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Ligand-controlled NiH-catalyzed regiodivergent hydroalkylation of 2-alkenylazaarenes

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Science China Chemistry 2024年第6期67卷 1935-1940页

作者： Ya-ping shao Zhuo-Min Chi Yong-Min Liang State Key Laboratory of Applied Organic Chemistry School of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000China

A nickel-hydride(Ni H)-catalyzed migratory and nonmigratory hydroalkylation reaction of 2-alkenyl azaarenes with alkyl iodines has been established through strategic modulation of N-or P-donor ligands.This method enables the synthesis of diverseβ-orγ-branched aromatic N-heterocycles.The mild regiodivergent protocols exhibit wide substrate scope,excellent functional tolerance,and great reaction yield with remarkable regioselectivity.Importantly,deuterium labeling studies reveal Ni H-catalyzed interrupted chain-walking mode as the mechanism behind remotedβ-selective hydroalkylation reaction—an interesting phenomenon mediated through aromatic imine directing groups.

关键词： NiH regiodivergent hydroalkylation azaarenes interrupted chain-walking

Prenatal diagnosis of congenital chloride diarrhea by whole exome sequencing in four Chinese families and prenatal genotype–phenotype association study

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World Journal of Pediatrics 2023年第2期19卷 200-207页

作者： Ying-Fei shao Hong Wang Yi-Xiu Wang le-ping shao Sai Wang Renji College of Wenzhou Medical University WenzhouChina Department of Nephrology The Affiliated Qingdao Municipal Hospital of Qingdao UniversityNo.5 Donghai Middle RoadQingdao266071China Laboratory of Renal Disease QingdaoChina Department of Nephrology Eighth People’s Hospital of QingdaoQingdaoChina Darpartment of Hepatic Surgery Shanghai Cancer CenterShanghai Medical CollegeFudan UniversityShanghaiChina Department of Dermatology Peking University First HospitalBeijingChina

Congenital chloride diarrhea(CCD;OMIM 214700)is an intestinal disease of an electrolyte defect characterized by dilated bowel loops,maternal polyhydramnios,premature birth,and lack of infant meconium[l].The incidence of CCD is variable worldwide.Most cases are sporadic;however,there are three high-incidence areas,Finland,Poland,and Saudi Arabia.In addition,large genetic heterogeneity has been reported in about 300 sporadic patients with CCD from other ethnic groups[2-4].Undiagnosed or untreated CCD can be lethal within the first year of life,but with adequate treatment,patients are usually able to survive into adulthood[5,6].

关键词： diagnosis diarrhea congenital

Estimating the optimal vegetation coverage for the dominant tree and shrub species over China's northwest drylands

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Science China Earth Sciences 2024年第5期67卷 1500-1517页

作者： Zhongdian ZHANG Xiaoxu JIA ping ZHU Mingbin HUANG Lidong REN Ming’an shao School of Geographic Sciences Xinyang Normal UniversityXinyang 464000China Key Laboratory of Ecosystem Network Observation and Modeling Institute of Geographic Sciences and Natural Resources ResearchChinese Academy of SciencesBeijing 100101China College of Resources and Environment University of Chinese Academy of SciencesBeijing 100190China Yellow River Delta Modern Agricultural Engineering Laboratory Chinese Academy of SciencesBeijing 100101China State Key Laboratory of Soil Erosion and Dryland Farming on the Loess Plateau Institute of Soil and Water ConservationNorthwest A&F UniversityYangling 712100China

Anthropogenic revegetation is an effective way to control soil erosion and restore degraded ecosystems in China's northwest drylands(NWD).However,excessive vegetation cover expansion has long been known to increase evapotranspiration,leading to reduced local water availability,which can in turn threaten the health and services of restored ecosystems.Determining the optimal vegetation coverage(OVC)is critical for balancing the trade-off between plant growth and water consumption in water-stressed areas,yet quantitative assessments over the entire NWD are still lacking.In this study,a modified Biome BioGeochemical Cycles(Biome-BGC)model was used to simulate the long-term(1961–2020)dynamics of actual evapotranspiration(ET_(a)),net primary productivity(NPP),and leaf area index(LAI)for the dominant non-native tree(R.pseudoacacia and P.sylvestris)and shrub(C.korshinkii and H.rhamnoides)species at 246 meteorological sites over NWD.The modified model incorporated the Richards equation to simulate transient unsaturated water flow in a multilayer soil module,and both soil and eco-physiological parameters required by the model were validated using field-observed ETadata for each species.Spatial distributions of OVC(given by the mean maximum LAI,LAI_(max))for the dominant species were determined within three hydrogeomorphic sub-areas(i.e.,the loess hilly-gully sub-area,the windy and sandy sub-area,and the desert sub-area).The modified Biome-BGC model performed well in terms of simulating ET_(a) dynamics for the four plant species.Spatial distributions of mean ET_a,NPP,and LAI_(max)generally exhibited patterns similar to mean annual precipitation(MAP).In the loess hilly-gully sub-area(MAP:210 to 710 mm),the OVC respectively ranged from 1.7 to 2.9 and 0.8 to 2.9 for R.pseudoacacia and H.rhamnoides.In the windy and sandy sub-area(MAP:135 to 500 mm),the OVC ranged from 0.3 to 3.3,0.5 to 2.6 and 0.6 to 2.1for P.sylvestris,C.korshinkii and H.rhamnoides,respectively.In the desert sub-area(MAP:90 to 500 mm),the OVC ranged from 0.4 t

