High-Compressive, Elastic, and Wearable Cellulose Nanofiber-Based Carbon Aerogels for Efficient Electromagnetic Interference Shielding.

Developing excellent electromagnetic interference (EMI) shielding materials with robust EMI shielding efficiency (SE), high mechanical performance, and multifunctionality is imperative. Carbon materials are well recognized as promising alternatives for high-performance EMI shielding, but their high brittleness greatly hampers their applications. In this work, a cellulose nanofiber/reduced graphene oxide-glucose carbon aerogel (C-CNFs/rGO-glu) with high compression, elasticity, and excellent EMI shielding performance was fabricated by directional freeze-drying followed by carbonization. Specifically, the height and stress retention are 88% and 90.9%, respectively, after 100 cycles of compression release at a high strain of 70%. The electromagnetic shielding effectiveness of the aerogels reached 67.5 dB and presented an absorption-dominant shielding mechanism with a 97.5% absorption loss ratio. Further, the carbon aerogel could capture subtle electrical signals to monitor different human behaviors and showed excellent heat insulation and infrared stealth performance.

Wood aerogels decorated amino-functionalized MIL-101(Cr) as efficient filter for multistage purification of wastewater.

Exploring novel water purifier to efficiently remove heavy metal ions from the wastewater is of vital importance. Inspired by the hierarchical structure of natural wood and the chelation of amino group, a high-efficiency water purifier with ethylenediamine functionalized MIL-101(Cr) octahedrons anchored on the wood aerogel (MIL-101(Cr)-ED/WA) was constructed. Benefiting from the two-pronged approach with the hierarchical structure of the wood aerogel frame for multistage filtration and the -NH2 that capable of chelation with metal ions, the fabricated MIL-101(Cr)-ED/WA exhibits excellent water purification performances, and its adsorption capacity of toxic Pb2+ ions could reach up to 6.46 mmol g-1. Furthermore, it demonstrates superior recyclability without secondary pollution and is also suitable for simultaneous treatment of multiple metal species. In general, this work will broaden the utilization of wood-based structural engineering materials in the treatment of heavy metal wastewater.

High-Performance Quasi-Solid-State Lithium-Sulfur Battery with a Controllably Solidified Cathode-Electrolyte Interface.

Lithium-sulfur batteries are considered a promising "beyond Li-ion" energy storage technology. Currently, the practical realization of Li-S batteries is plagued by rapid electrochemical failure of S cathodes due to aggravated polysulfide dissolution and shuttle in the conventional liquid ether-based electrolytes. A gel polymer electrolyte obtained by in situ polymerization of liquid electrolyte solvent at the cathode-electrolyte interface has been proven an effective strategy to prevent polysulfide shuttle. However, notably reduced polysulfide solubility in the gel electrolyte leads to enrichment of poorly conductive sulfide species, which hinders charge migration across the interface and therefore accounts for retarded polysulfide conversion and a low capacity/energy output of batteries. Here, we show that thioacetamide, as a cathode additive, inhibits interfacial polymerization of ether molecules while assisting dissolution of polysulfides and Li2S at the cathode/electrolyte interface. In this way, a layer of liquid, sulfide-soluble electrolyte is preserved between the highly gelled electrolyte and the S particle surface, avoiding interfacial sulfide accumulation and improving polysulfide conversion kinetics. A Li-S battery with the controllably solidified interface demonstrates, without adding other performance-boosting agents or catalysts, a high reversible capacity, a long cycle life, and a favorable rate performance, showing promises for the next-generation storage applications.

ε-Poly-l-lysine-modified natural silk fiber membrane wound dressings with improved antimicrobial properties.

