Gradient “Single-Crystal” Li-Rich Cathode Materials for High-Stable Lithium-Ion Batteries

As one of the high-energy cathode materials of lithium-ion batteries (LIBs), lithium-rich-layered oxide with “single-crystal” characteristic (SC-LLO) can effectively restrain side reactions and cracks due to the reduced inner boundaries and enhanced mechanical stabilities. However, there are still high challenges for SC-LLO with diverse performance requirements, especially on their cycle stability improvement. Herein, a novel concentration gradient “single-crystal” LLO (GSC-LLO), with gradually decreasing Mn and increasing Ni contents from center to surface, is designed and prepared by combining co-precipitation and molten-salt sintering methods, yielding a capacity retention of 97.6% and an energy density retention of 95.8% within 100 cycles at 0.1 C. The enhanced performance is mostly attributed to the gradient-induced stabilized structure, free of cracks and less spinel-like structure formation after long-term cycling. Furthermore, the gradient design is also beneficial to the safety of LLOs as suggested by the improved thermal stability and reduced gas release. This study provides an effective strategy to prepare high-energy, high-stability, and high-safety LLOs for advanced LIBs.     

Exploring a Stable and Dense 3D Lead Chloride Hybrid with Emission of Self-Trapped Excitons toward X-Ray Scintillation

The exceptional photophysical properties of 3D organic–inorganic lead halide hybrids (OILHs) endow their significant potential for usage in optoelectronics, which has sparked intense research on novel 3D OILHs and associated applications. However, constructing new 3D OILHs based on large organic cations suffers from tough challenges due to the limitation of the Goldschmidt tolerance factor rule, let alone further explorations of their practical applications. Herein, a brand-new 3D lead chloride hybrid, (1MPZ)Pb₄Cl₁₀·H₂O ( 1 , 1MPZ = 1-methylpiperazine) is reported, featuring a dense 3D lead chloride framework made of the corner-, edge-, and face-shared lead chloride polyhedra. 1 presents a broadband white light emission with a large Stokes shift and a nanosecond photoluminescence lifetime, which originates from radiative recombination of self-trapped excitons (STEs) induced by the highly distorted structure. Such a reabsorption-free and fast-decayed STEs emission coupling with the dense 3D architecture further enables 1 with effective X-ray scintillation with good sensitivity. Impressively, 1 also shows superior environmental and radiation stability. This study provides a new 3D OILH with appealing luminescence, not only expanding the 3D OILH family but also inspiring the exploitation of their optoelectronic applications.     

19.28% Efficiency and Stable Polymer Solar Cells Enabled by Introducing an NIR-Absorbing Guest Acceptor

Here, a near-infrared (NIR)-absorbing small-molecule acceptor (SMA) Y-SeNF with strong intermolecular interaction and crystallinity is developed by combining selenophene-fused core with naphthalene-containing end-group, and then as a custom-tailor guest acceptor is incorporated into the binary PM6:L8-BO host system. Y-SeNF shows a 65 nm red-shifted absorption compared to L8-BO. Thanks to the strong crystallinity and intermolecular interaction of Y-SeNF, the morphology of PM6:L8-BO:Y-SeNF can be precisely regulated by introducing Y-SeNF, achieving improved charge-transporting and suppressed non-radiative energy loss. Consequently, ternary polymer solar cells (PSCs) offer an impressive device efficiency of 19.28% with both high photovoltage (0.873 V) and photocurrent (27.88 mA cm⁻²), which is one of the highest efficiencies in reported single-junction PSCs. Notably, ternary PSC has excellent stability under maximum-power-point tracking for even over 200 h, which is better than its parental binary devices. The study provides a novel strategy to construct NIR-absorbing SMA for efficient and stable PSCs toward practical applications.     

Marine-Derived Hydrogels for Biomedical Applications

Marine organisms provide novel and broad sources for the preparations and applications of biomaterials. Since the urgent requirement of bio-hydrogels to mimic tissue extracellular matrix (ECM), the natural biomacromolecule hydrogels derived from marine sources have received increasing attention. Benefiting from their outstanding bioactivity and biocompatibility, many attempts have been made to reconstruct ECM components by applying marine-derived natural hydrogels. Moreover, marine hydrogels have been successfully applied in biomedicine by means of microfluidics, electrospray, and bioprinting. In this review, the classification and characteristics of marine-derived hydrogels are summarized. In particular, their role in the development of biomaterials is also introduced. Then, the recent advances in bio-fabrication strategies for various hydrogel materials are focused upon. Besides, the influences of hydrogel types on their functions in biomedical applications are discussed in depth. Finally, critical reflections on the limitations and future development of marine-derived hydrogels are presented.     

