Shenzhen Polytechnic University

Abstract We present an update on recently developed methodology and functionality in the computer program Local Orbital Basis Suite Toward Electronic‐Structure Reconstruction (LOBSTER) for chemical‐bonding analysis in periodic systems. LOBSTER is based on an analytic projection from projector‐augmented wave (PAW) density‐functional theory (DFT) computations (Maintz et al., J. Comput. Chem. 2013 , 34 , 2557), reconstructing chemical information in terms of local, auxiliary atomic orbitals and thereby opening the output of PAW‐based DFT codes to chemical interpretation. We demonstrate how LOBSTER has been improved by taking into account time‐reversal symmetry, thereby speeding up the DFT and LOBSTER calculations by a factor of 2. Over the recent years, the functionalities have also been continually expanded, including accurate projected densities of states (DOSs), crystal orbital Hamilton population (COHP) analysis, atomic and orbital charges, gross populations, and the recently introduced k ‐dependent COHP. The software is offered free‐of‐charge for non‐commercial research.

Tissue engineering has become a promising strategy for repairing damaged cartilage and bone tissue. Among the scaffolds for tissue-engineering applications, injectable hydrogels have demonstrated great potential for use as three-dimensional cell culture scaffolds in cartilage and bone tissue engineering, owing to their high water content, similarity to the natural extracellular matrix (ECM), porous framework for cell transplantation and proliferation, minimal invasive properties, and ability to match irregular defects. In this review, we describe the selection of appropriate biomaterials and fabrication methods to prepare novel injectable hydrogels for cartilage and bone tissue engineering. In addition, the biology of cartilage and the bony ECM is also summarized. Finally, future perspectives for injectable hydrogels in cartilage and bone tissue engineering are discussed.

Abstract Anodic oxygen evolution reaction (OER) is recognized as kinetic bottleneck in water electrolysis. Transition metal sites with high valence states can accelerate the reaction kinetics to offer highly intrinsic activity, but suffer from thermodynamic formation barrier. Here, we show subtle engineering of highly oxidized Ni 4+ species in surface reconstructed (oxy)hydroxides on multicomponent FeCoCrNi alloy film through interatomically electronic interplay. Our spectroscopic investigations with theoretical studies uncover that Fe component enables the formation of Ni 4+ species, which is energetically favored by the multistep evolution of Ni 2+ →Ni 3+ →Ni 4+ . The dynamically constructed Ni 4+ species drives holes into oxygen ligands to facilitate intramolecular oxygen coupling, triggering lattice oxygen activation to form Fe-Ni dual-sites as ultimate catalytic center with highly intrinsic activity. As a result, the surface reconstructed FeCoCrNi OER catalyst delivers outstanding mass activity and turnover frequency of 3601 A g metal −1 and 0.483 s −1 at an overpotential of 300 mV in alkaline electrolyte, respectively.

It is well documented that the traditional Fenton reagent (i.e., the combination of Fe(II) and H2O2) produces hydroxyl radical (•OH) under acidic conditions, while at near-neutral pH the reactive intermediate converts to ferryl ion (Fe(IV)) that can oxidize sulfoxides to produce corresponding sulfones, markedly differing from their •OH-induced products. However, it remains unclear whether Fe(IV) is generated in the Fe(II) activated peroxydisulfate (PDS) process, where sulfate radical (SO4•–) is long recognized as the dominant intermediate in literature. Here we demonstrated that SO4•– oxidized methyl phenyl sulfoxide (PMSO, a model sulfoxide) to produce biphenyl compounds rather than methyl phenyl sulfone (PMSO2). Interestingly, the formation of PMSO2 was observed when PMSO was treated by the Fe(II)/PDS system over a wide pH range, and the yields of PMSO2 were quantified to be ∼100% at acidic pH 3–5. The identification of Fe(IV) in the Fe(II)/PDS system could also reasonably explain the literature results on alcohol scavenging effect and ESR spectra analysis. Further, a Fe(IV)-based kinetic model was shown to accurately simulate the experimental data. This work urges re-evaluation of the Fe(II)/PDS system for environmental decontamination, given that Fe(IV) would have different reactivity toward environmental contaminants compared with SO4•– and/or •OH.