Many complex diseases, such as bacterial infections, frequently accompany cutaneous wound healing, adding to the difficulty of clinical wound management. Consequently, in addition to displaying strong biocompatibility and actively promoting wound healing, an optimal wound dressing should also possess antimicrobial qualities to address issues with bacterial infection. This paper developed natural silk fiber (SF) membranes (also known as a flat silk cocoon (FSC)) with antimicrobial properties as a dressing for skin wounds. By changing the spinning tools and environment of silkworm larvae, a novel natural SF membrane with a cocoon structure and controllable size was prepared. The functional SF membranes were obtained via a hot press process and grafted with ε-Poly-l-lysine (EPL). The results showed that the SF membrane dressing was adjustable in size with a similar structure to the extracellular matrix (ECM), displaying inherent mechanical properties, excellent antimicrobial qualities, and biocompatibility. In vivo experiments using a full-thickness skin defect model indicated that EPL-modified SF membranes significantly promoted the rate of wound healing, exhibiting thicker granulation tissue and higher collagen disposition than commercial dressings (Tegaderm™ film). Therefore, the excellent mechanical qualities and cytocompatibility of the antimicrobial EPL-modified SF membranes substantially promote their potential application as a chronic wound dressing.

Nitrogen Disturbance Awakening the Intrinsic Activity of Nickel Phosphide for Boosted Hydrogen Evolution Reaction.

Invited for this month's cover is the group of Qingfeng Sun at the Zhejiang A&F University. The image shows that the N-doped Ni2 P exhibits excellent electrocatalytic activity for hydrogen evolution reaction (HER). The Research Article itself is available at 10.1002/cssc.202200072.

N-Doped sp2 /sp3 Carbon Derived from Carbon Dots to Boost the Performance of Ruthenium for Efficient Hydrogen Evolution Reaction.

The structure and properties of the carrier significantly affect the catalytic activity of the active centers for supported electrocatalysts. Therefore, elaborate design and regulation of the physicochemical properties of carbon carriers are essential to improve the activity and stability of the carbon-supported ruthenium-based catalysts. Herein, enlightened by the unique characteristics of coexisting sp2 and sp3 carbon nuclei in N-doped carbon dots (NCDs), a hybrid structure of N-doped carbon substrates featuring N-doped sp2 /sp3 carbon interfaces loaded with Ru nanoparticles (Ru/NCDs) is obtained. Spectroscopic analysis and density functional theory calculations illustrate that the interaction between Ru and NCDs effectively modulates the electronic structure of the active center Ru, and the formed N-doped sp2 /sp3 carbon interface lowers the energy barrier of the intermediates in hydrogen evolution reaction (HER) and balances the hydrogen adsorption and desorption and, thereby, greatly improves the activity of Ru/NCDs. Remarkably, Ru/NCDs exhibit excellent HER activity and stability in comparison to Pt/C, which merely requires overpotentials as low as 37 and 14 mV at 10 mA cm-2 in alkaline and acidic electrolytes, respectively. This finding will provide more thoughts about the influence of substrate properties on the catalytic activity and rational design of carbon-loaded electrocatalysts.

Mo propellant boosting the activity of Ni-P for efficient urea-assisted water electrolysis of hydrogen evolution.

Replacing the sluggish oxygen evolution reaction (OER) with thermodynamically favorable urea oxidation reaction (UOR) is an appealing tactic in the energy-saving water splitting system. Herein, by a facile composite electrodeposition method, an electrocatalyst with Mo particles anchored on the Ni-P matrix (Mo/Ni-P) was fabricated and utilized for urea-assisted water electrolysis of hydrogen production. As expected, the urea-involved electrolytic cell with the as-obtained Mo/Ni-P served as both the anode and cathode merely needs a voltage of 1.55 V to sustain a current density of 50 mA cm-2 (0.16 V less than that of the conventional water splitting at 50 mA cm-2) and can maintain the stability for 12 h. Additionally, the solar-driven urea-assisted water electrolysis system was constructed under lab conditions and solar-hydrogen-electricity energy conversion processes were also simulated. Moreover, it was demonstrated that tungsten (W) particles can also serve as an accelerant for promotion both the hydrogen evolution reaction (HER) and UOR activity of pristine Ni-P. This work will present a facile method for rational integration of metal particles with Ni-P layer for highly efficient electrocatalysts applied in economic production of H2.

Nitrogen Disturbance Awakening the Intrinsic Activity of Nickel Phosphide for Boosted Hydrogen Evolution Reaction.

