Encapsulation of Sulfur into N-Doped Porous Carbon Cages by a Facile, Template-Free Method for Stable Lithium-Sulfur Cathode.

Lithium-sulfur (Li-S) batteries with a high energy density and long lifespan are considered as promising candidates for next-generation electrochemical energy-storage devices. However, the sluggish redox kinetics of electrochemistry and high solubility of polysulfide during cycling render insufficient sulfur utilization and poor cycling stability. Herein, a facile, template-free procedure based on controlled pyrolysis of polydopamine vesicles is described to prepare N-doped porous carbon cages (NHSC) as a new sulfur host, which significantly improves both the sulfur utilization and cycling stability. As NHSC shows a high pore volume, continuous electron and ion transport paths, and good catalytic activity, encapsulation of S nanoparticles into NHSC endows the resulting S@NHSC electrode with a good energy storage capacity and exceptionally high electrochemical stability. Consequently, a Li-S cell with the S@NHSC as the cathode achieves a high initial capacity of 1280.7 mAh g-1 , and cycling stability over 500 cycles with the capacity decay as low as 0.0373% per cycle.

Electrostatic self-assembly endows cellulose paper with durable efficient flame retardancy and mechanical performance improvement.

Flameproof modification of paper can improve safety and application performance. However, traditional paper is prone to moisture absorption, resulting in significant reduction in flame retardant performance, even complete failure, greatly limiting the application environment. In order to achieve long-term flame retardant properties of paper, while avoiding the loss of physical properties caused by the introduction of flame retardants, in this work, a plant acid/phosphate and melamine formaldehyde coating (PyA/PA-MF) is prepared through electrostatic self-assembly for durable flame retardant performance of cellulose paper. Due to the electrostatic interaction, the paper surface become greatly rough with introduction of PyA/PA-MF, a uniform microsphere structure is formed on the surface of the paper cellulose, which effectively fix the phosphorus-containing groups. The oxygen index reaches 33 % and the carbon length was only 6.3 ± 0.2 cm, the pHRR and THR are decreased by 80 % and 73 %, respectively. After being immersed for 72 h, the oxygen index is still 31.4 % and carbon length is no more than 12 cm. mechanical property of modified paper is significant increased in the tensile strength (2.4 MPa) compared to the blank paper (1 MPa), as well as that the whiteness of the surface of the modified paper will not change. In summary, PyA/PA-MF endows paper long-term flame retardant performance while maintaining its basic performance.

Functional thermoelectric composite endows cellulose paper with superior fire safety.

Due to intrinsic defect of fire hazard security, improving the flame retardant capacity of paper is still insufficient in case of precombustion. Herein, we integrate the flame retardant with flame detection performance on the surface of paper, the restricts of graphene oxide (GO) are overcome between high thermoelectric performance and flexibility. A flexible lamellar thermoelectric composite (GO-LA-HP) is constructed through the co-assembly of GO, ascorbic acid (LA), and phenoxycycloposphazene (HP), lamellar GO-LA-HP avoid GO's toughness decline after modification, but also enhance fire sensitivity and flame resistance. The composite could significantly decrease the temperature rise stage (<150 °C), and trigger the fire-warning within 2 s. The hybrid coating composed of phytic acid/phosphoric acid (PyA/PA) and modified thermoelectric GO-LA-HP becomes excellent compatibility on the surface of the modified paper (GPP). GPP is able to extinguish itself immediately after leaving the fire in the vertical combustion, and display the excellent flame resistance. Furthermore, GPP's alarm signal could be timely generated as little as 3 s of contacting the flame, and the response time can exceed 600 s. According to the structure observation and analysis, the related synergistic fire detection reinforcing and flame-retardant mechanisms are also proposed and clarified.

Viscoelasticity­Controlled Relaxation in Wrinkling Surface for Multistage Time­Resolved Optical Information Encryption.

