Rational design of biogenic PdxAuy nanoparticles with enhanced catalytic performance for electrocatalysis and azo dyes degradation.

The green biogenic PdAu nanoparticles (bio-PdAu NPs) exhibits remarkable catalytic performance in hydrogenation, which is highly desired. However, the catalytic principles and effectiveness of bio-PdxAuy NPs in response to various catalytic systems (electrocatalysis and suspension-catalysis) are unclear. Herein, a facile synthetic strategy for bio-PdxAuy NPs synthesis with controlled size and the catalytic principles for hydrogen evolution reaction (HER) and azo dye degradation is reported. In the biosynthetic process, the size and composition of the bio-PdxAuy NPs could be precisely controlled by predesigning the precursor mass ratio of Pd/Au, and the Au proportion showed a linear relationship with the size of NPs (R2 = 0.92). The obtained bio-PdxAuy NPs exhibit variable activity in electrocatalysis (HER) and suspension-catalysis (azo dye degradation). For electrocatalysis, the formation of conductive networks that facilitates the extracellular electron transfer is crucial. It was revealed that the bio-Pd2Au8 exhibited superior electrocatalytic performance in HER/toward hydrogen evolution, with a maximum current density of 1.65 mA cm-2, which was 1.54 times higher than that commercial Pd/C (1.07 mA cm-2). The high electrocatalytic activity was attributed to its appropriate size (81.38 ± 6.14 nm) and uniform distribution on the cell surface, which promoted the extracellular electron transfer by constructing a conductive network between catalyst and electrode. However, for suspension-catalysis, the size effect and synergistic effect of bimetallic NPs have a more prominent effect on the degradation of azo dyes. As the increase of Au proportion the particle size decreases, and the catalytic activity of bio-PdxAuy improved significantly. The response principles of bio-PdxAuy proposed in this study provide a reliable reference for the rational design of bio-based bimetallic catalysts with enhanced catalytic performance.

Shewanella oneidensis MR-1 self-assembled Pd-cells-rGO conductive composite for enhancing electrocatalysis.

Biosynthesized noble metal nanoparticles (NPs) as promising green catalysts for electrochemical application has invited a lot of attention. However, effective electron transfer between biosynthesized NPs and electrode remains a challenge due to the uncontrollable and poor conductive property of cell substrates. In this study, graphene oxide (GO) was introduced into a bio-Pd synthesis process governed by Shewanella oneidensis MR-1, which was demonstrated to be simultaneously reduced with Pd(II) and transformed to reduced GO (rGO), resulting in the formation of a Pd-cells-rGO composite. Compared to the control without rGO (Pd-cells), the electrochemical conductivity of Pd-cells-rGO composite increased from almost zero to 196 µS cm-1, indicating the rGO facilities the electron transport across the composite. Electrochemical characterizations revealed the electrochemical active surface area (ECSA) of Pd in Pd-cells-rGO was enlarged by increasing the amount of rGO in the composite, clearly indicating that the conductive network created by rGO enable the Pd NPs receive electrons from electrode and become electrochemical active. A considerable enhancement of electrocatalytic activity was further confirmed for Pd-cells-rGO as indicated by 36.7- and 17.2-fold increase (Pd-cells-rGO with Pd/GO ratio of 5/1 vs Pd-cells) of steady state current density toward hydrogen evolution and nitrobenzene reduction at -0.7 V and -0.55 V vs Ag/AgCl, respectively. We also compared the electrocatalytic performance with MWCNTs hybrids Pd-cells-CNTs. It was found that the association of Pd, cells and rGO creates an interactive and synergistic environment to allow higher conductivity and catalytic activity under the same amount of carbon nanomaterial. The strategy developed in this work activates a highly reactive NPs and proposed a designable protocol for enhancing electrocatalytic activity of biocatalysts.

A pillar[5]arene-based multiple-stimuli responsive metal-organic gel was constructed for facile removal of mercury ions.

A thioacetohydrazide functionalized pillar[5]arene was synthesized, which could further assemble into a linear supramolecular metal-organic polymer upon adding Zn2+. Furthermore, the obtained linear supramolecular metal-organic polymer could self-assemble to form a fluorescent supramolecular metal-organic gel at high concentration. When TBAOH was added to the viscous solution at high temperature, the obtained solution could not form a supramolecular metal-organic gel upon cooling. More importantly, when Hg2+ ions are added to the metal-organic gel, the strong blue fluorescence is clearly quenched, and this metal-organic gel (xerogel) could effectively remove Hg2+ from water. Simultaneously, a thin film based on the metal-organic gel was prepared, which was confirmed to be a convenient test kit for detecting Hg2+.

MiR-125a Rs12976445 Polymorphism is Associated with the Apoptosis Status of Nucleus Pulposus Cells and the Risk of Intervertebral Disc Degeneration.

