Spatial Heterogeneity and Strong Coupling of FeII /FeIII in an Individual Metal-Organic Framework Nanoparticle for Efficient CO2 Photoreduction.

The synthesis and characterization of an FeII /FeIII metal-organic framework (MOF) nanocrystal with spatial heterogeneity that arises from the non-uniform distribution of different valence states is disclosed. The FeII /FeIII -Ni Prussian blue analog (PBA) delivers superior photocatalytic performance in the selective CO2 reduction reaction thanks to the strong FeII /FeIII coupling, with CO yield up to 12.27 mmol g-1 h-1 and 90.6% selectivity under visible-light irradiation. Density functional theory calculation and experimental studies prove that the spatial heterogeneity of FeII /FeIII in the individual MOF nanocrystal not only directs and expedites the charge transfer within a catalyst particle but also creates the heterogeneity of catalytically-active Ni sites for efficient CO2 photoreduction. The current findings add to a growing literature of materials with compositional heterogeneity and provide a reference for future research.

General and Scalable Synthesis of Mesoporous 2D MZrO2 (M = Co, Mn, Ni, Cu, Fe) Nanocatalysts by Amorphous-to-Crystalline Transformation.

In modern heterogeneous catalysis, it remains highly challenging to create stable, low-cost, mesoporous 2D photo-/electro-catalysts that carry atomically dispersed active sites. In this work, a general shape-preserving amorphous-to-crystalline transformation (ACT) strategy is developed to dope various transition metal (TM) heteroatoms in ZrO2, which enabled the scalable synthesis of TMs/oxide with a mesoporous 2D structure and rich defects. During the ACT process, the amorphous MZrO2 nanoparticles (M = Fe, Ni, Cu, Co, Mn) are deposited within a confined space created by the NaCl template, and they transform to crystalline 2D ACT-MZrO2 nanosheets in a shape-preserving manner. The interconnected crystalline ACT-MZrO2 nanoparticles thus inherit the same structure as the original MZrO2 precursor. Owing to its rich active sites on the surface and abundant oxygen vacancies (OVs), ACT-CoZrO2 gives superior performance in catalyzing the CO2-to-syngas conversion as demonstrated by experiments and theoretical calculations. The ACT chemistry opens a general route for the scalable synthesis of advanced catalysts with precise microstructure by reconciliating the control of crystalline morphologies and the dispersion of heteroatoms.

Reinforcing 2D Single-Crystal Bi2O2CO3 with Additional Interlayer Carbonates by CO2-Assisted Solid-to-Solid Phase Transition.

A facile gaseous CO2 mediated solid-to-solid transformation principle is adopted to insert additional CO3 2- anions into the thin single-crystal nanosheets of Bi2O2CO3, which is built of periodic arrays of intrinsic CO3 2- anions and (Bi2O2)2+ layers. The additional CO3 2- anions create abundant defects. The Bi2O2CO3 nanosheets with rich interlayer CO3 2- exhibit superior electronic properties and charge transfer kinetics than the pristine single-crystal 2D Bi2O2CO3 and display enhanced catalytic activity in photocatalytic CO2 reduction reaction and the photocatalytic oxidative degradation of organic pollutants. This work thus illustrates interlayer engineering as a flexible means to build layered 2D materials with excellent properties.

A lower eGFRcystatin C/eGFRcreatinine ratio is associated with greater cardiovascular risk (higher Framingham Risk Score) in Chinese patients with newly diagnosed type 2 diabetes mellitus.