Nickel phosphide (Ni2 P) has emerged as a promising candidate to substitute Pt-based catalysts for hydrogen evolution reaction (HER) due to the hydrogenase-like catalytic mechanism and concomitantly low cost. However, its catalytic activity is still not comparable to that of noble-metal-based catalysts, and innovative strategies are still urgently needed to further improve its performance. Herein, a self-supported N-doped Ni2 P on Ni foam (N-Ni2 P/NF) was rationally designed and fabricated through a facile NH4 H2 PO2 -assisted gas-solid reaction process. As an HER catalyst in alkaline medium, the obtained N-Ni2 P/NF revealed excellent electrocatalytic performance with a distinctly low overpotential of 50 mV at 10 mA cm-2 , a small Tafel slope of 45 mV dec-1 , and long-term stability for 25 h. In addition, the spectroscopic characterizations and density functional theory calculations confirmed that the incorporation of N regulated the original electronic structure of Ni2 P, enhanced its intrinsic catalytic property, optimized the Gibbs free energy of reaction intermediates, and ultimately promoted the HER process. This work provides an atomic-level insight into the electronic structure modulation of metal phosphides and opens an avenue for developing advanced transition metal phosphides-based catalysts.

Modulation of Water Dissociation Kinetics with a "Breathable" Wooden Electrode for Efficient Hydrogen Evolution.

Innovative breakthroughs regarding self-supported open and porous electrodes that can promote gas-liquid transmission and regulate the water dissociation kinetics are critical for sustainable hydrogen economy. Herein, a free-standing porous electrode with Pd-NiS nanoparticles assembled in a multichannel carbonized wood framework (Pd-NiS/CW) was ingeniously constructed. Specifically, carbonized wood (CW) with a mass of open microchannels and high electrical conductivity can significantly facilitate electrolyte permeation ("inhalation"), hydrogen evolution ("exhalation"), and electron transfer. As expected, the fabricated "breathable" wooden electrode exhibits remarkable hydrogen evolution activity in 1.0 M KOH, only requiring a low overpotential of 80 mV to sustain a current density of 10 mA cm-2, and can maintain this current density for 100 h. Further, the spectroscopic characterization and density functional theory (DFT) calculations manifest that the electron interaction between Pd and NiS is beneficial to reduce the water dissociation energy barriers, optimize the adsorption/desorption of H, and ultimately accelerate the catalytic activity. The work reported here will provide a potential approach for the design of electrocatalysts combined with natural multichannel wood to achieve the goal of high electrocatalytic activity and superior durability for hydrogen production.

Multifunctional Ternary Hybrid Hydrogel Sensor Prepared via the Synergistic Stabilization Effect.

Since highly stretchable hydrogels have demonstrated their promising applications in flexible tactile sensors and wearable devices, the current challenge has been imposed on stretchable and multifunctional electronics. Here, we report a multifunctional sensor composed of a liquid metal (LM) nanodroplet-adhered self-assembled polymeric network, anionic carboxymethylcellulose (CMC), and cationic polyacrylamide (PAAm). The synergistic effect, zeta potential reduction, by CMC and macromolecules enveloped by LM contributes to the stabilization of the ternary system during preparation and, thus, the homogenization of the products. By engineering and optimizing the ternary hybrid hydrogels, excellent extensibility (tensile strain near 300%), readily reversible hysteresis loops, and accessible deformability (low modulus of 104 Pa) are afforded. The fabricated sensor exhibits a high tensile strain gauge factor of around 0.7 and a high compressive stress sensitivity of up to 0.12 kPa-1, a fast response time below 125 ms, and a high stability and precision in usage. In a series of practical scenarios, the assembled sensor displays distinguished abilities to monitor bodily motions, record electrocardiograms, authenticate handwriting, discern temperature, and infer materials, making them highly promising for multifunctional intelligent soft sensing.

Strong Electron Coupling of Ru and Vacancy-Rich Carbon Dots for Synergistically Enhanced Hydrogen Evolution Reaction.