关键词： Optimal vegetation coverage Water balance leaf area index Biome-BGC model Dryland

Circulating proteomic biomarkers for diagnosing sporadic amyotrophic lateral sclerosis:a cross-sectional study

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Neural Regeneration Research 2024年第8期19卷 1842-1848页

作者： Lu He Qinming Zhou Chaoyang Xiu Yaping shao Dingding Shen Huanyu Meng Weidong le Sheng Chen Department of Neurology and Institute of Neurology Ruijin HospitalShanghai Jiao Tong University School of MedicineShanghaiChina Department of Neurology Hospital of Chengdu University of Traditional Chinese MedicineChengduSichuan ProvinceChina Center for Translational Research on Neurological Diseases the First Affiliated HospitalDalian Medical UniversityDalianLiaoning ProvinceChina Co-innovation Center of Neuroregeneration Nantong UniversityNantongJiangsu ProvinceChina Institute of Neurology Sichuan Academy of Medical Sciences-Sichuan Provincial HospitalChengduSichuan ProvinceChina Department of Neurology Xinrui HospitalWuxiJiangsu ProvinceChina

Biomarke rs are required for the early detection,prognosis prediction,and monitoring of amyotrophic lateral sclerosis,a progressive disease.Proteomics is an unbiased and quantitative method that can be used to detect neurochemical signatures to aid in the identification of candidate biomarke rs.In this study,we used a label-free quantitative proteomics approach to screen for substantially differentially regulated proteins in ten patients with sporadic amyotrophic lateral scle rosis compared with five healthy controls.Su bstantial upregulation of serum proteins related to multiple functional clusters was observed in patients with spo radic amyotrophic lateral sclerosis.Potential biomarke rs were selected based on functionality and expression specificity.To validate the proteomics profiles,blood samples from an additional cohort comprising 100 patients with sporadic amyotrophic lateral sclerosis and 100 healthy controls were subjected to enzyme-linked immunosorbent assay.Eight substantially upregulated serum proteins in patients with spora dic amyotrophic lateral sclerosis were selected,of which the cathelicidin-related antimicrobial peptide demonstrated the best discriminative ability between patients with sporadic amyotrophic lateral sclerosis and healthy controls(area under the curve[AUC]=0.713,Pled tumor protein).The algo rithm achieved an AUC of 0.811 and a P-value ofle rosis.Subsequently,the ability of candidate biomarkers to discriminate between early-stage amyotrophic lateral sclerosis patients and controls,as well as patients with different disease severities,was examined.A two-protein panel comprising talin-1 and translationally-controlled tumor protein effectively d

关键词： amyotrophic lateral sclerosis cathelicidin-related antimicrobial peptide hemoglobin label-free quantitative proteomics multi-protein combined diagnostic panel serum biomarkers talin-1 translationally-controlled tumor protein zyxin

A deoxidation thermodynamic model for 304 stainless steel considering multiple-components coupled reactions

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Journal of Iron and Steel Research(International) 2024年第1期31卷 74-91页

作者： Yan Yan Guang-hao Shang Li-ping Zhang shao-ying Li Han-jie Guo School of Metallurgical and Ecological Engineering University of Science and Technology BeijingBeijing100083China Beijing Key Laboratory of Special Melting and Preparation of High-End Metal Materials Beijing100083China Henan Jinhui Stainless Steel Industry Group Co. Ltd.Xuchang461500HenanChina Changge Jinhui Recycling Metal R&D Co. Ltd.Xuchang461500HenanChina