The electrical and optical measurements, in combination with density functional theory calculations, show distinct layer-dependent semiconductor-to-semimetal evolution of 2D layered PtSe2. The high room-temperature electron mobility and near-infrared photo­response, together with much better air-stability, make PtSe2 a versatile electronic 2D layered material. As a service to our authors and readers, this journal provides supporting information supplied by the authors. Such materials are peer reviewed and may be re-organized for online delivery, but are not copy-edited or typeset. Technical support issues arising from supporting information (other than missing files) should be addressed to the authors. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.

Lattice oxygen redox chemistry in solid-state electrocatalysts rationalizes the remarkable OER activity by lattice oxygen-mediated mechanism. Here we elucidate the fundamental principle of this mechanism and summarize recently related developments.

Non-fullerene acceptors based organic solar cells represent the frontier of the field, owing to both the materials and morphology manipulation innovations. Non-radiative recombination loss suppression and performance boosting are in the center of organic solar cell research. Here, we developed a non-monotonic intermediate state manipulation strategy for state-of-the-art organic solar cells by employing 1,3,5-trichlorobenzene as crystallization regulator, which optimizes the film crystallization process, regulates the self-organization of bulk-heterojunction in a non-monotonic manner, i.e., first enhancing and then relaxing the molecular aggregation. As a result, the excessive aggregation of non-fullerene acceptors is avoided and we have achieved efficient organic solar cells with reduced non-radiative recombination loss. In PM6:BTP-eC9 organic solar cell, our strategy successfully offers a record binary organic solar cell efficiency of 19.31% (18.93% certified) with very low non-radiative recombination loss of 0.190 eV. And lower non-radiative recombination loss of 0.168 eV is further achieved in PM1:BTP-eC9 organic solar cell (19.10% efficiency), giving great promise to future organic solar cell research.

Platinum disulfide (PtS2), a new member of the group-10 transition-metal dichalcogenides, is studied experimentally and theoretically. The indirect bandgap of PtS2 can be drastically tuned from 1.6 eV (monolayer) to 0.25 eV (bulk counterpart), and the interlayer mechanical coupling is almost isotropic. It can be explained by strongly interlayer interaction from the pz orbital hybridization of S atoms. As a service to our authors and readers, this journal provides supporting information supplied by the authors. Such materials are peer reviewed and may be re-organized for online delivery, but are not copy-edited or typeset. Technical support issues arising from supporting information (other than missing files) should be addressed to the authors. Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.

Abstract Noise pollution has become a significant global problem in recent years. Unfortunately, conventional acoustic materials cannot offer substantial improvements in noise reduction. However, acoustic metamaterials are providing new solutions for controlling sound waves, and have huge potential for mitigating noise propagation in particular. Recently, owing to the rapid development of acoustic metamaterials, metamaterials for acoustic noise reduction have drawn the attention of researchers worldwide. These metamaterials are often both light and compact, and are excellent at reducing low‐frequency noise, which is difficult to control with conventional acoustic materials. Recent progress has illustrated that acoustic metamaterials effectively control sound waves, and optimizing their structure can enable functionality based on new physical phenomena. This review introduces the development of acoustic metamaterials, and summarizes the basic classification, underlying physical mechanism, application scenarios, and emerging research trends for both passive and active noise‐reduction metamaterials. Focusing on noise reduction, the shortcomings of current technologies are discussed, and future development trends are predicted. As our knowledge in this area continues to expand, it is expected that acoustic metamaterials will continue to improve and find more practical applications in emerging fields in the future.