The exploitation of ingenious strategies to improve the activity and stability of ruthenium (Ru) is crucial for the advancement of Ru-based electrocatalysts. Vacancy engineering is a typical strategy for modulating the catalytic activity of electrocatalysts. However, creating vacancies directly into pure metallic Ru is difficult because of the extremely stringent conditions required and will result in instability because the integrity of the crystal structure is destroyed. In response, a compromise tactic by introducing vacancies in a Ru composite structure is proposed, and vacancy-rich carbon dots coupled with Ru (Ru@CDs) are elaborately constructed. Specifically, the vacancy-rich carbon dots (CDs) serve as an excellent platform for anchoring and trapping Ru nanoparticles, thus restraining their agglomeration and growth. As expected, Ru@CDs exhibited excellent catalytic performance with a low overpotential of 30 mV at 10 mA cm-2 in 1 m KOH, a small Tafel slope of 22 mV decade-1 , and robust stability even after 10 000 cycles. The low overpotential is comparable to those of most previously reported Ru-based electrocatalysts. Additionally, spectroscopic characterizations and theoretical calculations demonstrate that the rich vacancies and the electron interactions between Ru and CDs synergistically lower the intermediate energy barrier and thereby maximize the activity of the Ru@CDs electrocatalyst.

Cellulose-Based Hybrid Structural Material for Radiative Cooling.

Structural materials with excellent mechanical properties are vitally important for architectural application. However, the traditional structural materials with complex manufacturing processes cannot effectively regulate heat flow, causing a large impact on global energy consumption. Here, we processed a high-performance and inexpensive cooling structural material by bottom-up assembling delignified biomass cellulose fiber and inorganic microspheres into a 3D network bulk followed by a hot-pressing process; we constructed a cooling lignocellulosic bulk that exhibits strong mechanical strength more than eight times that of the pure wood fiber bulk and greater specific strength than the majority of structural materials. The cellulose acts as a photonic solar reflector and thermal emitter, enabling a material that can accomplish 24-h continuous cooling with an average dT of 6 and 8 °C during day and night, respectively. Combined with excellent fire-retardant and outdoor antibacterial performance, it will pave the way for the design of high-performance cooling structural materials.

Anisotropic, Flexible Wood Hydrogels and Wrinkled, Electrodeposited Film Electrodes for Highly Sensitive, Wide-Range Pressure Sensing.

Biological muscles generally possess well-aligned muscle fibers and thus excellent strength and toughness. Inspired by their microstructure, tough wood hydrogels with a preserved unique alignment of cellulose fibers, mechanical anisotropy, and desirable flexibility were developed by introducing chemically and ionically cross-linked poly(acrylic acid) (PAA) into the abundant pores of delignified wood. PAA chains well infiltrated the parallelly aligned cellulose fibers of wood and formed a layer-by-layer network structure, resulting in strong, elastic tangential, and radial wood hydrogel slices. The tangential slices had a high compressive strength of 1.73 MPa and a maximum strain at fracture of 69.4%, while those of the radial slices were 0.6 MPa and 47.0%. After sandwiching the radial and tangential hydrogel slices with reduced graphene oxide (rGO) film electrodes into capacitive pressure sensors (CPSs), the tangential CPS displayed the most desired, gradient sensitivity values in the whole stress range. Additionally, the wrinkling treatment of the rGO electrode greatly improved the capacitance responsiveness toward pressure. The real-time sensing stress values of our tangential CPS during monitoring practical human activities were calculated in the range of 0.1-1.3 MPa, demonstrating the achievement of ultrafast, highly sensitive, and wide-stress-range detection for potential applications in human-machine interfaces.

[Molecular cloning and characterization of a novel metagenome-derived bacterial perhydrolase].

The aim of this study is to obtain bacterial perhydrolases with chlorination activity, expands the resources of perhydrolases, and lays a foundation for it's industrial applications. We constructed a metagenomic library using environmental DNA isolated from sludge samples of a paper mill of Tanghe county, and identified a per822 gene encoding a bacteria perhydrolase via activity-based functional screening. Then, we overexpressed Per822 heterologously in Escherichia coli, and characterized the recombinant enzyme after purification. Finally, we further investigated the ability of Per822 to produce peracetic acid (PAA). Sequence analysis revealed that per822 encoded a protein of 273 amino acids. The recombinant Per822 had the activity of peroxidase, esterase and halogenase respectively, and thus was regarded as a typical representative of multifunctional enzymes. The purified Per822 exhibited maximal chlorination activity (hyperhydrolysis) at 55 °C and pH 4.5 with monochlorodimedone as substrate, and the enzyme was stable in the pH range of 3.5-8.0 and below 70 °C. Also, the chlorination activity of this enzyme could be activated by Fe²âº. In addition, the enzyme displayed high ability to generate PAA using ethyl acetate as cosubstrate. The highly soluble expression, catalytic versatility and good PAA production capacity of Per822 make it a potential candidate in organic synthesis, wastewater treatment, disinfection and biomass pretreatment, etc.

