Fluorination modification enhanced the water resistance of Universitetet i Oslo-67 for multiple volatile organic compounds adsorption under high humidity conditions: Mechanism study.

The construction of metal-organic frameworks (MOFs) with highly efficient capture for volatile organic compounds (VOCs) adsorption under humid conditions is a significant yet formidable task. Herein, series of fluorinated UiO-67 modified with trifluoroacetic acid (TFA) and 4-fluorobenzoic acid were successfully synthesized for VOCs adsorption under high humidity conditions. Experiments results showed that UiO-67 modified with 4-fluorobenzoic acid (67-F) presented excellent adsorption capacity of 345 mg/g for toluene adsorption and exhibited great water resistance (10.0 vol% H2O, 374 mg/g toluene adsorption capacity). Characterization results indicated that the introduction of 4-fluorobenzoic acid induced the competitive coordination between 4-fluorobenzoic acid and 4,4-biphenyl dicarboxylic acid (BPDC) with Zr4+, causing the formation of abundant defects to provide extra adsorption sites. Meanwhile, the benzene ring in 4-fluorobenzoic acid enhanced the π-π conjugation, causing the further promotion of VOCs adsorption capacity. More importantly, the water resistance mechanism was investigated and elucidated that the introduction of F decreased the surface energy of 67-F and its affinity with water. Meanwhile, the metal complex induced by the fluorinated modification produced an electron-dense pore environment, which greatly improved its chemical and water stability. This work provided a strategy for preparing an adsorbent with high water resistance for real-world VOCs adsorption at high humidity conditions.

Loureirin A is a narrow-spectrum antimicrobial agent against Helicobacter pylori.

Currently, Helicobacter pylori eradication by antibiotic therapy faces various challenges, including antibiotic resistance, side effects on intestinal commensal bacteria, and patient compliance. In this study, loureirin A (LrA), a traditional Chinese medicine monomer extracted from Sanguis Draconis flavones, was found to possess specific antibacterial activity against H. pylori without the bacteria displaying a tendency to develop resistance in vitro. LrA demonstrated a synergistic or additive effect when combined with omeprazole (a proton pump inhibitor) against H. pylori. The combination of LrA and omeprazole showed promising anti-H. pylori potential, exhibiting notable in vivo efficacy comparable to standard triple therapy in mouse models infected with both drug-sensitive and drug-resistant H. pylori strains. Moreover, the narrow-spectrum antibacterial profile of LrA is reflected in its minimal effect on the diversity and composition of the mouse gut microbiota. The underlying mechanism of action of LrA against H. pylori involves the generation of bactericidal levels of reactive oxygen species, resulting in apoptosis-like cell death. These findings indicate that LrA is a promising lead compound targeting H. pylori without harming the commensal bacteria.

Photonic Pigments of Polystyrene-block-Polyvinylpyrrolidone Bottlebrush Block Copolymers via Sustainable Organized Spontaneous Emulsification.

Prior studies on photonic pigments of amphiphilic bottlebrush block copolymers (BBCPs) through an organized spontaneous emulsification (OSE) mechanism have been limited to using polyethylene glycol (PEG) as the hydrophilic side chains and toluene as the organic phase. Herein, a family of polystyrene-block-polyvinylpyrrolidone (PS-b-PVP) BBCPs are synthesized with PVP as the hydrophilic block. Biocompatible and sustainable anisole is employed for dissolving the obtained BBCPs followed by emulsification of the solutions in water. Subsequent evaporation of oil-in-water emulsion droplets triggers the OSE mechanism, producing thermodynamically stable water-in-oil-in-water (w/o/w) multiple emulsions with uniform and closely packed internal droplet arrays through the assembly of the BBCPs at the w/o interface. Upon solidification, the homogeneous porous structures are formed within the photonic microparticles that exhibit visible structural colors. The pore diameter is widely tunable (150∼314 nm) by changing the degree of polymerization of BBCP (69∼110), resulting in tunable colors across the whole visible spectrum. This work demonstrates useful knowledge that OSE can be generally used in the fabrication of ordered porous materials with tunable internal functional groups, not only for photonic applications, but also offers a potential platform for catalysis, sensing, separation, encapsulation, etc.

Vital role of CYP450 in the biodegradation of antidiabetic drugs in the aerobic activated sludge system and the mechanisms.