Tremendous efforts have been devoted to the synthesis and application of two-dimensional (2D) nanomaterials due to their extraordinary and unique properties in electronics, photonics, catalysis, etc., upon exfoliation from their bulk counterparts. One of the greatest challenges that scientists are confronted with is how to produce large quantities of 2D nanomaterials of high quality in a commercially viable way. This review summarizes the state-of-the-art of the production of 2D nanomaterials using liquid-based direct exfoliation (LBE), a very promising and highly scalable wet approach for synthesizing high quality 2D nanomaterials in mild conditions. LBE is a collection of methods that directly exfoliates bulk layered materials into thin flakes of 2D nanomaterials in liquid media without any, or with a minimum degree of, chemical reactions, so as to maintain the high crystallinity of 2D nanomaterials. Different synthetic methods are categorized in the following, in which material characteristics including dispersion concentration, flake thickness, flake size and some applications are discussed in detail. At the end, we provide an overview of the advantages and disadvantages of such synthetic methods of LBE and propose future perspectives.

Abstract Palladium diselenide (PdSe 2 ), a thus far scarcely studied group‐10 transition metal dichalcogenide has exhibited promising potential in future optoelectronic and electronic devices due to unique structures and electrical properties. Here, the controllable synthesis of wafer‐scale and homogeneous 2D PdSe 2 film is reported by a simple selenization approach. By choosing different thickness of precursor Pd layer, 2D PdSe 2 with thickness of 1.2–20 nm can be readily synthesized. Interestingly, with the increase in thickness, obvious redshift in wavenumber is revealed by Raman spectroscopy. Moreover, in accordance with density functional theory (DFT) calculation, optical absorption and ultraviolet photoemission spectroscopy (UPS) analyses confirm that the PdSe 2 exhibits an evolution from a semiconductor (monolayer) to semimetal (bulk). Further combination of the PdSe 2 layer with Si leads to a highly sensitive, fast, and broadband photodetector with a high responsivity (300.2 mA W −1 ) and specific detectivity (≈10 13 Jones). By decorating the device with black phosphorus quantum dots, the device performance can be further optimized. These results suggest the as‐selenized PdSe 2 is a promising material for optoelectronic application.

To reduce the dependence on oil and environmental pollution, the development of electric vehicles has been accelerated in many countries. The implementation of EVs, especially battery electric vehicles, is considered a solution to the energy crisis and environmental issues. This paper provides a comprehensive review of the technical development of EVs and emerging technologies for their future application. Key technologies regarding batteries, charging technology, electric motors and control, and charging infrastructure of EVs are summarized. This paper also highlights the technical challenges and emerging technologies for the improvement of efficiency, reliability, and safety of EVs in the coming stages as another contribution.

Natural products, and especially the active ingredients found in traditional Chinese medicine (TCM), have a thousand-year-long history of clinical use and a strong theoretical basis in TCM. As such, traditional remedies provide shortcuts for the development of original new drugs in China, and increasing numbers of natural products are showing great therapeutic potential in various diseases. This paper reviews the molecular mechanisms of action of natural products from different sources used in the treatment of inflammatory diseases and cancer, introduces the methods and newly emerging technologies used to identify and validate the targets of natural active ingredients, enumerates the expansive list of TCM used to treat inflammatory diseases and cancer, and summarizes the patterns of action of emerging technologies such as single-cell multiomics, network pharmacology, and artificial intelligence in the pharmacological studies of natural products to provide insights for the development of innovative natural product-based drugs. Our hope is that we can make use of advances in target identification and single-cell multiomics to obtain a deeper understanding of actions of mechanisms of natural products that will allow innovation and revitalization of TCM and its swift industrialization and internationalization.

