Applications of Metal–Organic Frameworks and Their Derivatives in Electrochemical CO_(2)Reduction

Electrochemically reducing CO_(2)to more reduced chemical species is a promising way that not only enables the conversion of intermittent energy resources to stable fuels,but also helps to build a closed-loop anthropogenic carbon cycle.Among various electrocatalysts for electrochemical CO_(2)reduction,multifunctional metal–organic frameworks(MOFs)have been employed as highly efficient and selective heterogeneous electrocatalysts due to their ultrahigh porosity and topologically diverse structures.Up to now,great progress has been achieved in the design and synthesis of highly active and selective MOF-related catalysts for electrochemical CO_(2)reduction reaction(CO_(2)RR),and their corresponding reaction mechanisms have been thoroughly studied.In this review,we summarize the recent progress of applying MOFs and their derivatives in CO_(2)RR,with a focus on the design strategies for electrocatalysts and electrolyzers.We first discussed the reaction mechanisms for different CO_(2)RR products and introduced the commonly applied electrolyzer configurations in the current CO_(2)RR system.Then,an overview of several categories of products(CO,HCOOH,CH_(4),CH_(3)OH,and multi-carbon chemicals)generated from MOFs or their derivatives via CO_(2)RR was discussed.Finally,we offer some insights and perspectives for the future development of MOFs and their derivatives in electrochemical CO_(2)reduction.We aim to provide new insights into this field and further guide future research for large-scale applications.

Electrochemical CO_(2) reduction:Progress and opportunity with alloying copper

Electroreduction of carbon dioxide(CO_(2)) into value-added chemicals offers an entrancing approach to main-taining the global carbon cycle and eliminating environmental threats.A key obstacle to achieving long-term and large-scale implementation of electrochemical CO_(2) reduction technology is the lack of active and selective cat-alysts.Copper(Cu)is one of the few candidates that can facilitate C–C coupling to obtain high-energy oxygenates and hydrocarbons beyond carbon monoxide(CO),but it suffers from poor selectivity for products of interest and high overpotentials.Alloying is an effective way to break the linear scaling relations and uniquely manipulate the reactivity and selectivity,which is hard to achieve by using monometallic compositions alone.By alloying Cu with other metals,one could change the catalytic properties of the catalyst by tuning the local electronic structure and modulating the adsorption strength of the reaction intermediates,thus improving the catalytic activity and selectivity.In this review,we focus on the recently developed Cu-based alloy catalysts(including conventional alloys,high-entropy alloys and single-atom alloys)that have been applied in electrocatalytic CO_(2) reduction(ECR).Theoretical calculations and experimental advances in understanding the key rate-limiting and selectivity-determining steps in those alloys are summarized,with a particular focus on identifying binding energy de-scriptors and the dynamic product formation mechanisms.In addition,we outline the opportunities and chal-lenges in the fundamental understanding of ECR by recommending advanced in-situ characterization techniques and standardized electrochemical methods and offer atomic-level design principles for steering the reaction pathways to the desired products.

Prostate cancer in Asia:A collaborative report

The incidence of prostate cancer(PCa)within Asian population used to be much lower than in the Western population;however,in recent years the incidence and mortality rate of PCa in some Asian countries have grown rapidly.This collaborative report summarized the latest epidemiology information,risk factors,and racial differences in PCa diagnosis,current status and new trends in surgery management and novel agents for castration-resistant prostate cancer.We believe such information would be helpful in clinical decision making for urologists and oncologists,health-care ministries and medical researchers.

Bipolar transurethral enucleation and resection of the prostate:Whether it is ready to supersede TURP?