A thermodynamic model for predicting the equilibrium oxygens of 304 stainless steel was developed based on the theory of slag-steel equilibrium,the law of mass conservation,and the ion and molecule coexistence theory.In the developed model,the Fe-Cr-Mn-Si-Al-S-O-melts reaction system and CaO-MgO-CaF_(2)-FeO-MnO-Al_(2)O_(3)-SiO_(2)-Cr2O_(3)slags were considered.The oxygen contents calculated by the model are in good agreement with experimental results and reference data.The equilibrium oxygen contents in 304 stainless steel mainly decrease with increasing binary basicity(w(CaO)/w(SiO_(2)),where w(i)is the mass percentage of component i)and decreasing temperature.Controlling binary basicity at 2.0 while maintaining temperatures lower than 1823 K will keep the oxygen contents in the 304 stainless steel lower than 15×10^(-6).The equilibrium oxygen contents may also be decreased with increasing content of MgO in slags,which is more significant at lower binary basicity.Besides,a small amount of FeO,MnO,and Al_(2)O_(3)(about 0-2.5 wt.%)in slags has little effect on equilibrium oxygen contents.Furthermore,it is found that the[C]-[O]reaction may occur during refining process but will not significantly affect the equilibrium oxygen contents.

关键词： Complex deoxidation Thermodynamic model Ion and molecule coexistence theory 304 stainless steel Slag-steel reaction

Graphdiyne oxide substrate-enhanced peroxidase-mimicking performance of Ru nanoparticles with physiological pH preference

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Nano Research 2024年第3期17卷 1123-1131页

作者： Cong Xu Wenjie Ma Haozhi Wang leihou shao Weiqi Li ping Yu Lanqun Mao Beijing National Laboratory for Molecular Science Key Laboratory of Analytical Chemistry for Living BiosystemsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China State Key Laboratory of Marine Resource Utilization in South China Sea School of Materials Science and EngineeringHainan UniversityHaikou 570228China College of Chemistry Beijing Normal UniversityBeijing 100875China

Modulating electronic structure of metal nanoparticles via metal–support interaction has attracted intense interest in the field of catalytic science.However,the roles of supporting substrates in regulating catalytic properties of nanozymes remain elusive.In this study,we find that the use of graphdiyne oxide(GDYO)as the substrate for self-terminating growth of Ru nanoparticles(Ru@GDYO)endows the peroxidase-like activity of Ru nanoparticles with intrinsic physiological pH preference and natural horseradish peroxidase(HRP)comparable performance.Ru nanoparticles electrolessly deposited onto GDYO possess a partially oxidized electronic structure owing to limited charge transfer between Ru and GDYO,contributing to the intrinsic physiological pH preference of the peroxidase-mimicking nanozyme.More importantly,the substrate GDYO plays an influential factor in enhancing catalytic activity,that is,the activity of Ru@GDYO is much higher than that of Ru nanoparticles deposited on other carbon substrates including graphene oxides and graphdiyne.To demonstrate the application of Ru@GDYO nanozyme in neutral solutions,we employ Ru@GDYO with nicotinamide adenine dinucleotide(NAD+)-dependent dehydrogenases in physiological conditions to realize a sustainable cascade reaction by means of forming continuous NAD^(+)/dihydronicotiamide adenine dinucleotide(NADH)recycling.Our finding represents a promising perspective on designing high-performance peroxidase-mimicking nanozymes with broader applicability,raising fundamental understanding of structure–activity relationship,and investigating new applications of nanozymes in biological systems.

关键词： nanozyme graphdiyne reactive oxygen species electroless deposition metal–support interaction

Progress in research on metal-based materials in stabilized Zn anodes

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Rare Metals 2024年第1期43卷 20-40页

作者： le Li shao-Feng Jia Ming-Hui Cao Yong-Qiang Ji Heng-Wei Qiu Dan Zhang Shaanxi Key Laboratory of Industrial Automation School of Mechanical EngineeringShaanxi University of TechnologyHanzhong 723001China School of Electronic and Information Engineering Qingdao UniversityQingdao 266071China State Key Laboratory for Artifcial Microstructure and Mesoscopic Physics School of PhysicsPeking UniversityBeijing 100871China Department of Chemistry Key Laboratory of Bioorganic Phosphorus Chemistry and Chemical BiologyTsinghua UniversityBeijing 100084China Shaanxi Key Laboratory of Catalysis School of Chemistry and Environment ScienceShaanxi University of TechnologyHanzhong 723001China

Aqueous zinc-ion batteries(ZIBs) combine the benefits of metallic Zn anodes with those of aqueous electrolytes and are well suited for large-scale energy storage because of their inherent high safety, cost-effectiveness, and eco-friendliness. Currently, the practical application of such batteries is hindered by the poor cycling performance of Zn anodes due to uncontrolled dendrite formation and severe side reactions, although recent reports suggest that these problems can be mitigated through the modification of Zn anodes with metal-based materials.Given that the mechanisms of improving Zn deposition and the structural evolution of metal-based materials have not been systematically reviewed, we herein systematically overview the metal-based materials used to stabilize Zn anodes, starting with a brief summary of the anode working mechanism and the challenges faced by stabilized Zn anodes. Subsequently, the design principles of Zn anodes stabilized by metal-based materials and the related recent progress are reviewed, and the key challenges and perspectives for the future development of such Zn anodes are proposed.