The extensive use of antidiabetic drugs (ADDs) and their detection in high concentrations in the environment have been extensively documented. However, the mechanism of ADDs dissipation in aquatic environments is still not well understood. This study thoroughly investigates the dissipation behavior of ADDs and the underlying mechanisms in the aerobic activated sludge system. The results indicate that the removal efficiencies of ADDs range from 3.98% to 100% within 48 h, largely due to the biodegradation process. Additionally, the gene expression of cytochrome P450 (CYP450) is shown to be significantly upregulated in most ADDs-polluted samples (P < 0.05), indicating the vital role of CYP450 enzymes in the biodegradation of ADDs. Enzyme inhibition experiments validated this hypothesis. Moreover, molecular docking and simulation results indicate that a strong correlation between the biodegradation of ADDs and the interactions between ADDs and CYP450 (Ebinding). The differences in dissipation behavior among the tested ADDs are possibly due to their electrophilic characteristics. Overall, this study makes the initial contribution to a more profound comprehension of the crucial function of CYP450 enzymes in the dissipation behavior of ADDs in a typical aquatic environment.

[Comparison of talonavicular-cuneiform joint fusion with bone grafting and without bone grafting in treatment of Müller-Weiss disease].

Objective: To compare the effectiveness of talonavicular-cuneiform joint fusion with iliac bone grafting and without bone grafting in the treatment of Müller-Weiss diseases (MWD). Methods: The clinical data of 44 patients (44 feet) with MWD who received talonavicular-cuneiform joint fusion between January 2017 and November 2022 and met the selection criteria was retrospectively analyzed. Among them, 25 patients were treated with structural iliac bone grafting (bone grafting group) and 19 patients without bone grafting (non-bone grafting group). There was no significant difference ( P>0.05) in age, gender composition, body mass index, disease duration, affected side, Maceira stage, and preoperative American Orthopaedic Foot and Ankle Society (AOFAS) score, visual analogue scale (VAS) score, anteroposterior/lateral Meary angle, and Pitch angle between the two groups. Operation time, operation cost, and postoperative complications were recorded in the two groups. AOFAS and VAS scores were used to evaluate the function and pain degree of the affected foot. Meary angle and Pitch angle were measured on the X-ray film, and the joint fusion was observed after operation. The difference (change value) of the above indexes before and after operation was calculated for comparison between groups to evaluate the difference in effectiveness. Results: The operation was successfully completed in both groups, and the incisions in the two groups healed by first intention. The operation time and cost in the bone grafting group were significantly more than those in the non-bone grafting group ( P<0.05). All patients were followed up. The median follow-up time was 41.0 months (range, 16-77 months) in the non-bone grafting group and 40.0 months (range, 16-80 months) in the bone grafting group. There was skin numbness of the medial dorsalis of the foot in 1 case, internal fixation stimulation in 2 cases, and pain at the iliac bone harvesting area in 1 case of the bone grafting group. There was skin numbness of the medial dorsalis of the foot in 1 case and muscle atrophy of the lower limb in 1 case of the non-bone grafting group. There was no significant difference in the incidence of complications between the two groups ( P>0.05). At last follow-up, the AOFAS scores of the two groups significantly improved when compared with those before operation, while the VAS scores significantly decreased, the anteroposterior/lateral Meary angle and Pitch angle significantly improved, and the differences were significant ( P<0.05). There was no significant difference in the change values of outcome indicators between the two groups ( P>0.05). There was no delayed bone union or bone nonunion in both groups, and joint fusion was achieved at last follow-up. Conclusion: In the treatment of MWD, there is no significant difference in effectiveness and imaging improvement of talonavicular-cuneiform joint fusion combined with or without bone grafting. However, non-bone grafting can shorten the operation time, reduce the cost, and may avoid the complications of bone donor site.

Müller-Weiss Disease: Midfoot Arthrodesis in Reduction vs Malreduction.