Objective:According to the EAU Guidelines,transurethral resection of the prostate(TURP)has so far still been considered as the gold standard for surgical treatment for patients with obstructing clinical benign prostate hyperplasia(BPH).However,its relatively high rate of complications and postoperative recurrence necessitates further modification and innovation on the surgery technique.We reported the patient outcomes with our technique.Methods:We retrospectively analyzed 52 patients with obstructing clinical BPH who underwent bipolar transurethral enucleation and resection of the prostate(B-TUERP)between March 2015 and September 2015.Pre-and perioperative parameters were obtained from medical charts.Postoperative follow-ups were administrated at 1,3,6,12 and 24 month(s)after surgery,respectively.Results:All the operations were performed successfully with a mean operative time of 43.1 min and an average tissue removal rate of 74.7%.Qmax was significantly improved immediately after surgery,followed by a continuous improvement throughout the follow-ups.Following a steep decrease in mean prostate specific antigen(PSA)and post void residual(PVR)observed within the first half year after surgery,the serum PSA was then maintained at a constant level of 0.61 ng/mL.Temporary urinary retention was found in four cases(7.7%).Stress urinary incontinence occurred in five patients(9.6%),with the condition resolved in 1e2 weeks without extra treatment.Urethral strictures and bladder neck contractures,as the most commonly observed long-term complications,developed in four patients(7.7%).No recurrence was found during 2 years of follow-ups.An improvement in International Index of Erectile Function(IIEF-5)scores was witnessed in 17 patients preoperatively with normal sexual function during the first 6 months after surgery,and sustained throughout the 24-month period.Conclusions:Enucleation reflects an improvement on surgical technique in many ways with a need for surgical equipment that can be broadly accessible in clinical practice.Currently,bipolar resection is a commonly employed procedure in clinical settings,and its similarity shared with bipolar enucleation technique warrants a quick learning of B-TUERP by urologists.Based on these findings,we believe that the substitution of TURP by TUERP as the gold standard for prostate endoscopic procedure can be expected in the future.

Percent free prostate-specific antigen for prostate cancer diagnosis in Chinese men with a PSA of 4.0-10.0 ng/mL:Results from the Chinese Prostate Cancer Consortium

Objective:To test the diagnostic performance of percent free prostate-specific antigen(%fPSA)in predicting any prostate cancer(PCa)and high-grade prostate cancer(HGPCa)in a retrospective multi-center biopsy cohort with a PSA level of 4.0e10.0 ng/mL in China.Methods:Consecutive patients with a PSA of 4.0-10.0 ng/mL who underwent transrectal ultrasound-guided biopsy were enrolled at 16 Chinese medical centers from January 1st,2010 to December 31st,2013.Total and free serum PSA determinations were performed using three types of electro-chemiluminescence immunoassays recalibrated to the World Health Organization(WHO)standard.The diagnostic accuracy of PSA,%fPSA,and %fPSA in combination with PSA(%fPSA t PSA)was determined using the area under the receiver operating characteristic(ROC)curve(AUC).Results:A total of 2310 consecutive men with PSA levels between 4.0 and 10.0 ng/mL were included,and the detection rate of PCa was 25.1%.The AUC of%fPSA and %fPSA t PSA in predicting any PCa was superior to PSA alone in men aged≥60 years(0.623 vs.0.534,p<0.0001)but not in men aged 40e59 years(0.517 vs.0.518,p=0.939).Similar result was yield in predicting HGPCa.Conclusion:In a clinical setting of Chinese men with 4.0e10.0 ng/mL PSA undergoing initial prostate biopsy,adding %fPSA to PSA can moderately improve the diagnostic accuracy for any PCa and HGPCa compared with PSA alone in patients≥60 but not in patients aged 40-59 years.

The chromosome-level Stevia genome provides insights into steviol glycoside biosynthesis

Stevia(Stevia rebaudiana Bertoni)is well known for its very sweet steviol glycosides(SGs)consisting of a common tetracyclic diterpenoid steviol backbone and a variable glycone.Steviol glycosides are 150–300 times sweeter than sucrose and are used as natural zero-calorie sweeteners.However,the most promising compounds are biosynthesized in small amounts.Based on Illumina,PacBio,and Hi-C sequencing,we constructed a chromosome-level assembly of Stevia covering 1416 Mb with a contig N50 value of 616.85 kb and a scaffold N50 value of 106.55 Mb.More than four-fifths of the Stevia genome consisted of repetitive elements.We annotated 44,143 high-confidence protein-coding genes in the high-quality genome.Genome evolution analysis suggested that Stevia and sunflower diverged~29.4 million years ago(Mya),shortly after the whole-genome duplication(WGD)event(WGD-2,~32.1 Mya)that occurred in their common ancestor.Comparative genomic analysis revealed that the expanded genes in Stevia were mainly enriched for biosynthesis of specialized metabolites,especially biosynthesis of terpenoid backbones,and for further oxidation and glycosylation of these compounds.We further identified all candidate genes involved in SG biosynthesis.Collectively,our current findings on the Stevia reference genome will be very helpful for dissecting the evolutionary history of Stevia and for discovering novel genes contributing to SG biosynthesis and other important agronomic traits in future breeding programs.

