State Key Laboratory of Solidification Processing

Despite being one of the oldest materials described in the chemical literature, graphitic carbon nitride (g-C3N4) has just recently experienced a renaissance as a highly active photocatalyst, and the metal-free polymer was shown to be able to generate hydrogen under visible light. The semiconductor nature of g-C3N4 has triggered tremendous endeavors on its structural manipulation for enhanced photo(electro)chemical performance, aiming at an affordable clean energy future. While pursuing the stem of g-C3N4 related catalysis (photocatalysis, electrocatalysis and photoelectrocatalysis), a number of emerging intrinsic properties of g-C3N4 are certainly interesting, but less well covered, and we believe that these novel applications outside of conventional catalysis can be favorably exploited as well. Thanks to the general efforts devoted to the exploration and enrichment of g-C3N4 based chemistry, the boundaries of this area have been possibly pushed far beyond what people could imagine in the beginning. This review strives to cover the achievements of g-C3N4 related materials in these unconventional application fields for depicting the broader future of these metal-free and fully stable semiconductors. This review starts with the general protocols to engineer g-C3N4 micro/nanostructures for practical use, and then discusses the newly disclosed applications in sensing, bioimaging, novel solar energy exploitation including photocatalytic coenzyme regeneration, templating, and carbon nitride based devices. Finally, we attempt an outlook on possible further developments in g-C3N4 based research.

Abstract High‐performance graphene microwave absorption materials are highly desirable in daily life and some extreme situations. A simple technique for the direct growth of graphene as absorption fillers in wave‐transmitting matrices is of paramount importance to bring it to real‐world application. Herein, a simple chemical vapor deposition (CVD) route for the direct growth of edge‐rich graphene (ERG) with tailored structures and tunable dielectric properties in porous Si 3 N 4 ceramics using only methyl alcohol (CH 3 OH) as precursor is reported. The large O/C atomic ratio of CH 3 OH helps to build a mild oxidizing atmosphere and leads to a unique structure featuring open graphite nanosteps and freestanding nanoplanes, endowing the ERG/Si 3 N 4 hybrid with an appropriate balance between good impedance matching and strong loss capacity. Accordingly, the prepared materials exhibit superior electromagnetic wave absorption, far surpassing that of traditional CVD graphene and reduced graphene oxide‐based materials, achieving an effective absorption bandwidth of 4.2 GHz covering the entire X band, with a thickness of 3.75 mm and a negligibly low loading content of absorbents. The results provide new insights for developing novel microwave absorption materials with strong reflection loss and wide absorption frequency range.

Nitrogen self-doped graphitic carbon nitride was successfully synthesized by the co-thermal condensation of the precursor with a nitrogen-rich additive.

Zinc ion stabilized MnO₂ nanospheres with a flower-like morphology and mesoporous texture are prepared, and they show high specific capacity and superior cycling stability for Zn-ion batteries.

Simultaneous achievement of a large <italic>W</italic>_rec of 3.51 J cm⁻³ and a high <italic>η</italic> of 80.1% in 0.86NN–0.14BNH ceramics under 350 kV cm⁻¹, leading to an excellent comprehensive energy storage performance in lead-free bulk ceramics.

Due to the excellent electrical transport properties and optoelectronic performance, thin indium selenide (InSe) has recently attracted attention in the field of 2D semiconducting materials.

Considering the recent breakthroughs in the synthesis of novel two-dimensional (2D) materials from layered bulk structures, ternary layered transition metal borides, known as MAB phases, have come under scrutiny as a means of obtaining novel 2D transition metal borides, the so-called MBenes. Here, based on a set of phonon calculations, we show the dynamic stability of many Al-containing MAB phases, MAlB (M = Ti, Hf, V, Nb, Ta, Cr, Mo, W, Mn, Tc), M2AlB2 (Sc, Ti, Zr, Hf, V, Cr, Mo, W, Mn, Tc, Fe, Rh, Ni), M3Al2B2 (M = Sc, T, Zr, Hf, Cr, Mn, Tc, Fe, Ru, Ni), M3AlB4 (M = Sc, Ti, Zr, Hf, V, Nb, Ta, Cr, Mo, W, Mn, Fe), and M4AlB6 (M = Sc, Ti, Zr, Hf, V, Nb, Ta, Cr, Mo). By comparing the formation energies of these MAB phases with those of their available competing binary M-B and M-Al, and ternary M-Al-B phases, we find that some of the Sc-, Ti-, V-, Cr-, Mo-, W-, Mn-, Tc-, and Fe-based MAB phases could be favorably synthesized under appropriate experimental conditions. In addition, by examining the strengths of various bonds in MAB phases via crystal orbital Hamilton population and spring constant calculations, we find that the B-B and then M-B bonds are stiffer than the M-Al and Al-B bonds. The different strengths between these bonds imply the etching possibility of Al atoms from MAB phases, consequently forming various 2D MB, M2B3, and M3B4 MBenes. Furthermore, we employ the nudged elastic band method to investigate the possibility of the structural phase transformation of the 2D MB MBenes into graphene-like boron sheets sandwiched between transition metals and find that the energy barrier of the transformation is less than 0.4 eV per atom.