BACKGROUND: Midfoot arthrodesis is regarded as the main surgical approach for treating Müller-Weiss disease (MWD). This study aimed to investigate the incidence of postoperative pain during MWD treatment through midfoot reduction or malreduction during arthrodesis and to explore the factors influencing postoperative pain in patients with MWD. METHODS: A total of 67 patients with MWD were recruited and divided into two groups according to whether midfoot alignment was reduced: reduction group (n = 38) and malreduction group (n = 29). Demographic characteristics before the operation and at the last follow-up, as well as clinical and radiographic parameters, were compared between the two groups. Clinical parameters included the American Orthopaedic Foot & Ankle Society score and visual analog scale score, whereas radiographic parameters included the calcaneal pitch angle, lateral Meary's angle, talometatarsal-1 angle dorsoplantar (TMT1dp), talocalcaneal angle dorsoplantar (Kite angle), talonavicular coverage angle, and medial navicular pole extrusion. Postoperative complications and incidence of midfoot pain were evaluated at the last follow-up visit. RESULTS: The reduction group exhibited better clinical and radiological parameters, including the TMT1dp and medial navicular pole extrusion, than the malreduction group at the last follow-up (all P < .05). However, the calcaneal pitch angle, lateral Meary's angle, Kite angle, and talonavicular coverage angle did not significantly differ between the two groups (all P > .05). The overall incidence of midfoot pain was 26.4%. The reduction group showed a lower incidence of medial pain than the malreduction group (15.7% vs. 40.0%, P < .05). Regression analysis revealed that midfoot abduction, represented by the TMT1dp, was a critical factor for midfoot arthrodesis failure and that medial navicular pole extrusion was not correlated with postoperative midfoot pain. CONCLUSION: Midfoot reduction arthrodesis yields better clinical outcomes than malreduction arthrodesis. The TMT1dp, representing midfoot abduction, is a key factor for midfoot arthrodesis failure. The extruded medial navicular bone may not affect postoperative medial midfoot pain. LEVEL OF EVIDENCE: Level III, retrospective comparative study.

Defects materials of Institut Lavoisier-125(Ti) materials enhanced photocatalytic activity for toluene and chlorobenzene mixtures degradation: Mechanism study.

In this paper, the effect of three monocarboxylic acids on MIL-125 synthesis was systematically investigated and the results were discussed in detail. X-ray diffractometry (XRD) and nitrogen adsorption-desorption curves indicated that small molecule acids (acetic acid, propionic acid and butyric acid) affected the morphology of MIL-125 and induced lamellar pores and structural defects in the crystals. Thermogravimetric measurements confirmed the presence of acid-regulated defective metal-organic frameworks (MOFs). Electrochemical tests and density function theory calculations indicated that acid modulation could change the forbidden bandwidth of the material. The acid modification strategy effectively promoted the transfer of photogenerated electrons and enhanced the adsorption and activation of O2 and H2O molecules, generating reactive radicals. The modified MOFs also showed excellent performance in the removal of mixed toluene and chlorobenzene. The degradation pathways of the mixture were analyzed by in situ infrared (IR) and gas chromatography-mass spectrometry (GC-MS). The mixture was converted to chlorophenolic intermediates in the presence of reactive oxygen species, further decomposed to form ethers and ethanol, and finally formed small molecules such as carbon dioxide and water. A feasible method was provided for the preparation of photocatalysts for the treatment of mixed VOCs.

Changes in clinical outcomes and alignment of the ipsilateral knee and ankle after supramalleolar osteotomy in patients with varus osteoarthritis of the ankle: a short-term follow-up study.