BACKGROUND: Cardiovascular disease (CVD) is the leading cause of mortality in type 2 diabetes mellitus (T2DM) patients. Shrunken pore syndrome (SPS) is defined as eGFRcystatin C/eGFRcreatinine ratio <0.70 and predicts high CVD mortality. The Framingham Risk Score (FRS) is used to estimate an individual's 10-year CVD risk. This study investigated the association between FRS and eGFRcystatin C/eGFRcreatinine ratio in T2DM patients. METHODS: Patients aged 18-80 years who were newly diagnosed with T2DM were included in this retrospective study. Ordinal logistic regression analysis was used to investigate the association between risk factors of T2DM and FRS. A Generalized Linear Model was used to calculate odds ratios (OR) and 95% confidence intervals (CI). RESULTS: There were 270 patients included in the study. Only 27 patients (10%) met the diagnostic criteria of SPS. Ordinal logistic regression analysis showed that SPS was not correlated with FRS risk (OR = 1.99, 95%CI = 0.94-4.23, p = 0.07), whereas eGFRcystatin C/eGFRcreatinine (OR = 0.86, 95%CI = 0.77-0.97, p = 0.01) showed a significant negative association with FRS risk. Compared with eGFRcystatin C/eGFRcreatinine>0.85, eGFRcystatin C/eGFRcreatinine≤0.85 increased FRS risk (OR = 1.95, 95%CI = 1.18-3.21, p < 0.01). After adjustment for confounding factors, increased eGFRcystatin C/eGFRcreatinine ratio was associated with decreased FRS risk when considered as a continuous variable (OR = 0.87, 95%CI = 0.77-0.99, p = 0.03). The FRS risk in patients with eGFRcystatin C/eGFRcreatinine≤0.85 is 1.86 times higher than that in patients with eGFRcystatin C/eGFRcreatinine>0.85 (OR = 1.86, 95%CI = 1.08-3.21, p = 0.03). CONCLUSIONS: In the current study, no significant association between SPS and FRS was identified. However, lower eGFRcystatin C/eGFRcreatinine and eGFRcystatin C/eGFRcreatinine≤0.85 were associated with a significantly increased CVD risk in T2DM.

Localized Phase Transformation Triggering Lattice Matching of Metal Oxide and Carbonate Hydroxide for Efficient CO2 Photoreduction.

Orderly heterostructured catalysts, which integrate nanomaterials of complementary structures and dimensions into single-entity structures, have hold great promise for sustainability applications. In this work, it is showcased that air as green reagent can trigger in situ localized phase transformation and transform the metal carbonate hydroxide nanowires into ordered heterostructured catalyst. In single-crystal nanowire heterostructure, the in situ generated and nanosized Co3 O4 will be anchored in single-crystal Co6 (CO3 )2 (OH)8 nanowires spontaneously, triggered by the lattice matching between the (220) plane of Co3 O4 and the (001) plane of Co6 (CO3 )2 (OH)8 . The lattice matching allows intimate contact at heterointerface with well-defined orientation and strong interfacial coupling, and thus significantly expedites the transfer of photogenerated electrons from tiny Co3 O4 to catalytically active Co6 (CO3 )2 (OH)8 in single-crystal nanowire, which elevates the catalytic efficiency of metal carbonate catalyst in the CO2 reduction reaction (VCO = 19.46 mmol g-1 h-1 and VH2 = 11.53 mmol g-1 h-1 ). The present findings add to the growing body of knowledge on exploiting Earth-abundant metal-carbonate catalysts, and demonstrate the utility of localized phase transformation in constructing advanced catalysts for energy and environmental sustainability applications.

Scalable Synthesis of Holey Deficient 2D Co/NiO Single-Crystal Nanomeshes via Topological Transformation for Efficient Photocatalytic CO2 Reduction.

Preparation of holey, single-crystal, 2D nanomaterials containing in-plane nanosized pores is very appealing for the environment and energy-related applications. Herein, an in situ topological transformation is showcased of 2D layered double hydroxides (LDHs) allows scalable synthesis of holey, single-crystal 2D transition metal oxides (TMOs) nanomesh of ultrathin thickness. As-synthesized 2D Co/NiO-2 nanomesh delivers superior photocatalytic CO2 -syngas conversion efficiency (i.e., VCO of 32460 µmol h-1 g-1 CO and V H 2 ${V_{{{\rm{H}}_2}}}$ of 17840 µmol h-1 g-1 H2 ), with VCO about 7.08 and 2.53 times that of NiO and 2D Co/NiO-1 nanomesh containing larger pore size, respectively. As revealed in high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), the high performance of Co/NiO-2 nanomesh primarily originates from the edge sites of nanopores, which carry more defect structures (e.g., atomic steps or vacancies) than basal plane for CO2 adsorption, and from its single-crystal structure adept at charge transport. Theoretical calculation shows the topological transformation from 2D hydroxide to holey 2D oxide can be achieved, probably since the trace Co dopant induces a lattice distortion and thus a sharp decrease of the dehydration energy of hydroxide precursor. The findings can advance the design of intriguing holey 2D materials with well-defined geometric and electronic properties.

Thin In-Plane In2 O3 /ZnIn2 S4 Heterostructure Formed by Topological-Atom-Extraction: Optimal Distance and Charge Transfer for Effective CO2 Photoreduction.