Preventing ice formation and ice swift removal from the solid surface are essential in numerous application fields. Superhydrophobic coating is an effective way to delay the icing phenomenon. However, the superhydrophobic coating was wetted easily after icing-deicing cycles that led to the failure of anti-icing. In this study, a robust, amphiphobic coating consisted of fluorinated multiwalled carbon nanotubes (FMWCNTs) and commercial polyurethane was constructed by a simply spray process. Because of the addition of FMWCNTs, the coating demonstrated a good amphiphobic feature and highly efficient photothermal conversion, which endowed the coating surface with excellent deicing and defrosting characteristics under sunlight irradiation. In addition, self-cleaning and self-healing properties of the coating under sunlight ensured its efficient photothermal conversion and long service life. To further improve the photothermal deicing effect, a coating system containing a photothermal layer (P), thermal-conductive layer (C), and thermal-protective layer (P) was constructed. The heat generating from the photothermal layer can transfer the whole coating surface by the conductive layer, but with limited transmission to substrate materials by a thermal-protective layer. The coating system can still deice and defrost rapidly on the whole surface and only a small portion of photothermal coating was irradiated under extremely low temperature. The outdoor experiment has confirmed that the coating melted and removed snow rapidly in a winter environment. The multifunctional photothermal deicing coating may have a wide application in outdoor surrounding.

Graphene nanosheet (GN)/Al₂O₃ ceramics were prepared by hot press sintering with a significant improvement in both mechanical and electromagnetic properties.

As a member of the lead-halide perovskite family, inorganic perovskite CsPbBr3 exhibits excellent optical and electrical properties with higher stability to the environment. However, former efforts to obtain large-size CsPbBr3 single crystals with satisfactory quality using low temperature solution methods reached limited results. In this work, we have studied the growth of CsPbBr3 crystals using the antisolvent vapor-assisted crystallization (AVC) method. By adjusting the mole ratio of PbBr2 and CsBr, the phase diagram of the final products is acquired. Five regions are identified, including the Cs4PbBr6 single phase region, Cs4PbBr6 and CsPbBr3 two phases region, CsPbBr3 single phase region, CsPbBr3 and PbBr2·2[(CH3)2SO] metastable two phases region, and CsPbBr3 and PbBr2·2[(CH3)2SO] two phases region. Three methods are adopted to improve the size and crystalline quality of CsPbBr3. The growth rate is effectively tailored by diluting the antisolvent MeOH solution using DMSO to reduce the MeOH vapor pressure. Centimeter-size bright CsPbBr3 crystals have been obtained. The room temperature bandgap of CsPbBr3 is estimated at ∼2.29 eV by the transmission spectra. The photoluminescence spectra show two strong emission peaks, located at 530 and 555 nm, respectively, which are related to the free and bond excitons. The resistivity is as large as 2.1 × 109 Ω·cm. Hall effect measurements demonstrate the CsPbBr3 is p-type conductivity with a hole carrier concentration of 4.55 × 107 cm–3 and the mobility of 143 cm2 V–1 s–1. The resulting Au/CsPbBr3/Au device exhibits strong photoresponse to optical light, with an on–off ratio of two orders under a light emitting diode (∼1 mW/cm2) with a wavelength of 365–420 nm. Our research would shed more light on the growth and the photoresponse properties of CsPbBr3 crystals.

Graphene nanosheets filled BaTiO₃ ceramics with high-performance EMI shielding effectiveness, greater than 40 dB in the X-band at 1.5 mm thickness, were prepared <italic>via</italic> pressureless sintering.

A 3D hierarchical structure of MoSe₂/NiSe₂ exhibits superior HER activity because of more active sites and faster transfer of electrons.