Modulation of Molecular Spatial Distribution and Chemisorption with Perforated Nanosheets for Ethanol Electro-oxidation.

Integrating thermodynamically favorable ethanol reforming reactions with hybrid water electrolysis will allow room-temperature production of high-value organic products and decoupled hydrogen evolution. However, electrochemical reforming of ethanol has not received adequate attention due to its low catalytic efficiency and poor selectivity, which are caused by the multiple groups and chemical bonds of ethanol. In addition to the thermodynamic properties affected by the electronic structure of the catalyst, the dynamics of molecule/ion dynamics in electrolytes also play a significant role in the efficiency of a catalyst. The relatively large size and viscosity of the ethanol molecule necessitates large channels for molecule/ion transport through catalysts. Perforated CoNi hydroxide nanosheets are proposed as a model catalyst to synergistically regulate the dynamics of molecules and electronic structures. Molecular dynamics simulations directly reveal that these nanosheets can act as a "dam" to enrich ethanol molecules and facilitate permeation through the nanopores. Additionally, the charge transfer behavior of heteroatoms modifies the local charge density to promote molecular chemisorption. As expected, the perforated nanosheets exhibit a small potential (1.39 V) and high Faradaic efficiency for the conversion of ethanol into acetic acid. Moreover, the concept in this work provides new perspectives for exploring other molecular catalysts.

[Efficacy and safety of autohemotherapy at acupoint for acne: systematic review].

OBJECTIVE: To evaluate the efficacy and safety of autohemotherapy at acupoint for acne. METHODS: Randomized controlled trials (RCTs) regarding autohemotherapy at acupoint for acne were searched in CNKI, WanFang, VIP database and PubMed. According to the inclusion and exclusion criteria, two investigators performed the literature screening, data extraction and basis evaluation, independently. Meta analysis was performed by using Review Manager 5.3 software. RESULTS: Eight RCTs were included, involving 573 patients. The combined effect of effective rate was 1.21 (95% Cl : 1.12, 1.30); the combined effect of skin lesions improvement was -1.00 (95%Cl: -2.14, -0.14, Z＝1.73, P=0.08); the combined effect of recurrence rate was 0.44 (95%Cl: 0.09, 2.15, Z＝1.01, P=0.31). CONCLUSION: The autohemotherapy at acupoint has better efficacy and skin lesions improvement for acne than control treatment, and autohemotherapy is safer.

QGQS Granule in SHR Serum Metabonomics Study Based on Tools of UPLC-Q-TOF and Renin-Angiotensin-Aldosterone System Form Protein Profilin-1.

QGQS granule is effective for the therapeutic of hypertension in clinic. The aim of this research is to observe the antihypertension effect of QGQS granule on SHR and explain the mechanism of its lowering blood pressure. 30 SHR were selected as model group, captopril group, and QGQS group, 10 WKYr were used as control group, and RBP were measured on tail artery consciously. And all the serum sample analysis was carried out on UPLC-TOF-MS system to determine endogenous metabolites and to find the metabonomics pathways. Meanwhile, ELISA kits for the determination pharmacological indexes of PRA, AngI, AngII, and ALD were used for pathway confirmatory; WB for determination of profilin-1 protein expression was conducted for Ang II pathway analysis as well. It is demonstrated that QGQS granule has an excellent therapeutic effect on antihypertension, which exerts effect mainly on metabonomics pathway by regulating glycerophospholipid, sphingolipid, and arachidonic acid metabolism, and it could inhibit the overexpression of the profilin-1 protein. We can come to a conclusion that RAAS should be responsible mainly for the metabonomics pathway of QGQS granule on antihypertension, and it plays a very important role in protein of profilin-1 inhibition.