PURPOSE: The purpose of this study was to investigate the changes in clinical outcomes and alignment of the ipsilateral knee and ankle in patients with varus ankle osteoarthritis after supramalleolar osteotomy (SMO). METHODS: We retrospectively reviewed 23 patients (24 ankles) with Takakura II, IIIa and IIIb ankle osteoarthritis treated with SMO between May 2017 and March 2022. The radiologic parameters of ankles contained medial distal tibial angle (TAS), tibiotalar angle (TT), tibial lateral surface (TLS), tibial plafond inclination (TPI) and talar inclination (TI). The radiologic parameters of knees contained medial proximal tibial angle (MPTA), joint line convergence angle (JLCA), the knee joint line orientation relative to ground (G-KJLO) and WBL. Hip-knee-ankle angle (HKA) was also collected. The Takakura system was used for evaluating the ankle osteoarthritis and the Kellgren-Lawrence (KL) system was used for evaluating the knee osteoarthritis. Clinical evaluation of the ankle joints contained American Orthopedic Foot and Ankle Society (AOFAS), range of motion (ROM) and visual analogue scale (VAS). Clinical evaluation of the knee joints contained Japanese Orthopaedic Association Scores (JOA), ROM, VAS. RESULTS: The mean follow-up times were 20.3 ± 7.3 months (range 12-38). According to the radiologic evaluation, the TAS increased from preoperative 84.7° ± 2.0° to 91.2° ± 1.8° at the last follow-up (P < 0.001). The TPI and TI decreased from 4.4° ± 4.2° and 11.0° ± 5.2° to 0.1° ± 4.7° and 4.1° ± 4.8° (P < 0.001 for both). The TT angel improved from 9.5° ± 4.1° to 4.9° ± 3.3° (P < 0.001). No significant differences were found regarding MPTA, JLCA, G-KJLO, knee WBL and HKA (P > 0.05 for all). The Takakura stage improved after SMO (P < 0.001) whilst the KL stage maintains the similar lever (P > 0.05). According to the clinical evaluation, the AOFAS significantly increased from 67.5 ± 10.6 to 88.5 ± 9.3 and the VAS of the ankle decreased from 4.7 ± 1.6 to 1.2 ± 1.1, whilst there were no changes on VAS and even the JOA and knee ROM after SMO (P > 0.05 for all). CONCLUSIONS: SMO can alleviate the symptoms of varus ankle osteoarthritis and delay the time for ankle replacement or arthrodesis by redistributing the abnormal stress of the ankle and restoring the congruence of the tibiotalar joint. In addition, it did not induce the clinical symptoms of knee without compromising lower limb alignment or knee joint line orientation in the short term. LEVEL OF EVIDENCE: Level IV case series.

Transition Metal Functionalized C30N12S6 as High-Performance Trifunctional Catalysts with Integrated Descriptors toward Hydrogen Evolution, Oxygen Evolution, and Oxygen Reduction Reactions: A Case of High-Throughput First-Principles Screening within the Framework of TM-N2@C30N10S6.

In energy conversion and storage technologies, the design of highly efficient trifunctional electrocatalysts integrating with the high hydrogen evolution reaction (HER) and oxygen evolution/reduction reaction (OER/ORR) activities is highly desirable. Herein, utilizing first-principles computations, a novel periodically ordered macropore C30N12S6 monolayer was proposed, and the stability analysis attests to its good stability. Single transition metal (TM) atom anchored onto this newly proposed C30N12S6 monolayer to form single-atom catalysts, as achieved by TM-N2@C30N10S6, among which the Co-N2@C30N10S6 is the most promising multifunctional catalyst toward HER/OER/ORR with low overpotential of 0.01/0.59/0.3 V; meanwhile, the Rh-N2@C30N10S6 can be used as a bifunctional OER/ORR catalyst with low overpotential of 0.37/0.44 V, overmatching the landmark Pt (111) and IrO2/RuO2 catalysts. Particularly, the TM-d orbital in TM@CNS is remarkably hybridized with the O-p orbital of oxygenated intermediates, so that the lone electrons initially located at the antibonding orbital pair up and fill the downward bonding orbital, allowing OH* to be suitably adsorbed on TM@CNS, enhancing the catalytic performance. The relevant attributes, such as good stabilities and metallic features, ensured their applications in ambient conditions. Moreover, multilevel descriptors were constructed to clarify the origin of activity on TM@CNS, such as ΔGOH* (Gibbs free energy of OH*), εd (d-band center), COHP (crystal orbital Hamilton population), Nd/Nd + s (number of d/d + s electrons) and φ (descriptor), among which the filling of outer d-electrons of TM atom significantly affects the value of ΔGOH* that can determine the overpotential and, thus, become a key descriptor.

Efficacy and Safety of Niraparib as First-Line Maintenance Treatment for Patients with Advanced Ovarian Cancer: Real-World Data from a Multicenter Study in China.