Optimizing the Oxygen-Catalytic Performance of Zn–Mn–Co Spinel by Regulating the Bond Competition at Octahedral Sites

By using the more electro-negative Mn³⁺ ion to partially replace Co³⁺ at the octahedral site of spinel ZnCo₂O₄, i.e., forming ternary Zn–Mn–Co spinel oxide, the electrocatalytic oxygen reduction/evolution activity is found to be significantly increased. Considering the physical characterization and theoretical calculations, it demonstrated that the bond competition played a key role in regulating the cobalt valence state and the electrocatalytic activity. The partial replacement of octahedral-site-occupied Co³⁺ by Mn³⁺ can effectively modulate the adjacent Co–O bond and induce the Jahn–Teller effect, thus changing the originally stable crystal structure and optimizing the binding strength between the active center and reaction intermediates. Certainly, the Mn-substituted ZnMn_1.4Co_0.6O₄/NCNTs exhibit higher electrocatalytic oxygen reduction reaction (ORR) activity than that of ZnCo₂O₄/NCNTs and ZnMn₂O₄/NCNTs, supporting that the Co–O bond covalency determines the ORR activity of spinel ZnCo₂O₄. This study offers the competition between adjacent Co–O and Mn–O bonds via the B_Oh–O–B_Oh edge-sharing geometry. The ion substitution at octahedral sites by less electronegative cations can be a new and effective way to improve the electrocatalytic performance of cobalt-based spinel oxides.     

Hydrofluoric Acid-Removable Additive Optimizing Electrode Electrolyte Interphases with Li+ Conductive Moieties for 4.5 V Lithium Metal Batteries

High-voltage lithium metal batteries (LMBs) are capable to achieve the increasing energy density. However, their cycling life is seriously affected by unstable electrolyte/electrode interfaces and capacity instability at high voltage. Herein, a hydrofluoric acid (HF)-removable additive is proposed to optimize electrode electrolyte interphases for addressing the above issues. N, N-dimethyl-4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl) aniline (DMPATMB) is used as the electrolyte additive to induce PF₆⁻ decomposition to form a dense and robust LiF-rich solid electrolyte interphase (SEI) for suppressing Li dendrite growth. Moreover, DMPATMB can help to form highly Li⁺ conductive Li₃N and LiBO₂, which can boost the Li⁺ transport across SEI and cathode electrolyte interphase (CEI). In addition, DMPATMB can scavenge traced HF in the electrolyte to protect both SEI and CEI from the corrosion. As expected, 4.5 V Li|| LiNi_0.6Co_0.2Mn_0.2O₂ batteries with such electrolyte deliver 145 mAh g⁻¹ after 140 cycles at 200 mA g⁻¹. This work provides a novel insight into high-voltage electrolyte additives for LMBs.     

2D MoN1.2-rGO Stacked Heterostructures Enabled Water State Modification for Highly Efficient Interfacial Solar Evaporation

Improving interfacial solar evaporation performance is crucial for the practical application of this technology in solar-driven seawater desalination. Lowering evaporation enthalpy is one of the most promising and effective strategies to significantly improve solar evaporation rate. In this study, a new pathway to lower vaporization enthalpy by introducing heterogeneous interactions between hydrophilic hybrid materials and water molecules is developed. 2D MoN_1.2 nanosheets are synthesized and integrated with rGO nanosheets to form stacked MoN_1.2-rGO heterostructures with massive junction interfaces for interfacial solar evaporation. Molecular dynamics simulation confirms that atomic thick 2D MoN_1.2 and rGO in the MoN_1.2-rGO heterostructures simultaneously interact with water molecules, while the interactions are remarkably different. These heterogeneous interactions cause an imbalanced water state, which easily breaks the hydrogen bonds between water molecules, leading to dramatically lowered vaporization enthalpy and improved solar evaporation rate (2.6 kg m⁻² h⁻¹). This study provides a promising strategy for designing 2D-2D heterostructures to regulate evaporation enthalpy to improve solar evaporate rate for clean water production.     