BACKGROUND: Spinal degenerative diseases are a major health problem and social burden worldwide. Intervertebral disc degeneration (IDD) is the pathological basis of spinal degenerative diseases and is characterized by loss of nucleus pulposus cells due to excessive apoptosis caused by various factors. MicroRNAs (miRNAs) have been reported to be functionally involved in the control of apoptosis. METHODS: computational analysis and luciferase assay were used to identify the target of miR-125a, and cell culture, transfection were used to confirm such relationship. Sequencing was used to determine the genotype of each participant. RESULTS: We confirmed the previous report that the presence of the minor allele (T) of rs12976445 polymorphism significantly downregulated the expression level of miR-125a in nucleus pulposus cells, leading to less efficient inhibition of its target gene. We also validated TP53INP1 as a target of miR-125a in nucleus pulposus cells using a dual luciferase reporter system, and the transfection of miR-125a significantly reduced the expression of TP53INP1. The expression level of TP53INP1 was significantly lower in nucleus pulposus cells genotyped as CT or TT than in those genotyped as CC, and the apoptosis rate was consistently lower in the CC group than in the nucleus pulposus cells collected from individuals carrying at least one minor allele of rs12976445 polymorphism. To study the association between rs12976445 polymorphism and the risk of IDD, we enrolled 242 patients diagnosed with IDD and 278 normal controls, and significant differences were noted regarding the genotype distribution of rs12976445 between the IDD and the control groups (OR = 2.69, 95% C.I. = 1.88-3.83, p < 0.0001). In summary, rs12976445 polymorphism is significantly associated with the risk of IDD in the Chinese population. CONCLUSION: The present study indicated that miR-125a is a promising potential target for patients with IDD in clinical practice.

Spatial difference on nitrogen removal in the water based on different resolutions for Sanhuanpao wetland, Northeast China.

The research on the deviations caused by different resolutions is relevant to the study of spatial scale effects. In 2018, spatial interpolations were performed using the removal ratios of the TN, NH4-N, and NO3-N of the layers of different resolutions, respectively. Based on the mean and the standard deviation, the area, shape, and position were obtained for four levels related to the removal ratios of the three nitrogen forms. The linear and 6th function fitting methods were used to reveal the differences in nitrogen removal in wetland water at different spatial resolutions. The results showed that a resolution of 25 times the original was the key scale of the spatial effects. Due to the fact that 52 of the 72 functions did not reach a significant level (P < 0.05), the spatial scale effect of the nitrogen removal was mainly characterized by disorderly fluctuations. The results have a certain extrapolation value for the analysis of spatial scale effects. PRACTITIONER POINTS: The resolution difference was not sufficient to change the spatial pattern of the geographic phenomena. The resolution of 25 times the original was the important scale for determining spatial effects. When studying the spatial scale effects caused by differences in resolution, it was necessary to comprehensively consider various resolutions.

Safe and potent anti-CD19 CAR T-cells with shRNA-IL-6 gene silencing element in patients with refractory or relapsed B-cell acute lymphoblastic leukemia.

Severe cytokine release syndrome (sCRS) and immune effector cell-associated neurotoxicity syndrome (ICANS) have limited the widespread use of chimeric antigen receptor T (CAR T)-cell therapy. We designed a novel anti-CD19 CAR (ssCART-19) with a small hairpin RNA (shRNA) element to silence the interleukin-6 (IL-6) gene, hypothesizing it could reduce sCRS and ICANS by alleviating monocyte activation and proinflammatory cytokine release. In a post hoc analysis of two clinical trials, we compared ssCART-19 with common CAR T-cells (cCART-19) in relapsed/refractory B-cell acute lymphoblastic leukemia (r/r B-ALL). Among 87 patients, 47 received ssCART-19 and 40 received cCART-19. Grade ≥3 CRS occurred in 14.89% (7/47) of the ssCART-19 group versus 37.5% (15/40) in the cCART-19 group (p = 0.036). ICANS occurred in 4.26% (2/47) of the ssCART-19 group (all grade 1) compared to 15% (2/40) of the cCART-19 group. Patients in the ssCART-19 group showed comparable rates of treatment response (calculated with rates of complete remission and incomplete hematological recovery) were 91.49% (43/47) for ssCART-19 and 85% (34/40) for cCART-19 (p = 0.999). With a median follow-up of 21.9 months, cumulative nonrelapse mortality was 10.4% for ssCART-19 and 13.6% for cCART-19 (p = 0.33). Median overall survival was 37.17 months for ssCART-19 and 32.93 months for cCART-19 (p = 0.40). Median progression-free survival was 24.17 months for ssCART-19 and 9.33 months for cCART-19 (p = 0.23). These data support the safety and efficacy of ssCART-19 for r/r B-ALL, suggesting its potential as a promising therapy.