Survival after radical cystectomy for bladder cancer:Multicenter comparison between minimally invasive and open approaches

Objective:To investigate oncological outcomes in patients with bladder cancer who underwent minimally invasive radical cystectomy(MIRC)or open radical cystectomy(ORC).Methods:We identified patients with bladder cancer who underwent radical cystectomy(RC)in 13 centers of the Chinese Bladder Cancer Consortium(CBCC).Perioperative outcomes were compared between MIRC and ORC.The influence of surgical approaches on overall survival(OS)and cancer-specific survival(CSS)in the entire study group and subgroups classified according to pathologic stage or lymph node(LN)status was assessed with the log-rank test.Multivariable Cox proportional hazard models were used to evaluate the association among OS,CSS and risk factors of interest.Results:Of 2098 patients who underwent RC,1243 patients underwent MIRC(1087 laparoscopic RC and 156 robotic-assisted RC,respectively),while 855 patients underwent ORC.No significant differences were noted in positive surgical margin rate and 90-day postoperative mortality rate.MIRC was associated with less estimated blood loss,more LN yield,higher rate of neobladder diversion,longer operative time,and longer length of hospital stay.There was no significant difference in OS and CSS according to surgical approaches(pZ0.653,and 0.816,respectively).Subgroup analysis revealed that OS and CSS were not significantly different regardless of the status of extravesical involvement or LN involvement.Multivariable Cox regression analyses showed that the surgical approach was not a significant predictor of OS and CSS.Conclusions:Our study showed that MIRC was comparable to conventional ORC in terms of OS and CSS.

Exploration and Practice of Training for Management Cadres of Standardized Nurse Training

We have made a summary for Chongqing Standardized Nurse Training Class at several aspects, including the basic information of trainees, the configuration of teachers, the setting of courses, and the effect analysis. Meanwhile, some improvement measures are proposed according to the comments and suggestions. This study provides a reliable basis for cultivating the management cadres of standardized nurse training.

ON FINITE ELEMENT APPROXIMATIONS TO A SHAPE GRADIENT FLOW IN SHAPE OPTIMIZATION OF ELLIPTIC PROBLEMS

Shape gradient flows are widely used in numerical shape optimization algorithms.We investigate the accuracy and effectiveness of approximate shape gradients flows for shape optimization of elliptic problems.We present convergence analysis with a priori error estimates for finite element approximations of shape gradient flows associated with a distributed or boundary expression of Eulerian derivative.Numerical examples are presented to verify theory and show that using the volume expression is effective for shape optimization with Dirichlet and Neumann boundary conditions.

代谢工程改造大肠杆菌合成羟基酪醇

羟基酪醇是重要精细化学品,作为天然抗氧化剂被广泛应用于食品、医药领域。利用合成生物学技术生产羟基酪醇具有重要意义。本文克隆并功能鉴定了来源于大肠杆菌EscherichiacoliBL21的羟化酶编码基因HpaBC,结果表明该酶的两个亚基均能成功表达并能催化酪醇生成羟基酪醇。通过CRISPR-Cas9技术将由tac启动子调控的HpaBC基因表达盒整合到前期构建的酪醇高产菌株YMG5A*R基因组中,同时删除副产物乙酸的合成途径,获得大肠杆菌代谢工程菌株YMGRD1H1。摇瓶发酵实验结果表明,重组菌株能够直接利用葡萄糖生产羟基酪醇,产量达到1.81g/L,同时发现几乎没有副产物积累。5L发酵罐规模的流加补料发酵实验表明,羟基酪醇最高产量达到2.95 g/L,是目前文献报道以葡萄糖从头合成羟基酪醇的最高水平。通过系统改造大肠杆菌,实现了羟基酪醇的大量合成,为进一步构建具有工业应用潜力的羟基酪醇细胞工厂奠定了基础,也为拓展芳香族化合物的微生物制造路线提供了有益的参考。