BACKGROUND: Poly (ADP-ribose) polymerase (PARP) inhibitors are a new maintenance therapy option for patients with ovarian cancer (OC). OBJECTIVE: To evaluate the efficacy and influencing factors of the novel PARP inhibitor niraparib for maintenance treatment of Chinese patients with advanced OC. PATIENTS AND METHODS: In this retrospective multicenter real-world study patients with advanced OC from 15 hospitals throughout China were enrolled. The primary endpoint was progression-free survival (PFS) and the secondary endpoints included the time to treatment discontinuation and safety. Least Absolute Shrinkage and Selection Operator (LASSO) regression was used to identify possible risk factors for PFS, after which a prediction model was established to evaluate the likelihood of achieving an 18-month PFS. The relationship between the dose of niraparib and PFS was also evaluated. RESULTS: The PFS rates of 199 patients at 6, 12, 18, 24, and 30 months were 87.4%, 75.9%, 63.6%, 56.1%, and 51.8%, respectively. LASSO regression model revealed that only age < 65 years (P = 0.011), BRCA mutations (P < 0.001), and R0 status after cytoreductive surgery (P = 0.01) were significant factors associated with prolonged PFS times. Based on the LASSO logistic regression analysis, a clinical prediction formula was developed: - 2.412 + 1.396Age≥65yr + 2.374BRCAwt + 1.387R1 + 0.793Interval≥12w + 0.178BMI>24kg/m2 which yielded a cut-off value of 0.091, an area under the curve (AUC) of 0.839 (0.763-0.916), a sensitivity of 94.3%, and an accuracy of 78.5%. A nomogram was then built to visualize the results. The major treatment-emergent adverse events of ≥ grade 3 included a platelet count decrease (19.1%), white blood cell count decrease (15.1%), neutrophil count decrease (13.1%), and anemia (18.6%). The 18-month PFS rates in patients treated with 200 mg niraparib were somewhat higher than in patients treated with 100 mg after 3-months of therapy. CONCLUSIONS: For Chinese OC patients, niraparib, particularly at a 200 mg individual starting dose, was an effective therapy with easily manageable safety.

Maintenance therapy with poly (ADP-ribose) polymerase inhibitors is a new option for patients with ovarian cancer (OC) after they have received platinum-based chemotherapy to reduce the recurrence or relapse rates, but it remains unclear whether there are any changes in efficacy and safety when different starting doses of niraparib are administrated to Chinese patients, who typically have a bodyweight < 77 kg. We found that niraparib exhibited satisfactory efficacy with tolerable safety during maintenance therapy for advanced OC whether administered at 100 mg or 200 mg doses. We believe these regimens can serve as a valuable addition to the previous results of randomized controlled trials.

Genomic Analysis of Leptolyngbya boryana CZ1 Reveals Efficient Carbon Fixation Modules.

Cyanobacteria, one of the most widespread photoautotrophic microorganisms on Earth, have evolved an inorganic CO2-concentrating mechanism (CCM) to adapt to a variety of habitats, especially in CO2-limited environments. Leptolyngbya boryana, a filamentous cyanobacterium, is widespread in a variety of environments and is well adapted to low-inorganic-carbon environments. However, little is currently known about the CCM of L. boryana, in particular its efficient carbon fixation module. In this study, we isolated and purified the cyanobacterium CZ1 from the Xin'anjiang River basin and identified it as L. boryana by 16S rRNA sequencing. Genome analysis revealed that L. boryana CZ1 contains ß-carboxysome shell proteins and form 1B of Rubisco, which is classify it as belonging to the ß-cyanobacteria. Further analysis revealed that L. boryana CZ1 employs a fine CCM involving two CO2 uptake systems NDH-13 and NDH-14, three HCO3- transporters (SbtA, BicA, and BCT1), and two carboxysomal carbonic anhydrases. Notably, we found that NDH-13 and NDH-14 are located close to each other in the L. boryana CZ1 genome and are back-to-back with the ccm operon, which is a novel gene arrangement. In addition, L. boryana CZ1 encodes two high-affinity Na+/HCO3- symporters (SbtA1 and SbtA2), three low-affinity Na+-dependent HCO3- transporters (BicA1, BicA2, and BicA3), and a BCT1; it is rare for a single strain to encode all three bicarbonate transporters in such large numbers. Interestingly, L. boryana CZ1 also uniquely encodes two active carbonic anhydrases, CcaA1 and CcaA2, which are also rare. Taken together, all these results indicated that L. boryana CZ1 is more efficient at CO2 fixation. Moreover, compared with the reported CCM gene arrangement of cyanobacteria, the CCM-related gene distribution pattern of L. boryana CZ1 was completely different, indicating a novel gene organization structure. These results can enrich our understanding of the CCM-related gene arrangement of cyanobacteria, and provide data support for the subsequent improvement and increase in biomass through cyanobacterial photosynthesis.