Clinical development of mRNA therapies against solid tumors.

The mRNA-based therapeutics have become the hot spot of biopharmaceutical industries in recent years. The landscape of this area is expanding from infectious disease to cancer, which needs to be summarized to provide data supports for industries and research institutions. Based on the Trialtrove database, a total of 108 clinical trials from 1999 to 2021 were retrospectively analyzed. We have demonstrated that the clinical development of mRNA therapies against solid tumors is still at an early stage. There are evolutions in delivery systems from the dendritic cell to the lipid-based platform and in encoding strategies from the fixed tumor antigens to the personalized neoantigens. The adjuvant or maintenance therapy and the combination treatment with checkpoint inhibitors are becoming the major clinical development orientation.

[Correlation analysis of serum CTRP3 and PGC-1α expression with traumatic fracture healing].

OBJECTIVE: To investigate the relationship between serum C1q/tumor necrosis factor-related protein-3(CTRP3) and peroxisome proliferator-activated receptor γ coactivator-1α(PGC-1α) on predictive value of expression level on fracture healing. METHODS: From January 2019 to January 2020, 80 patients with traumatic tibial plateau fractures were treated by internal fixation with support plates through the posterior approach of the knee joint. The patients were followed up for 12 months. According to the criteria for delayed fracture healing, the patients were divided into two groups:54 patients in fracture healing group included 24 males and 30 females, aged 29 to 75 years old with an average of (52.36±13.17) years;In the delayed healing group, there were 26 cases, 13 males and 13 females, aged from 29 to 75 with an average od (53.82±13.52) years. The serum levels of CTRP3, PGC-1αand 25 hydroxyvitamin D3[25(OH)D3] in patients with traumatic fracture were detected by enzyme-linked immunosorbent assay(ELISA);Blood phosphorus and calcium levels were measured by automatic biochemical analyzer, and the product of calcium and phosphorus was calculated;Pearson's method was used to analyze the correlation between serum CTRP3, PGC-1αand bone biochemical indexes in patients with delayed union one week after operation;The predictive value of serum levels of CTRP3 and PGC-1αon traumatic fracture healing was analyzed by receiver operating characteristic curve(ROC curve). RESULTS: PGC-1α, calcium phosphorus product and 25(OH)D3 in the fracture healing group were higher than those in the delayed healing group at 1 and 4 weeks after operation(P<0.05). Serum CTRP3 was positively correlated with PGC-1α(r=0.637, P<0.05) and positively correlated with calcium phosphorus product and 25(OH)D3(P<0.05). The areas under the curve(AUC) of serum ctrp3 and PGC-1α levels in predicting traumatic fracture healing were 0.845 and 0.855, respectively. The cutoff values were 188.678 pg/ml and 2.697 ng/ml, respectively. The specificity was 96.2% and 80.8%, and the sensitivity was 53.7% and 77.8%;The predicted AUC was 0.904, the specificity was 88.5%, and the sensitivity was 81.5%. CONCLUSION: The serum levels of CTRP3 and PGC-1 in patients with delayed union of traumatic fracture at 1 and 4 weeks after operation α The expression level is of certain reference value to predict the fracture healing status of patients.

Two new iridoid glycosides from the fruit of Gardenia jasminoides.

Two new iridoid glycosides, 2'-O-cis-coumaroylgardoside (1), and 6'-O-caffeoylioxide (2), were isolated from the fruit of Gardenia jasminoides. The structures of these compounds were elucidated based on spectroscopic analysis (HR-ESI-MS, NMR) and chemical methods. The anti-inflammatory activities of the isolates were evaluated by measuring their inhibitory effects on PGE2 production in LPS stimulated RAW 264.7 macrophages, compounds 1 and 2 could reduce PGE2 levels in LPS-activated RAW 264.7 macrophages with IC50 values of 121.4 and 83.38 µM, respectively.

[Study on quantitative model for suspended sediment concentration in Taihu Lake].

The complicated compositions of Case II waters result in the complex properties of spectral curves. The present paper analyzed the in situ measurements data of spectral curves, and further realized the relationships between the properties of spectral curves and suspended sediment concentration. The study found that the max peak of spectral curves was moving to the direction of shortwavelength as increasing suspended sediment concentration, namely the blue shift of wavelength; the area enclosed by spectral curve and coordinate axis in the range of sensitive bands had preferably linear relationship with the suspended sediment concentration (curve area model); the trapezoidal area model which was an approximation of curve area model could also excellently reflect those relationships, and be greatly suitable for multi-spectral satellite imagery retrieval such as LandSat/TM, MODIS and so on. The inversion results of trapezoidal area model for LandSat/TM imagery on October 27, 2003 in Taihu Lake showed that the suspended sediment concentration ranged from 30 to 80 mg x L(-1), the distribution pattern was higher in the west, south and central lake and lower in the east lake; compared with the in situ measurements in the regions, and the relative error of retrieval model was 6.035%.