关键词： Zinc-ion batteries(ZIBs) Zn anode Metalbased materials Alloying metal Stabilized Zn anodes

Impact of frailty on short-term postoperative outcomes in patients undergoing colorectal cancer surgery:A systematic review and meta-analysis

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World Journal of Gastrointestinal Surgery 2024年第3期16卷 893-906页

作者： Yao Zhou Xiao-lei Zhang Hong-Xia Ni Tian-Jing shao ping Wang Department of Operating Room Affiliated Tumor Hospital of Nantong University&Nantong Tumor HospitalNantong 226361Jiangsu ProvinceChina Department of Gastrointestinal Surgery The Affiliated Tumor Hospital of Nantong University&Nantong Tumor HospitalNantong 226361Jiangsu ProvinceChina

BACKGROUND Colorectal cancer is a major global health challenge that predominantly affects older people.Surgical management,despite advancements,requires careful consideration of preoperative patient status for optimal outcomes.AIM To summarize existing evidence on the association of frailty with short-term postoperative outcomes in patients undergoing colorectal cancer surgery.METHODS A literature search was conducted using PubMed,EMBASE and Scopus databases for observational studies in adult patients aged≥18 years undergoing planned or elective colorectal surgery for primary carcinoma and/or secondary metastasis.Only studies that conducted frailty assessment using recognized frailty assess-ment tools and had a comparator group,comprising nonfrail patients,were included.Pooled effect sizes were reported as weighted mean difference or relative risk(RR)with 95%confidence intervals(CIs).RESULTS A total of 24 studies were included.Compared with nonfrail patients,frailty was associated with an increased risk of mortality at 30 d(RR:1.99,95%CI:1.47-2.69),at 90 d(RR:4.76,95%CI:1.56-14.6)and at 1 year(RR:5.73,95%CI:2.74-12.0)of follow up.Frail patients had an increased risk of any complications(RR:1.81,95%CI:1.57-2.10)as well as major complications(Clavien-Dindo classification grade≥III)(RR:2.87,95%CI:1.65-4.99)compared with the control group.The risk of reoperation(RR:1.18,95%CI:1.07-1.31),readmission(RR:1.70,95%CI:1.36-2.12),need for blood transfusion(RR:1.67,95%CI:1.52-1.85),wound complications(RR:1.49,95%CI:1.11-1.99),delirium(RR:4.60,95%CI:2.31-9.16),risk of prolonged hospitalization(RR:2.09,95%CI:1.22-3.60)and discharge to a skilled nursing facility or rehabilitation center(RR:3.19,95%CI:2.0-5.08)was all higher in frail patients.CONCLUSION Frailty in colorectal cancer surgery patients was associated with more complications,longer hospital stays,higher reoperation risk,and increased mortality.Integrating frailty assessment appears crucial for tailored surgical management.

关键词： Frailty Frail adults Colorectal surgery Colorectal cancer Complications Mortality Survival Slinical outcomes Meta-analysis

Hydrometallurgical recovery of lithium carbonate and iron phosphate from blended cathode materials of spent lithium-ion battery

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Rare Metals 2024年第3期43卷 1275-1287页

作者： shao-le Song Run-Qing Liu Miao-Miao Sun Ai-Gang Zhen Fan-Zhen Kong Yue Yang School of Minerals Processing and Bioengineering Central South UniversityChangsha410083China Zhejiang Tianneng New Materials Co. Ltd.Huzhou313103China

The recycling of cathode materials from spent lithium-ion battery has attracted extensive attention,but few research have focused on spent blended cathode materials.In reality,the blended materials of lithium iron phosphate and ternary are widely used in electric vehicles,so it is critical to design an effective recycling technique.In this study,an efficient method for recovering Li and Fe from the blended cathode materials of spent LiFePO_(4)and LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)batteries is proposed.First,87%A1 was removed by alkali leaching.Then,91.65%Li,72.08%Ni,64.6%Co and 71.66%Mn were further separated by selective leaching with H_(2)SO_(4)and H_(2)O_(2).Li,Ni,Co and Mn in solution were recovered in the form of Li_(2)CO_(3)and hydroxide respectively.Subsequently,98.38%Fe was leached from the residue by two stage process,and it is recovered as FePO_(4)·2H_(2)O with a purity of 99.5%by precipitation.Fe and P were present in FePO_(4)·2H_(2)O in amounts of 28.34%and 15.98%,respectively.Additionally,the drift and control of various components were discussed,and cost-benefit analysis was used to assess the feasibility of potential application.

关键词： Spent lithium-ion battery Blended cathode materials Recovery Lithium carbonate Iron phosphate