Responses of antibiotic resistance genes in the enhanced biological phosphorus removal system under various antibiotics: Mechanisms and implications.

The effects of antibiotics on the proliferation of antibiotic resistant genes (ARGs) in WWTPs have drawn great attention in recent years. The effects of antibiotics on ARGs in the enhanced biological phosphorus removal (EBPR) system and its mechanisms, however, are still not well understood. In this study, EBPR systems were constructed using activated sludge to investigate the effects of ten commonly detected antibiotics in the environment on the proliferation of ARGs and the mechanisms involved. The results showed that the total abundance of ARGs increased to varying degrees with the addition of different antibiotics (0.05 mmol/L), and the top 30 ARGs increased by 271.1 % to 370.0 %. Mobile genetic elements (MGEs), functional modules, and the bacteria community were consistently related to the changes in ARGs. Refractory antibiotics, in particular, have a stronger promoting effect on transduction in the EBPR system. The insertion sequence common region (ISCR) and transposon (Tnp) were identified as crucial factors in the proliferation of ARGs. Moreover, the risk of polyphosphate accumulating organisms (PAOs) carrying ARGs in the presence of antibiotics should not be ignored. Our findings emphasize the potential efficacy of employing strategies that target the reduction of MGEs, regulation of cellular communication, and management of microbial communities to effectively mitigate the risks associated with ARGs.

Effect of benzoic acid and dopamine hydrochloride as a modulator in the water resistance of Universitetet i Oslo-67: Adsorption performance and mechanism.

The severe hazards on ecological environment and human body caused by volatile organic compounds (VOCs) have attracted worldwide substantial attention. In this research, a series of novel modified Universitetet i Oslo-67 (UiO-67) with water resistance were prepared and characterized, which had modified by benzoic acid and dopamine hydrochloride (67-ben-DH). On this basis, the adsorption performance, adsorption kinetics, defect engineering and water resistance of adsorbent were investigated. The results indicated that the excellent pore structure and specific surface area of 67-ben-DH-6 (molar ratio of Zr4+ to DH was 1:6) were retained while the adsorption performance and water resistance of the adsorbent were improved. Due to more defects, excellent adsorption diffusion and strong π-π interactions of 67-ben-DH-6, it performed the maximum adsorption capacity of toluene (793 mg g-1). Furthermore, the outstanding water resistance was attributed to the fact that N element of DH reduced the affinity of the adsorbent with water. Finally, the density functional theory (DFT) calculations showed that the adsorbent 67-ben-DH-6 had the maximum adsorption energy for toluene (-99.4 kJ mol-1) and the minimum adsorption energy for water (-17.8 kJ mol-1). Thus, the potential mechanism of 67-ben-DH for efficient toluene adsorption and water resistance was verified from a microscopic perspective.

Kagome-like BiP3 Monolayer: An Emerging Quasi-Direct Auxetic Semiconductor Coupled with High Anisotropic Mobility toward Visible-Light-Driven Photoelectrocatalytic pH-Robust Overall Water-Splitting.

Two-dimensional (2D) Janus materials exhibit an outstanding potential that can meet the rigorous requirements of photocatalytic water splitting resulting from their unique atomic arrangement. However, these materials are quite scarce. Through ab initio density functional theory calculations, we introduce a kagome topology into the honeycomb lattice of blue phosphorene using phosphorus and bismuth atoms to build a hybrid honeycomb-like kagome lattice, realized by a hitherto unknown kagome-like Janus-like BiP3 monolayer with robust stability. Excitingly, the out-of-plane asymmetry benefiting from kagome and honeycomb topologies gives rise to a significantly negative out-of-plane Poisson's ratio and an obvious built-in electric field pointing from the sublayer of the P atom to the sublayer of the Bi atom. In conjunction with the investigations that encompass semiconducting properties, such as a quasi-direct gap, suitable band-edge positions, effective visible-light absorption, and high carrier mobility, the BiP3 monolayer achieves overall water splitting at pH 0-14 regardless of strain. Moreover, this intrinsic electric field provides a sufficient photogenerated carrier driving force for water splitting. The bare BiP3 comprises P and Bi atoms that function as catalysts for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) active sites, respectively. Upon exposure to light, the reaction of water into H2 and O2 can be observed across a pH range of 0-14. Meanwhile, by designing a transition-metal single-atom catalyst (TM@BiP3), our investigations have shown that embedding a single TM on BiP3 is a feasible route to improving the HER/OER activity by reducing the overpotentials to -0.039 and 0.58 eV for Mo and Os atoms, respectively. In this case, the positive value of the external potential acts as a sufficient OER driving force, i.e., in the light environment, the Os@BiP3 system can promote water molecules spontaneously oxidized into O2 at pH 0-14.