Piezoelectric Nanostructured Surface for Ultrasound-Driven Immunoregulation to Rescue Titanium Implant Infection

Treating bacterial biofilm infections on implanted materials remains challenging in clinical practice, as bacteria can be resistant by weakening the host defense from immune cells like macrophages. Herein, a metal-piezoelectric hetero-nanostructure with mechanical energy-driven antimicrobial property is in situ constructed on the Ti implant. Under ultrasonic irradiation, the formed piezotronic Ti (piezoTi) can promote the generation of reactive oxygen species (ROS) by facilitating local charge transfer at the surface, thus leading to piezodynamic killing of Staphylococcus aureus (S. aureus) while downregulating biofilm-forming genes. In addition, the stimulated macrophages on piezoTi display potent phagocytosis and anti-bacterial activity through the activation of PI3K-AKT and MAPK pathway. As a demonstration, one-time ultrasound irradiation of piezoTi pillar implanted in an osteomyelitis model efficiently eliminates the S. aureus biofilm infection and rescues the implant with enhanced osteointegration. By the synergistic effect of ultrasound-driven piezodynamic therapy and immuno-regulation, the proposed piezoelectric nanostructured surface can endow Ti implants with highly efficient antibacterial performance in an antibiotic-free, noninvasive, and on-demand manner.     

A Dual-Mode Electrochromic Platform Integrating Zinc Anode-Based and Rocking-Chair Electrochromic Devices

The complementary electrochromic device, where the optical transmittance changes upon the flow of cations back and forth between anodic and cathodic electrodes, operates in a rocking-chair fashion if it can inherently self-discharge. Herein, the first demonstration of a dual-mode electrochromic platform having self-coloring and self-bleaching characteristics is reported, which is realized by sandwiching zinc metal within a newly-designed Prussian blue (PB)-WO₃ rocking-chair type electrochromic device. It is demonstrated that the redox potential differences between the zinc metal and the WO₃/PB electrodes endow the self-color-switching of these electrodes. By employing a hybrid electrolyte of Zn²⁺/K⁺, it is further shown that the colored PB-WO₃ rocking-chair device is capable of spontaneously bleaching when the anodic and cathodic electrodes are coupled. This dual-mode light-control strategy enables the electrochromic devices to exhibit four distinct optical states with the highest optical contrast of 72.6% and fast switching times (<5 s for the bleaching/coloration processes). Furthermore, the built-in voltage of the dual-mode electrochromic devices not only promotes energy efficiency, but also augments the bistability of the devices. It is envisioned that the broad implication of the present platform is in the development of self-powered smart windows, colorful displays, optoelectronic switches, and optical sensors.     

High-Performing Quasi-2D Perovskite Photodetectors with Efficient Charge Transport Network Built from Vertically Orientated and Evenly Distributed 3D-Like Phases

Quasi-two-dimensional (Q-2D) perovskites are emerging as one of the most promising materials for photodetectors. However, a significant challenge to Q-2D perovskites for photodetection is their insufficient charge transport ability, which is mainly attributed to their hybrid low-dimensional n-phase structure. This study demonstrates that evenly-distributed 3D-like phases with vertical orientation throughout the film can greatly facilitate charge transport and suppress charge recombination, outperforming the prevalent phase structure with a vertical dimension gradient. Based on such a phase structure, a Q-2D Ruddlesden−Popper perovskite self-powered photodetector achieving a combination of exceptional figures-of-merit is realized, including a responsivity of 0.45 AW⁻¹, a peak specific detectivity of 2.3 × 10¹³ Jones, a 156 dB linear dynamic range, and a rise/fall time of 2.89 µs/1.93 µs. The desired phase structure is obtained by utilizing a double-hole transport layer (HTL), combining hydrophobic PTAA and hydrophilic PEDOT: PSS. Besides, the dependence of the hybrid low-dimensional phase structure is also identified on the surface energy of the buried HTL substrate. This study gives insight into the correlation between Q-2D perovskites’ phase structure and performance, providing a valuable design guide for Q-2D perovskite-based photodetectors.