“Side-chain-type” and crosslinkable quaternized polypropylene was prepared by heterogeneous Ziegler–Natta catalyst mediated polymerization for use in highly stable anion exchange membranes.

Abstract To tackle the increasing electromagnetic pollution, broadband electromagnetic wave (EMW) absorption materials are urgently needed. Toward this goal, traditional strategies resort to the construction of multicomponent dielectric/magnetic hybrid materials, including ternary, quaternary, or even more complicated systems. However, they always suffer from many intrinsic drawbacks in practical applications. Herein, a theory‐directed strategy is presented to design plainified EMW absorption materials (binary hybrids) via amplified interface effects, which are based on well‐designed multilayer alternating core‐shell nanostructures by chemical vapor deposition (CVD). A defect‐engineered CVD graphene (DG) core composed of graphitic open edges and in‐plane defects is used as a lossy phase. Correspondingly, a CVD Si 3 N 4 layer with nanometer thickness is used as an impedance matching shell. By optimizing the alternating numbers of DG/Si 3 N 4 units, enhanced interface polarization and strong frequency dispersion behavior of permittivity (especially the real part, ε′) are obtained, which helps the plainified binary hybrids to reach an effective absorption bandwidth (EAB) of 8.0 GHz at a thickness of 2.7 mm. Moreover, these plainified hybrids show excellent thermal and pH stability. Even after 1000 °C oxidation, for example, an EAB of 7.44 GHz coupling with a minimum reflection coefficient of −77.3 dB is still achieved.

High-sensitivity X-ray detectors made of solution grown CsPbBr₃ single crystals with high crystalline quality was reported in this work. The device with asymmetric electrodes configuration shows high sensitivity of 1256 μC Gy⁻¹ cm⁻².

Two-dimensional (2D) graphene-like nanomaterials show wide applications in the fields of nanodevices, sensors, energy materials, catalysis, drug delivery, bioimaging, and tissue engineering. Recently, many studies have been focused on the synthesis and application of 2D transition metal dichalcogenide (TMD) nanosheets for various biomedical applications. In particular, 2D TMD nanosheets exhibit great advantages for tumor imaging and therapy compared to some traditional nanomaterials due to their high specific surface area, good biocompatibility, easy modification, and ultrahigh light and heat conversion efficiency. In this review, we summarize the recent advances in the synthesis, modification, and photo/thermo-based tumor imaging and therapy of 2D TMD nanosheets. The important studies on tumor bioimaging with TMD nanosheets, such as X-ray computed tomography, magnetic resonance imaging, and photoacoustic imaging, are demonstrated and discussed. In another section, the physical photothermal and photodynamic therapies as well as the pharmacological therapy of tumors with TMD nanosheet-based nanohybrids are introduced. It is expected that this work will be valuable for readers to understand the synthesis and modification of TMD nanosheets to design novel 2D functional nanomaterials for photo/thermo-based tumor imaging and therapy in one aspect, and in another aspect will extend the applications of TMD-based nanomaterials in materials science, analytical science, electrocatalysis, tissue engineering, and others.

Niobium and aluminum co-doped TiO₂ ceramics, <italic>i.e.</italic>, (Nb_0.5Al_0.5)_xTi_1−xO₂ (<italic>x</italic> = 0, 0.01, 0.05, 0.1, 0.15, abbreviated as NAT100<italic>x</italic>) were synthesized <italic>via</italic> a solid-state reaction route.

The aligned one-dimensional channels found in covalent organic frameworks offer a unique space for energy storage. However, physical isolation of sulfur in the channels is not sufficient to prevent the shuttle of lithium-sulfide intermediates that eventually results in a poor performance of lithium-sulfur energy storage. Herein, we report a strategy based on imine-linked frameworks for addressing this shuttle issue by covalently engineering polysulfide chains on the pore walls. The imine linkages can trigger the polymerization of sulfur to form polysulfide chains and anchor them on the channel walls. The immobilized polysulfide chains suppress the shuttle effect and are highly redox active. This structural evolution induces multifold positive effects on energy storage and achieves improved capacity, sulfur accessibility, rate capability and cycle stability. Our results suggest a porous platform achieved by pore wall engineering for tackling key issues in energy storage.

An effective strategy of surface &amp; grain boundary co-passivation is demonstrated to access perovskite solar cells with 21.31% champion efficiency as well as a highly improved stability of less than 3% efficiency loss after 2500 hours at a humidity of 70%.

We for the first time report the application of a polymeric room-temperature molten salt in high efficiency and excellent stability inverted perovskite solar cells.