Shape-Controlled Synthesis of Mn_(3)O_(4) Nanocrystals and Their Catalysis of the Degradation of Methylene Blue

Various sizes and shapes of Mn_(3)O_(4) nanocrystals have been prepared in a one-pot synthesis in extremely dilute solution by soft template self-assembly. To better control size and shape, the effects of varying the growth time, reaction temperature, surfactant, and manganese source were examined. The average size of octahedral Mn_(3)O_(4) crystallites was found to be related to the reaction time, while higher reaction temperature (150 °C) and the use of a cetyltrimethylammonium bromide/poly(vinylpyrrolidone) (CTAB/PVP) mixture allowed construction of a better-defined octahedral morphologies. When PVP or poly(ethylene oxide)-poly(propylene oxide) (P123) was used as template, large-scale agglomeration resulting in loss of the octahedral morphology occurred and crystallites with a quasi-spherical shape were obtained. The nano-octahedral crystallites were shown to be an efficient catalyst for the oxidation of methylene blue.

p38α has an important role in antigen cross-presentation by dendritic cells

The role of the p38 signaling pathway in the innate and adaptive immune responses has been well documented,especially in inflammatory cytokine production by dendritic cells(DCs).However,whether the p38 signaling pathway affects the important antigen(Ag)presentation function of DCs remains largely unknown.In this study,we reported that the deletion of p38αresulted in an impaired cross-presentation ability of CD8^(+) conventional DCs(cDCs)and a reduction in the direct presentation ability of CD8−cDCs ex vivo.Further study revealed that p38αhad a crucial role in Ag processing by CD8^(+) cDCs but did not affect the Ag uptake or co-stimulation of T cells.Moreover,p38αdeficiency led to reduced cross-priming of T cells in vivo.The production of the IL-12p40 and IL-12p70 cytokines by p38α-deficient cDCs was also significantly reduced.Our study identified a new role for p38αin modulating the important antigen cross-presentation function of DCs.

A Novel mRNA Signature Related to Immunity to Predict Survival and Immunotherapy Response in Hepatocellular Carcinoma

Background and Aims:Hepatocellular carcinoma(HCC)is the most common primary liver cancer and the incidence and mortality rates are increasing.Given the limited treatments of HCC and promising application of immunotherapy for cancer,we aimed to identify an immune-related prognostic signature that can predict overall survival(OS)rates and immunotherapy response in HCC.Methods:The initial signature development was conducted using a training dataset from the Cancer Genome Atlas followed by independent internal and external validations from that resource and the Gene Expression Omnibus.A signature based nomogram was generated using multivariate Cox regression analysis.The associations of signature score with tumor immune phenotype and response to immunotherapy were analyzed using single-sample gene set enrichment analysis and tumor immune dysfunction and exclusion algorithm.A cohort from Zhongshan Hospital was employed to verify the pre dictive robustness of the signature regarding prognostic risk and immunotherapy response.Results:The prognostic signature,IGS_(HCC),consisting of 22 immune-related genes,had independent prognostic ability,with training and validation cohorts.Also,IGS_(HCC)stratified HCC patients with different outcomes in subgroups.The prognostic accuracy of IGS_(HCC)was better than three reported prognostic signatures.The IGS_(HCC)-based nomogram had high accuracy and significant clinical benefits in predicting 3-and 5-year OS.IGS_(HCC)reflected distinct immunosuppressive phenotypes in low-and high-score groups.Patients with low IGS_(HCC)scores were more likely than those with high scores to benefit from immunotherapy.Conclusions:IGS_(HCC)predicted HCC prognosis and response to immunotherapy,and contributed to individualized clinical management.

A Primal-Dual Hybrid Gradient Algorithm to Solve the LLT Model for Image Denoising

We propose an efficient gradient-type algorithm to solve the fourth-order LLT denoising model for both gray-scale and vector-valued images.Based on the primal-dual formulation of the original nondifferentiable model,the new algorithm updates the primal and dual variables alternately using the gradient descent/ascent flows.Numerical examples are provided to demonstrate the superiority of our algorithm.