As counterfeit techniques continue to evolve, ensuring the security of conventional "static" encryption methods becomes increasingly challenging. Here, the viscoelasticity-controlled relaxation is introduced for the first time in a bilayer wrinkling system by regulating the density of hydrogen bond networks in polymer to construct a "dynamic" encryption material. The wrinkling surface can manipulate light during the dynamic relaxation process, exhibiting three stages with frosted glass, structural color, and mirror reflection. By regulating the viscoelasticity of skin layer through UV irradiation, the wavelength and the relaxation rate of the wrinkles can be controlled. As a result, dynamic wrinkling anti-counterfeiting patterns and time-resolved multistage information encryption are achieved. Crucially, the encryption material is developed as an anti-counterfeiting label for packing boxes in daily applications, allowing the encrypted information to be activated manually and identified by naked eyes, surpassing the existing time-resolved encryption materials in utilization potential. Besides, the dynamic hydrogen bond networks are extended to various dynamic interaction networks, demonstrating the versatility of the dynamic encryption strategy. This work not only provides an additional dimension for dynamic information encryption in daily practical use, but also offers theoretical guidance for the development of advanced optical anti-counterfeiting and smart display materials in the future.

Designed wrinkles for optical encryption and flexible integrated circuit carrier board.

Patterns on polymers usually have different mechanical properties as those of the substrates, causing deformation or distortion and even detachment of the patterns from the polymer substrates. Herein, we present a wrinkling strategy, which utilizes photolithography to define the area of stress distribution by light-induced physical crosslinking of polymers and controls diffusion of residual solvent to redistribute the stress and then offers the same material for patterns as substrate by thermal polymerization, providing uniform wrinkles without worrying about force relaxation. The strategy allows the recording and hiding of up to eight switchable images in one place that can be read by the naked eye without crosstalk, applying the wrinkled polymer for optical anti-counterfeiting. The wrinkled polyimide film was also utilized to act as a substrate for the creation of fine copper circuit by a full-additive process. It generates flexible integrated circuit (IC) carrier board with copper wire density of 400% higher than that of the state-of-the-art in industry while fulfilling the standards for industrialization.

Interfacial Wrinkling Structures Based on a Double Cross-Linking Strategy Enable a Dual-Mode Optical Information Encryption.

Surface wrinkling structures based on a bilayer system are widely employed in storing and encrypting specific optical information. However, constructing a stable wrinkling structure with high-level security remains an extensive challenge due to the delamination issue between the skin layer and the substrate. Herein, a double cross-linking strategy is introduced between a hydrogel layer doped with fluorescent molecules and polydimethylsiloxane to establish a stable interfacial wrinkling structure with dual-mode functionality, in which the light reflection of the wrinkles and fluorescence intensity of fluorescent molecules can be simultaneously regulated by the modulus ratio between the two layers. The spontaneous wrinkling structures with a physically unclonable function can enhance the photoluminescence emission intensity of the wrinkling area under ultraviolet radiation. Meanwhile, the skin layer constructed of acrylamide and acrylic acid copolymer protects the interfacial wrinkling patterns from the loss of a detailed structure for authentication due to external damage. The stable interfacial wrinkling structures with fluorescence can find potential applications in the fields of information storage and encryption.

Dendrimer Modification Strategy Based on the Understanding of the Photovoltaic Mechanism of a Perovskite Device under Full Sun and Indoor Light.

The wide-band-gap inorganic CsPbI2Br perovskite material provides a highly matched absorption range with the indoor light spectrum and is expected to be used in the fabrication of highly efficient indoor photovoltaic cells (IPVs) and self-powered low-power Internet of Things (IoT) sensors. However, the defects that cause nonradiative recombination and ion migration are assumed to form leakage loss channels, resulting in a severe impact on the open-circuit voltage (VOC) and the fill factor (FF) of IPVs. Herein, we introduce poly(amidoamine) (PAMAM) dendrimers with multiple passivation sites to fully repair the leakage channels in the devices, taking into account the characteristics of IPVs that are extremely sensitive to nonradiative recombination and shunt resistance. The as-optimized IPVs demonstrate a promising PCE of 35.71% under a fluorescent light source (1000 lux), with VOC increased from 0.99 to 1.06 V and FF improved from 75.21 to 84.39%. The present work provides insight into the photovoltaic mechanism of perovskites under full sun and indoor light, which provides guidance for perovskite photovoltaic technology with industrialization prospects.