Low Frequency Attenuation Characteristics of Two-Dimensional Hollow Scatterer Locally Resonant Phonon Crystals.

The finite element method (FEM) was applied to study the low frequency band gap characteristics of a designed phonon crystal plate formed by embedding a hollow lead cylinder coated with silicone rubber into four epoxy resin short connecting plates. The energy band structure, transmission loss and displacement field were analyzed. Compared to the band gap characteristics of three traditional phonon crystal plates, namely, the square connecting plate adhesive structure, embedded structure and fine short connecting plate adhesive structure, the phonon crystal plate of the short connecting plate structure with a wrapping layer was more likely to generate low frequency broadband. The vibration mode of the displacement vector field was observed, and the mechanism of band gap formation was explained based on the spring mass model. By discussing the effects of the width of the connecting plate, the inner and outer radii and height of the scatterer on the first complete band gap, it indicated that the narrower the width of the connecting plate, the smaller the thickness; the smaller the inner radius of the scatterer, the larger the outer radius; and the higher the height, the more conducive it is to the expansion of the band gap.

Ultralow-iridium content NiIr alloy derivative nanochain arrays as bifunctional electrocatalysts for overall water splitting.

The development of low-cost and high-durability bifunctional electrocatalysts is of considerable importance for overall water splitting (OWS). This work reports the controlled synthesis of nickel-iridium alloy derivative nanochain array electrodes (NiIrx NCs) with fully exposed active sites that facilitated mass transfer for efficient OWS. The nanochains have a self-supported three-dimensional core-shell structure, composed of a metallic NiIrx core and a thin (5-10 nm) amorphous (hydr)oxide film as the shell (e.g., IrO2/NiIrx and Ni(OH)2/NiIrx). Interestingly, NiIrx NCs have bifunctional properties. Particularly, the oxygen evolution reaction (OER) current density (electrode geometrical area) of NiIr1 NCs is four times higher than that of IrO2 at 1.6 V vs. RHE. Meanwhile, its hydrogen evolution reaction (HER) overpotential at 10 mA cm-2 (η10 = 63 mV) is comparable to that of 10 wt% Pt/C. These performances may originate from the interfacial effect between the surface (hydr)oxide shell and metallic NiIrx core, which facilitates the charge transfer, along with the synergistic effect between Ni2+ and Ir4+ in the (hydr)oxide shell. Furthermore, NiIr1 NCs exhibits excellent OER durability (100 h @ 200 mA cm-2) and OWS durability (100 h @ 500 mA cm-2) with the nanochain array structure well preserved. This work provides a promising route for developing effective bifunctional electrocatalysts for OWS applications.

S-Scheme Porphyrin Covalent Organic Framework Heterojunction for Boosted Photoelectrochemical Immunoassays in Myocardial Infarction Diagnosis.

