chal-lenges/perspectives in this rapidly developing research field of meta-nanoprinting.

Full-space Cloud of Random Points with a Scrambling Metasurface

With the rapid progress in computer science,including artificial intelligence,big data and cloud computing,full-space spot generation can be pivotal to many practical applications,such as facial recognition,motion detection,augmented reality,etc.These opportunities may be achieved by using diffractive optical elements(DOEs)or light detection and ranging(LIDAR).However,DOEs suffer from intrinsic limitations,such as demanding depth-controlled fabrication techniques,large thicknesses(more than the wavelength),Lambertian operation only in half space,etc.LIDAR nevertheless relies on complex and bulky scanning systems,which hinders the miniaturization of the spot generator.Here,inspired by a Lambertian scatterer,we report a Hermitian-conjugate metasurface scrambling the incident light to a cloud of random points in full space with compressed information density,functioning in both transmission and reflection spaces.Over 4044 random spots are experimentally observed in the entire space,covering angles at nearly 90°.Our scrambling metasurface is made of amorphous silicon with a uniform subwavelength height,a nearly continuous phase coverage,a lightweight,flexible design,and low-heat dissipation.Thus,it may be mass produced by and integrated into existing semiconductor foundry designs.Our work opens important directions for emerging 3D recognition sensors,such as motion sensing,facial recognition,and other applications.

Cascaded metasurface for separated information encryption[Invited]

For a conventional cascaded metasurface,the combination channel and each single channel are mutually dependent because the phase modulation of a cascaded metasurface is the sum of each single one.Here we propose a cascaded metasurface that can independently encode information into multiple channels.Based on the orientation degeneracy of anisotropic metasurfaces,each single metasurface can produce a quick-response(QR)image in the near field,governed by the Malus law,while the combined channel can produce a holographic image in the far field,governed by geometric phase.The independent and physically separated trichannel design makes information encryption safer.

Perovskite single-pixel detector for dual-color metasurface imaging recognition in complex environment

Highly efficient multi-dimensional data storage and extraction are two primary ends for the design and fabrication of emerging optical materials.Although metasurfaces show great potential in information storage due to their modulation for different degrees of freedom of light,a compact and efficient detector for relevant multi-dimensional data retrieval is still a challenge,especially in complex environments.Here,we demonstrate a multi-dimensional image storage and retrieval process by using a dual-color metasurface and a double-layer integrated perovskite single-pixel detector(DIP-SPD).Benefitting from the photoelectric response characteristics of the FAPbBr2.4l0.6 and FAPbl3 films and their stacked structure,our filter-free DIP-SPD can accurately reconstruct different colorful images stored in a metasurface within a single-round measurement,even in complex environments with scattering media or strong background noise.Our work not only provides a compact,filter-free,and noise-robust detector for colorful image extraction in a metasurface,but also paves the way for color imaging application of perovskite-like bandgap tunable materials.

Malus-metasurface-assisted polarization multiplexing

Polarization optics plays a pivotal role in diffractive,refractive,and emerging flat optics,and has been widely employed in contemporary optical industries and daily life.Advanced polarization manipulation leads to robust control of the polarization direction of light.Nevertheless,polarization control has been studied largely independent of the phase or intensity of light.Here,we propose and experimentally validate a Malus-metasurface-assisted paradigm to enable simultaneous and independent control of the intensity and phase properties of light simply by polarization modulation.The orientation degeneracy of the classical Malus’s law implies a new degree of freedom and enables us to establish a one-to-many mapping strategy for designing anisotropic plasmonic nanostructures to engineer the Pancharatnam–Berry phase profile,while keeping the continuous intensity modulation unchanged.The proposed Malus metadevice can thus generate a near-field greyscale pattern,and project an independent far-field holographic image using an ultrathin and single-sized metasurface.This concept opens up distinct dimensions for conventional polarization optics,which allows one to merge the functionality of phase manipulation into an amplitudemanipulation-assisted optical component to form a multifunctional nano-optical device without increasing the complexity of the nanostructures.It can empower advanced applications in information multiplexing and encryption,anti-counterfeiting,dual-channel display for virtual/augmented reality,and many other related fields.

Zero-order-free meta-holograms in a broadband visible range

The unwanted zero-order light accompanied by the birth of diffractive optical elements and caused mainly by fabrication errors and wavelength variations is a key factor that deteriorates the performance of diffraction-related optical devices such as holograms,gratings,beam shapers,beam splitters,optical diffusers,and diffractive microlenses.Here,inspired by the unique characteristic of nano-polarizer-based metasurfaces for both positive and negative amplitude modulation of incident light,we propose a general design paradigm to eliminate zero-order diffraction without burdening the metasurface design and fabrication.The experimentally demonstrated metahologram,which projects a holographic image with a wide angle of 70°×70°in the for field,presents a very low zero-order intensity(only 0.7%of the total energy of the reconstructed image).More importantly,the zero-orderfree meta-hologram has a large tolerance limit for wavelength variations(under a broadband illumination from520 to 660 nm),which brings important technical advances.The strategy proposed could significantly relieve the fabrication difficulty of metasurfaces and be viable for various diffractive-optics-related applications includingholography,laser beam shaping,optical data storage,vortex beam generation,and so on.