Insight into the electrocatalytic performance of in-situ fabricated electroactive biofilm-Pd: The role of biofilm thickness, initial Pd(II) concentration and the exposure time to Pd precursor.

Biogenic palladium (bio-Pd) nanoparticles have been considered as promising biocatalyst for energy generation and contaminants remediation in water and sediment. Recently, an electroactive biofilm-Pd (EAB-Pd) network, which can be used directly as electrocatalyst and show enhanced electrocatalytic performance, has exhibited tremendous application potential. However, the information regarding to the controllable biosynthetic process and corresponding catalytic properties is scarce. This study demonstrated that the catalytic performance of EAB-Pd could be influenced by Pd loading on bacteria cells (Pd/cells), which was crucial to determine the final distribution characteristic of Pd nanocrystal on EAB skeleton. For instance, the high Pd/cells (over 0.18 pg cell-1) exhibited almost 6-fold and 1.5-fold enhancement over EAB-Pds with Pd/cells below 0.03 in catalytic current toward hydrogen evolution reaction and nitrobenzene reduction, respectively. In addition, the Pd/cells was found to be affected by the synthesis factors, such as the ratio of biomass to initial Pd(II) concentration (cells/PdII) and the exposure time of EAB to Pd(II) precursor solution. The Pd/cells increased significantly as the cell/PdII ratio decreased from ~5.5 × 107 to ~1.3 × 107 cells L mg-1 or the prolongation of exposure time from 3 h to 24 h. The findings developed in this work extensively expand our knowledge for the in-situ designing biogenic electrocatalyst and provide important information for the development of its catalytic property.

[Outcomes of posterior C(1-2) fusion for atlantoaxial instability or dislocation using pedicle screws of atlas and axis].

OBJECTIVE: To retrospectively analyze and evaluate the results of treatment for atlantoaxial instability or dislocation employing pedicle screws of atlas and axis. METHODS: Thirty-one patients (23 male and 8 female) with atlantoaxial instability or dislocation were stabilized using pedicle screws of atlas and axis between May 2005 to January 2008. The patients ranged in age from 17 to 67 years (mean 43.5 years). Patients consisted of chronic odontoid fracture in 17, Os odontoideum in 8, fresh odontoid fracture in 4, transverse ligament rupture in 1, rheumatoid arthritis in 1. Clinical features included neck pain in 31; restricted neck movement in 28, varying degrees of spastic quadriparesis in 19. All patients underwent posterior C(1) to C(2) pedicle screw fixation. Operative time, intraoperative blood loss, complications were recorded, neurological and radiographic studies were carried. RESULTS: Mean follow-up time was 13 months. Operative time averaged 2.5 h. Mean intraoperative blood loss was 300 ml. A patient had postoperative wound infection and was treated conservatively with antibiotics and local wound care. A patient developed pulmonary artery embolism and got well with anticoagulation. Satisfactory stability was achieved in all cases with no vascular and C(2) neuralgia. Average JOA score in 19 cases increased at final follow-up (P < 0.01). Solid fusion was achieved in 29 cases, fusion rate was 93.6%. CONCLUSIONS: Stabilization of atlantoaxial complex via pedicle screws of atlas and axis has advantages of intraoperative restoration, easier placement of screw, solid fixation. It is a safe and effective treatment modality for posterior C(1-2) fusion.

Protective effect of CDDO-ethyl amide against high-glucose-induced oxidative injury via the Nrf2/HO-1 pathway.

BACKGROUND CONTEXT: Intervertebral disc degeneration (IDD) is the main cause of low back pain, and nucleus pulposus (NP) cell apoptosis is an important risk factor of IDD. However, the molecular mechanism of this disease remains unknown. PURPOSE: To assess the potential protective effect of CDDO-ethyl amide (EA) against high-glucose-induced oxidative stress injury in NP cells and to investigate the mechanism of antioxidative effects and apoptotic inhibition. STUDY DESIGN/SETTING: To find new molecule to inhibit intervertebral disc degeneration. METHODS: Viability, reactive oxygen species (ROS) levels, and apoptosis were examined in NP cells. The protein expression levels of HO-1 and Nrf2 were measured through Western blot RESULTS: CDDO-EA elicited cytoprotective effects against NP cell apoptosis and ROS accumulation induced by high glucose. CDDO-EA treatment increased the HO-1 and Nrf2 expression abrogated by HO-1, Nrf2, and mitogen-activated protein kinase inhibitors. CONCLUSIONS: The phosphorylation and nuclear translocation of Nrf2 are crucial for HO-1 overexpression induced by CDDO-EA, which is essential for the cytoprotection against high-glucose-induced oxidative stress in NP cells.