Impermeable Atomic Layer Deposition for Sputtering Buffer Layer in Efficient Semi-Transparent and Tandem Solar Cells via Activating Unreactive Substrate.

Atomic layer deposition (ALD) turns out to be particularly attractive technology for the sputtering buffer layer when preparing the semi-transparent (ST) perovskite solar cells (PSCs) and the tandem solar cells. ALD process turns to be island growth when the substrate is unreactive with the ALD reactants, resulting in the pin-hole layer, which causes an adverse effect on anti-sputtering. Here, p-i-n structured PSCs with ALD SnOx as sputtering buffer layer are conducted. The commonly used electron transportation layer (ETL) PCBM in the p-i-n structured PVK solar cell is an unreactive substrate that prevents the layer-by-layer growth for the ALD SnOx . PCBM layer is activated by introducing reaction sites to form impermeable ALD layers. By introducing reaction sites/ALD SnOx as sputtering buffer layer, the authors succeed to fabricate ST-PSCs and perovskite/silicon (double-side polished) tandem solar cells with power conversion efficiency (PCE) of 20.25% and 23.31%, respectively. Besides, the unencapsulated device with reaction sites maintains more than 99% of the initial PCE after aging over 5100 h. This work opens a promising avenue to prepare impermeable layer for stable PSCs, ST-PSCs, tandem solar cells, and the related scale-up solar cells.

Interfacial engineering with carbon-graphite-Cu δ Ni1-δ O for ambient-air stable composite-based hole-conductor-free perovskite solar cells.

Ambient air atmosphere is inimical to organic-inorganic halide perovskites and organic hole transport materials, and is, thus, necessarily avoided during device fabrication. To solve this issue, it is highly desirable to design stable perovskite-based composites and device configurations. Here, fully ambient-air and antisolvent-free-processed, stable and all-inorganic metal-oxide selective contact hole-conductor-free perovskite solar cells (HCF-PSCs) based on perovskite-based composites with an interfacial engineering strategy are reported. The formation of perovskite-based composites by interfacial engineering with carbon-graphite-Cu δ Ni1-δ O not only improved interfacial contacts, charge extraction and transport but also passivated trap states of perovskite thin films and charge recombination at the interfaces. Thus, such perovskite composites with interfacial engineering-based HCF-PSCs without encapsulation showed excellent stability by sustaining 94% of initial PCE over 300 days under ambient conditions.

Tailoring the Vertical Morphology of Organic Films for Efficient Planar-Si/Organic Hybrid Solar Cells by Facile Nonpolar Solvent Treatment.

The optical and electrical properties of the blending organic film poly(3,4-ethylenedioxy-thiophene):poly(styrenesulfonate) (PEDOT:PSS) are strongly affected by its morphology, resulting in the performance variation in Si/organic hybrid solar cells. Here, a facile postsolvent treatment is used to tailor the vertical morphology of PEDOT:PSS by introducing a nonpolar solvent. X-ray photoelectron spectroscopy depth-profiling measurements show that the distribution of PEDOT and PSS on the surface of n-type Si can be changed by nonpolar solvent n-hexane (NHX) treatment, where more PSS aggregate at the bottom of the blend film and more PEDOT float up to the top, as compared with the reference sample. As a result, after NHX treatment, the average lifetime of the Si/organic films is increased from 152 µs for untreated samples to 248 µs for NHX-treated ones because of the better passivation effect of PSS on Si. Moreover, the transmission line model measurements indicate that the contact resistance (RC) of PEDOT:PSS film and the Ag electrode is decreased for better charge collection after NHX treatment. Eventually, the best power conversion efficiency (PCE) of 13.78% for NHX-treated planar solar cells is obtained, much higher than the PCE (with best of 12.78%) of reference devices without nonpolar solvent treatment. Our results provide a facile method to tailor the vertical morphology of the PEDOT:PSS in Si/organic hybrid solar cells.