Cardiac troponin I (cTnI) is an extremely sensitive biomarker for early indication of acute myocardial infarction (AMI). However, it still remains a tough challenge for many newly developed cTnI biosensors to achieve superior sensing performance including high sensitivity, rapid detection, and resistance to interference in clinical serum samples. Herein, a novel photocathodic immunosensor toward cTnI sensing has been successfully developed by designing a unique S-scheme heterojunction based on the porphyrin-based covalent organic frameworks (p-COFs) and p-type silicon nanowire arrays (p-SiNWs). In the novel heterojunction, the p-SiNWs are employed as the photocathode platform to acquire a strong photocurrent response. The in situ-grown p-COFs can accelerate the spatial migration rate of charge carriers by forming proper band alignment with the p-SiNWs. The crystalline π-conjugated network of p-COFs with abundant amino groups also promotes the electron transfer and anti-cTnI immobilizing process. The developed photocathodic immunosensor demonstrates a broad detection range of 5 pg/mL-10 ng/mL and a low limit of detection (LOD) of 1.36 pg/mL in clinical serum samples. Besides, the PEC sensor owns several advantages including good stability and superior anti-interference ability. By comparing our results with that of the commercial ELISA method, the relative deviations range from 0.06 to 0.18% (n = 3), and the recovery rates range from 95.4 to 109.5%. This work displays a novel strategy to design efficient and stable PEC sensing platforms for cTnI detection in real-life serums and provides guidance in future clinical diagnosis.

UWB Localization Based on Improved Robust Adaptive Cubature Kalman Filter.

Aiming at the problems of Non-Line-of-Sight (NLOS) observation errors and inaccurate kinematic model in ultra-wideband (UWB) systems, this paper proposed an improved robust adaptive cubature Kalman filter (IRACKF). Robust and adaptive filtering can weaken the influence of observed outliers and kinematic model errors on filtering, respectively. However, their application conditions are different, and improper use may reduce positioning accuracy. Therefore, this paper designed a sliding window recognition scheme based on polynomial fitting, which can process the observation data in real-time to identify error types. Simulation and experimental results indicate that compared to the robust CKF, adaptive CKF, and robust adaptive CKF, the IRACKF algorithm reduces the position error by 38.0%, 45.1%, and 25.3%, respectively. The proposed IRACKF algorithm significantly improves the positioning accuracy and stability of the UWB system.

Anisotropic Growth of Centimeter-Size CsCu2 I3 Single Crystals with Ultra-Low Trap Density for Aspect-Ratio-Dependent Photodetectors.

Low-dimensional ternary copper iodide metal halide with strong quantum confinement effects has made great progress in optoelectronic fields. However, efficient regulation of anisotropic growth of metal halides single crystal still remains a great challenge. Herein, 2 cm size CsCu2 I3 single crystals with tunable aspect ratio and the trap states (ntrap ) as low as 5.38 × 109  cm-3 are fabricated by optimized anti-solvent vapor-assisted method, in which the growth cycle is shortened by half. Evidenced by real-time observation and the LaMer growth model, the rapid and anisotropic growth mechanism is ascribed to preferential 1D growth, promoted by high concentration and fast vapor rate. Furthermore, the aspect-ratio-dependent optoelectronic performance is observed, the on-off ratio for 2 cm CsCu2 I3 single crystal are enhanced 350 times compared with those of short and thick single crystal, which shows ultrahigh on-off ratio of 1570, D* of 1.34 × 1012  Jones, Rλ of 276.94 mA W-1 , t rise /t decay of 0.37 and 1.08 ms, and EQE of 95.53%, which are clearly at very high level among lead-free perovskite-based photodetectors. This study not only provides a new strategy for overcoming anisotropic growth limitations of low-dimensional metal halides, but also paves a way for high-performance optoelectronic applications.

FeS combined ozonation to remove p-aminobenzenesulfonamide from water: Density functional theory insights into the mechanism.

The applicability and performance of FeS in ozonation process to remove p-aminobenzenesulfonamide (SN) from water was assessed, and the working mechanism of FeS was comprehensively explored by both experimental means and density functional theory (DFT) simulation. FeS combined ozonation achieved 74% of SN removal in 60 min under the optimal condition, which was 37% higher than by ozonation alone, and 12% higher than FeO combined ozonation. Highly active species of •OH, •SO4-, 1O2 and •O2- were detected in the FeS combined ozonation system, the evolution pathway of the involved species was expounded with the aid of DFT calculation. The results revealed that •O2-, H2O2 and SO42- were originally formed via interface reactions on FeS surface, then gradually transformed into •OH, 1O2 and •SO4- through subsequent chain reactions. Moreover, FeS had a lower energy barrier of 0.16 eV than FeO with a value of 0.83 eV for the transformation of ozone to active atomic oxygen. The presented study provided a significant insight into the role of Fe-based materials in ozonation, and was of great importance to guide the route for ozonation process improvement.