Exploitation of atomic-level principles to optimize the charge transfer on ultrathin 2D heterostructures is an emerging frontier in relieving the energy and environmental crisis. Herein, a facile "topological-atom-extraction" protocol is disclosed, i.e., selective extraction of Zn from ultrathin half-unit-cell ZnIn2 S4 (HZIS) can embed thin In2 O3 domain into 1.60 nm thick HZIS layer to create an atomically thin in-plane In2 O3 /HZIS heterostructure. Thanks to the optimal distance and capability of charge separation, the in-plane In2 O3 /HZIS heterostructure is among the best ZnIn2 S4 -based CO2 reduction reaction (CRR) photocatalysts, and indeed demonstrates a significant increase (from 6.8- to 128-fold) in CO production rate compared with those of out-plane ZIS@In2 O3 and out-plane In2 O3 -HZIScalcined heterostructures. Density Functional Theory simulation reveals that whereas the out-plane heterostructure has a much smaller ∆q of 0.2-0.25 e, the in-plane heterostructure with "zero distance contact" has an optimal ∆q of 1.05 e between In2 O3 and HZIS that induces remarkable charge redistribution on the in-plane heterojunction interface and creates local electric field confined within the ultrathin layer. The charge redistribution efficiently directs the charge-carrier separation in S-scheme photocatalytic system and endows long-lifetime carrier to CRR active HZIS. The findings demonstrate the strong versatility of engineering atomic-level heterojunctions for efficient catalysts design.

Role of composite objective nutritional indexes in patients with chronic kidney disease.

Malnutrition persists as one of the most severe symptoms in patients with chronic kidney disease (CKD) globally. It is a critical risk factor for cardiovascular and all-cause mortality in patients with CKD. Readily available objective indicators are used to calculate composite objective nutritional assessment indexes, including the geriatric nutritional risk index, prognostic nutritional index, and controlling nutritional status score. These indexes offer a straightforward and effective method for evaluating nutritional status and predicting clinical outcomes in patients with CKD. This review presents supporting evidence on the significance of composite nutritional indexes.

The predictive value of free thyroxine combined with tubular atrophy/interstitial fibrosis for poor prognosis in patients with IgA nephropathy.

Background: IgA nephropathy (IgAN), the most common type of glomerulonephritis, has great individual differences in prognosis. Many studies showed the relationship between thyroid hormones and chronic kidney disease. However, the relationship between free thyroxine (FT4), as a thyroid hormone, and IgAN is still unclear. This study aimed to evaluate the impact of FT4 on IgAN prognosis. Methods: This retrospective study involved 223 patients with biopsy-proven IgAN. The renal composite outcomes were defined as: (1) ESRD, defined as eGFR < 15 ml/(min·1.73 m2) or initiation of renal replacement therapy (hemodialysis, peritoneal dialysis, renal transplantation); (2) serum creatinine doubled from baseline; (3) eGFR decreased by more than 50% from baseline. The predictive value was determined by the area under the curve (AUC). Kaplan-Meier and Cox proportional hazards analyses assessed renal progression and prognosis. Results: After 38 (26-54) months of follow-up, 23 patients (10.3%) experienced renal composite outcomes. Kaplan-Meier survival curve analysis showed that the renal survival rate of the IgAN patients with FT4<15.18pmol/L was lower than that with FT4≥15.18pmol/L (P < 0. 001). Multivariate Cox regression model analysis showed that FT4 was a protective factor for poor prognosis of IgAN patients, whether as a continuous variable or a categorical variable (HR 0.68, 95%CI 0.51-0.90, P =0.007; HR 0.04, 95%CI 0.01-0.20, P <0.001). ROC curve analysis showed that FT4 combined with t score had a high predictive value for poor prognosis of IgAN patients (AUC=0.881, P<0.001). Conclusion: FT4 was a protective factor for IgAN. In addition, FT4 combined with tubular atrophy/interstitial fibrosis had a high predictive value for poor prognosis of IgAN.

Simultaneous determination of volatile phenol, cyanide, anionic surfactant, and ammonia nitrogen in drinking water by a continuous flow analyzer.