Tailoring C60 for Efficient Inorganic CsPbI2 Br Perovskite Solar Cells and Modules.

Although inorganic perovskite solar cells (PSCs) are promising in thermal stability, their large open-circuit voltage (VOC ) deficit and difficulty in large-area preparation still limit their development toward commercialization. The present work tailors C60 via a codoping strategy to construct an efficient electron-transporting layer (ETL), leading to a significant improvement in VOC of the inverted inorganic CsPbI2 Br PSC. Specifically, tris(pentafluorophenyl)borane (TPFPB) is introduced as a dopant to lower the lowest unoccupied molecular orbital (LUMO) level of the C60 layer by forming a Lewis acidic adduct. The enlarged free energy difference provides a favorable enhancement in electron injection and thereby reduces charge recombination. Subsequently, a nonhygroscopic lithium salt (LiClO4 ) is added to increase electron mobility and conductivity of the film, leading to a reduction in the device hysteresis and facilitating the fabrication of a large-area device. Finally, the as-optimized inorganic CsPbI2 Br PSCs gain a champion power conversion efficiency (PCE) of 15.19%, with a stabilized power output (SPO) of 14.21% (0.09 cm2 ). More importantly, this work also demonstrates a record PCE of 14.44% for large-area inorganic CsPbI2 Br PSCs (1.0 cm2 ) and reports the first inorganic perovskite solar module with the excellent efficiency exceeding 12% (10.92 cm2 ) by a self-developed quasi-curved heating method.

The Glass-Transition Temperature of Supported PMMA Thin Films with Hydrogen Bond/Plasmonic Interface.

The interfacial effect is one of the significant factors in the glass-transition temperature (Tg) of the polymeric thin film system, competing against the free surface effect. Herein, the Tgs of poly (methyl methacrylate) (PMMA) films with different thicknesses and substrates are studied by fluorescence measurements, focusing on the influence of interfacial effects on the Tgs. The strong interaction between PMMA and quartz substrate leads to increased Tgs with the decreased thickness of the film. The plasmonic silver substrate causes enhanced fluorescence intensity near the interface, resulting in the delayed reduction of the Tgs with the increasing film thickness. Moreover, as a proof of the interface-dependent Tgs, hydrogen bonds of PMMA/quartz and molecules orientation of PMMA/silver are explored by the Raman spectroscopy, and the interfacial interaction energy is calculated by the molecular dynamics simulation. In this study, we probe the inter-relationship between the interfacial interactions arising from the different substrates and the Tg behavior of polymer thin films.

One-Pot Large-Scale Synthesis of Carbon Quantum Dots: Efficient Cathode Interlayers for Polymer Solar Cells.

Cathode interlayers (CILs) with low-cost, low-toxicity, and excellent cathode modification ability are necessary for the large-scale industrialization of polymer solar cells (PSCs). In this contribution, we demonstrated one-pot synthesized carbon quantum dots (C-dots) with high production to serve as efficient CIL for inverted PSCs. The C-dots were synthesized by a facile, economical microwave pyrolysis in a household microwave oven within 7 min. Ultraviolet photoelectron spectroscopy (UPS) studies showed that the C-dots possessed the ability to form a dipole at the interface, resulting in the decrease of the work function (WF) of cathode. External quantum efficiency (EQE) measurements and 2D excitation-emission topographical maps revealed that the C-dots down-shifted the high energy near-ultraviolet light to low energy visible light to generate more photocurrent. Remarkably improvement of power conversion efficiency (PCE) was attained by incorporation of C-dots as CIL. The PCE was boosted up from 4.14% to 8.13% with C-dots as CIL, which is one of the best efficiency for i-PSCs used carbon based materials as interlayers. These results demonstrated that C-dots can be a potential candidate for future low cost and large area PSCs producing.