Abstract Metal halide perovskites (MHPs), emerging as innovative and promising semiconductor materials with prominent optoelectronic properties, has been pioneering a new era of light management (ranging from emission, absorption, modulation, to transmission) for next-generation optoelectronic technology. Notably, the exploration of fundamental characteristics of MHPs and their devices is the main research theme during the past decade, while in the next decade, it will be primarily critical to promote their implantation in the next-generation optoelectronics. In this review, we first retrospect the historical research milestones of MHPs and their optoelectronic devices. Thereafter, we introduce the origin of the unique optoelectronic features of MHPs, based on which we highlight the tunability of these features via regulating the phase, dimensionality, composition, and geometry of MHPs. Then, we show that owing to the convenient property control of MHPs, various optoelectronic devices with target performance can be designed. At last, we emphasize on the revolutionary applications of MHPs-based devices on the existing optoelectronic systems. This review demonstrates the key role of MHPs played in the development of modern optoelectronics, which is expected to inspire the novel research directions of MHPs and promote the widespread applications of MHPs in the next-generation optoelectronics.

Iron as an important element plays crucial roles in various physiological and pathological processes. Iron metabolism behaves in systemic and cellular two levels that usually are in balance conditions. The disorders of the iron metabolism balances relate with many kinds of diseases including Alzheimer's disease, osteoporosis and various cancers. In systemic iron metabolism that is regulated by hepcidin-ferroportin axis, plasma iron is bound with transferrin (TF) which has two high-affinity binding sites for ferric iron. The generic cellular iron metabolism consists of iron intake, utilization and efflux. During the iron intake process in generic cells, transferrin receptors (TFRs) act as the most important receptor mediated controls. TFR1 and TFR2 are two subtypes of TFRs those bind with iron-transferrin complex to facilitate iron into cells. TFR1 is ubiquitously expressed on the surfaces of generic cells, whereas TFR2 is specially expressed in liver cells. TFR1 has attracted more attention than TFR2 by having diverse functions in both invertebrates and vertebrates. Recently reports showed that TFR1 involved in many kinds of diseases including anemia, neurodegenerative diseases and cancers. Most importantly, TFR1 has been verified to be abnormally expressed in various cancers. Some experimental and clinical drugs and antibodies targeting TFR1 have showed strong anti-tumor effects, herein TFR1 probably become a potential molecular target for diagnosis and treatment for cancer therapy. This paper reviewed the research progresses of the roles of TFR1 in the tumorigenesis and cancer progression, the regulations of TFR1, and the therapeutic effects of targeting TFR1 on many kinds of cancers.

Abstract Adsorptive separation of olefin/paraffin mixtures by porous solids can greatly reduce the energy consumption associated with the currently employed cryogenic distillation technique. Here, the complete separation of propane and propylene by a designer microporous metal–organic framework material is reported. The compound, Y 6 (OH) 8 (abtc) 3 (H 2 O) 6 (DMA) 2 (Y‐abtc, abtc = 3,3′,5,5′‐azobenzene‐tetracarboxylates; DMA = dimethylammonium), is rationally designed through topology‐guided replacement of inorganic building units. Y‐abtc is both thermally and hydrothermally robust, and possesses optimal pore window size for propane/propylene separation. It adsorbs propylene with fast kinetics under ambient temperature and pressure, but fully excludes propane, as a result of selective size exclusion. Multicomponent column breakthrough experiments confirm that polymer‐grade propylene (99.5%) can be obtained by this process, demonstrating its true potential as an alternative sorbent for efficient separation of propane/propylene mixtures.