Near-infrared carbon-implanted Er^3＋/yb^3＋ co-doped phosphate glass waveguides

The Er3＋/yb3＋ co-doped phosphate （EYDP） glass waveguides operated at 1539 nm have been manufactured by using the implantation technique of carbon ions under the condition of 6.0 MeV energy and 5.0 × 10^13 ions/cm2 fluence in this work. The ion implantation process was computed by means of the stopping and range of ions in matter. The dark-mode spectrum at 1539 nm of the waveguide was recorded by the method of the prism coupling measurement. The microscopic image of the fabricated structure was photographed by an optical microscope. It is the first step for the application of the waveguides on the base of EYDP glasses in optical- integrated photonic devices at near-infrared band.

Functional diversifications of Gh ERF1 duplicate genes after the formation of allotetraploid cotton

Whole genome duplication, a prevalent force of evolution in plants, results in massive genome restructuring in different organisms. Roles of the resultant duplicated genes are poorly understood both functionally and evolutionarily. In the present study, differentially expressed ethylene responsive factors(GhERF1 s), anchored on Chr-A07 and Chr-D07 were isolated from a high-yielding cotton hybrid(XZM2)and its parents. The GhERF1 was located in the B3 subgroup of the ethylene responsive factors subfamily involved in conferring tolerance to abiotic stress Nucleotide sequence analysis of 524 diverse accessions together with quantitative real-time polymerase chain reaction analysis, elucidated that de-functionalization of GhERF1-7 A occurred due to one base insertion following formation of the allotetraploid cotton. Our quantitative trait loci and association mapping analyses highlighted a role for GhERF1-7 A in conferring high boll number per plant in modern cotton cultivars. Overexpression of GhERF1-7 A in transgenic Arabidopsis resulted in a substantial increase in the number of siliques and total seed yield. Neo-functionalization of GhERF1-7 A was also observed in modern cultivars rather than in races and/or landraces, further supporting its role in the development of high-yielding cotton cultivars. Both de-and neofunctionalization occurred in one of the duplicate genes,thus providing new genomic insight into the evolution of allotetraploid cotton species.

Synthesis and optical properties of LiNd(PO_3)_4 nanocrystals dispersion in DMSO/TBE

Lanthanide doped nanocrystals with strong fluorescence, long lifetime at high doping concentrations have great potential application in bio-imaging and liquid gain medium. LiNd(PO_3)_4(LNP) crystal was reported to be one of the most excellent laser crystals with high Nd3+ concentration, and their nanocrystals synthesized via improved combustion method for the first time had strong emission intensity and long fluorescence lifetime of 122 μs. Besides,LiNd(PO_3)_4 nanocrystals can be dispersed in mixed solvents of DMSO/TBE(CHBr2 CHBr2) to form a transparent colloidal dispersion, and Judd-Ofelt theory was used to evaluate their optical parameters. In summary, LiNd(PO_3)_4 nanocrystals possess long lifetime(116 μs), low solvents quenching rate(4.9%), large emission cross section(7.63 × 10^(-20) cm^2) and high quantum yield(35.2%) under high Nd3+ ions concentration(1×10^(20) cm^(-3)), which would be the most competitive colloidal gain medium of optical amplification and laser with LD pump and potential biomaterial with low particles concentration.

Near-infrared carbon-implanted waveguides in Tb^3+doped aluminum borosilicate glasses

Ion implantation has played a unique role in the fabrication of optical waveguide devices.Tb'-doped aluminum borosilicate(TDAB)glass has been considered as an important magneto-optical material.In this work,near-infrared waveguides have been manufactured by the(5.5+6.0)MeV C^3+ion implantation with doses of(4.0+8.0)×10^13 ions·cm^-2 in the TDAB glass.The modes propagated in the TDAB glass waveguide were recorded by a prism-coupling system.The finite-difference beam propagation method(FD-BPM)was carried out to simulate the guiding characteristics of the TDAB glass waveguide.The TDAB glass waveguide allows the light propagation with a single-mode at 1.539μm and can serve as a potential candidate for future waveguide isolators.