This study developed a method for the simultaneous determination of volatile phenol, cyanide, anionic surfactant, and ammonia nitrogen in drinking water, using a continuous flow analyzer. The samples were first distilled at 145 °C. The phenol in the distillate then subsequently reacted with alkaline ferricyanide and 4-aminoantipyrine to form a red complex that was measured colorimetrically at 505 nm. Cyanide in the distillate subsequently reacted with chloramine T to form cyanogen chloride, which then formed a blue complex with pyridinecarboxylic acid that was measured colorimetrically at 630 nm. The anionic surfactant reacted with basic methylene blue to form a compound that was extracted into chloroform and washed with acidic methylene blue to remove interfering substances. The blue compound in chloroform was determined colorimetrically at 660 nm. Ammonia reacted with salicylate and chlorine from dichloroisocyanuric acid to produce indophenol blue at 37 °C in an alkaline environment that was measured at 660 nm. The relative standard deviations were 0.75-6.10% and 0.36-5.41%, respectively, and the recoveries were 96.2-103.6% and 96.0-102.4% when the mass concentration of volatile phenol and cyanide was in the range of 2-100 µg/L. The linear correlation coefficients were ≥ 0.9999, and the detection limits were1.2 µg/L and 0.9 µg/L, respectively. The relative standard deviations were 0.27-4.86% and 0.33-5.39%, and the recoveries were 93.7-107.0% and 94.4-101.7%. When the mass concentration of anionic surfactant and ammonia nitrogen was 10-1000 µg/L. The linear correlation coefficients were 0.9995 and 0.9999, and the detection limits were 10.7 µg/L and 7.3 µg/L, respectively. When compared to the national standard method, no statistically significant difference was found. This approach saves time and labor, has a lower detection limit, higher precision and accuracy, less contamination, and is more appropriate for the analysis and determination of large-volume samples.

Identification and Characterization of a Vancomycin Intermediate-Resistant Staphylococcus haemolyticus Isolated from Guangzhou, China.

Background: Staphylococcus haemolyticus is an opportunistic pathogen that belongs to coagulase-negative Staphylococci (CoNS). Increasing infection and multi-drug resistance cases caused by this strain have been reported and thus it poses a great health threat. Methods: The third-generation sequencing technology was performed on a S. haemolyticus SH-1 isolated from a clinical sample to analyze the drug resistance genes, which included vancomycin resistance related genes. In addition, antimicrobial susceptibility tests, transmission electron microscopy and Triton X-100 stimulated autolysis were conducted to understand its biological characteristics. Results: The study shows that this clinical isolate is a vancomycin intermediate-resistant strain. Genome comparison also revealed that WalK(N70K) and WalK(R280Q) mutations may contribute to the vancomycin resistant phenotype. Besides, S. haemolyticus SH-1 exhibit common features of thicker cell wall and decreased autolytic activity. Conclusion: S. haemolyticus SH-1 with WalKR mutations shows typical characteristics of vancomycin resistant strains. Combining the genome features and biological properties, our findings may provide important information for the understanding of the molecular mechanism of S. haemolyticus to vancomycin intermediate-resistance.

Simultaneous Determination of 11 Aminoglycoside Residues in Honey, Milk, and Pork by Liquid Chromatography with Tandem Mass Spectrometry and Molecularly Imprinted Polymer Solid Phase Extraction.

An analytical method was developed for the simultaneous determination of 11 aminoglycoside (AG) antibiotics, including amikacin, paromomycin, dihydrostreptomycin, gentamicin C1a, hygromycin, kanamycin, netilmicin, spectinomycin, sisomicin, streptomycin, and tobramycin in honey, milk, and pork samples by LC with tandem MS and molecularly imprinted polymer (MIP) SPE. The AG antibiotics in milk and homogenated meat samples were extracted with a solution composed of 10 mmol/L potassium dihydrogen phosphate, 0.4 mmol/L EDTA-Na2, and 2% trichloroacetic acid. For honey samples, the extractant was 50 mmol/L potassium dihydrogen phosphate. The extracts were cleaned up with MIP SPE cartridges. The separation was performed on a zwitter ionic-HILIC column (50 × 2.1 mm, 3.5 µm), with the mobile phase consisting of methanol, 0.3% formic acid, and 175 mmol/L ammonium formate at 0.50 mL/min in gradient elution. A triple-quadrupole mass spectrometer equipped with an electrospray ionization source, which was operated in positive mode, was used for detection. The quantification was based on matrix-matched calibration curves. The method was applied to real samples with three different matrixes. The LODs of the method were 2-30 µg/kg and the LOQs were 7-100 µg/kg; the average recovery ranged from 78.2 to 94.8%; intraday RSDs and interday RSDs were ≤15 and ≤18%, respectively; and the absolute values of matrix effect for all AGs were RSDs ≤23%.