The removal of carbon dioxide (CO2) from acetylene (C2H2) is a critical industrial process for manufacturing high-purity C2H2. However, it remains challenging to address the tradeoff between adsorption capacity and selectivity, on account of their similar physical properties and molecular sizes. To overcome this difficulty, here we report a novel strategy involving the regulation of a hydrogen-bonding nanotrap on the pore surface to promote the separation of C2H2/CO2 mixtures in three isostructural metal–organic frameworks (MOFs, named MIL-160, CAU-10H, and CAU-23, respectively). Among them, MIL-160, which has abundant hydrogen-bonding acceptors as nanotraps, can selectively capture acetylene molecules and demonstrates an ultrahigh C2H2 storage capacity (191 cm3 g–1, or 213 cm3 cm–3) but much less CO2 uptake (90 cm3 g–1) under ambient conditions. The C2H2 adsorption amount of MIL-160 is remarkably higher than those for the other two isostructural MOFs (86 and 119 cm3 g–1 for CAU-10H and CAU-23, respectively) under the same conditions. More importantly, both simulation and experimental breakthrough results show that MIL-160 sets a new benchmark for equimolar C2H2/CO2 separation in terms of the separation potential (Δqbreak = 5.02 mol/kg) and C2H2 productivity (6.8 mol/kg). In addition, in situ FT-IR experiments and computational modeling further reveal that the unique host–guest multiple hydrogen-bonding interaction between the nanotrap and C2H2 is the key factor for achieving the extraordinary acetylene storage capacity and superior C2H2/CO2 selectivity. This work provides a novel and powerful approach to address the tradeoff of this extremely challenging gas separation.

Large-scale synthesis of two-dimensional (2D) materials is one of the significant issues for fabricating layered materials into practical devices. As one of the typical III–VI semiconductors, InSe has attracted much attention due to its outstanding electrical transport property, attractive quantum physics characteristics, and dramatic photoresponse when it is reduced to atomic scale. However, scalable synthesis of single phase 2D InSe has not yet been achieved so far, greatly hindering further fundamental studies and device applications. Here, we demonstrate the direct growth of wafer-scale layered InSe nanosheets by pulsed laser deposition (PLD). The obtained InSe layers exhibit good uniformity, high crystallinity with macro texture feature, and stoichiometric growth by in situ precise control. The characterization of optical properties indicates that PLD grown InSe nanosheets have a wide range tunable band gap (1.26–2.20 eV) among the large-scale 2D crystals. The device demonstration of field-effect transistor shows the n-type channel feature with high mobility of 10 cm2 V–1 s–1. Upon illumination, InSe-based phototransistors show a broad photoresponse to the wavelengths from ultraviolet to near-infrared. The maximum photoresponsivity attains 27 A/W, plus a response time of 0.5 s for the rise and 1.7 s for the decay, demonstrating the strong and fast photodetection ability. Our findings suggest that the PLD grown InSe would be a promising choice for future device applications in the 2D limit.

In the past few years, insensitive attentions have been drawn to wearable and flexible energy storage devices/systems along with the emergence of wearable electronics. Much progress has been achieved in developing flexible electrochemical energy storage devices with high end‐use performance. However, challenges still remain in well balancing the electrochemical properties, mechanical properties, and the processing technologies. In this review, a specific perspective on the development of textile‐based electrochemical energy storage devices (TEESDs), in which textile components and technologies are utilized to enhance the energy storage ability and mechanical properties of wearable electronic devices, is provided. The discussion focuses on the material preparation and characteristics, electrode and device fabrication strategies, electrochemical performance and metrics, wearable compatibility, and fabrication scalability of TEESDs including textile‐based supercapacitors and lithium‐ion batteries.

Hole-transporting layers (HTLs) are an essential component in inverted, p-i-n perovskite solar cells (PSCs) where they play a decisive role in extraction and transport of holes, surface passivation, perovskite crystallization, device stability, and cost. Currently, the exploration of efficient, stable, highly transparent and low-cost HTLs is of vital importance for propelling p-i-n PSCs toward commercialization. Compared to their inorganic counterparts, organic HTLs offer multiple advantages such as a tunable bandgap and energy level, easy synthesis and purification, solution processability, and overall low cost. Here, recent progress of organic HTLs, including conductive polymers, small molecules, and self-assembled monolayers, as utilized in inverted PSCs is systematically reviewed and summarized. Their molecular structure, hole-transport properties, energy levels, and relevant device properties and resulting performances are presented and analyzed. A summary of design principles and a future outlook toward highly efficient organic HTLs in inverted PSCs is proposed. This review aims to inspire further innovative development of novel organic HTLs for more efficient, stable, and scalable inverted PSCs.