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Cr-catalyzed allylic C(sp^(3))–H addition to aldehydes enabled by photoinduced ligand-to-metal charge transfer

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Science China Chemistry 2024年第5期67卷 1589-1595页

作者： Xianrong Zeng Feng-hua Zhang Runchen lai Xiaoyu Lin Zhaobin Wang Key Laboratory of Precise Synthesis of Functional Molecules of Zhejiang Province Department of ChemistrySchool of Science and Research Center for Industries of the FutureWestlake UniversityHangzhou 310030China Institute of Natural Sciences Westlake Institute for Advanced StudyHangzhou 310024China Key Laboratory of Precise Synthesis of Functional Molecules of Zhejiang Province Instrumentation and Service Center for Molecular SciencesWestlake UniversityHangzhou 310024China

Photoinduced ligand-to-metal charge transfer(LMCT) has emerged as an effective strategy for synthesizing organic molecules in a sustainable manner. However, the majority of existing reports on selective C(sp^(3))–H bond functionalization via photoinduced LMCT focus on the use of late transition metals or rare-earth metals for radical additions or cross-couplings. In contrast, the utilization of photoinduced LMCT with 3d early transition metals poses a significant challenge. Herein, we describe an unprecedented approach to allylic C(sp^(3))–H addition to aldehydes, employing chromium(Cr) complexes as catalysts through visible-light-induced LMCT. By investigating the reaction pathway through various mechanistic studies, including radical trapping, kinetic isotope effect(KIE) analysis, and transient absorption spectroscopy, valuable insights have been gained. The proposed mechanism suggests the intermediacy of bromine radicals through homolysis of the Cr–Br bond. Notably, this protocol expands our understanding of the photochemical properties of earth-abundant Cr complexes.

关键词： Cr catalysis photoinduced ligand-to-metal charge transfer hydrogen-atom transfer carbonyl addition

Synthesis of poly(thiourethane-alt-thioester)by alternating ring-opening copolymerization of N-thiocarboxyanhydrides and episulfides

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Science China Chemistry 2024年第9期67卷 3091-3097页

作者： Wei Xiong Tianjun Yue Haiwang lai Chunyan Lyu Weimin Ren hua Lu Beijing National Laboratory for Molecular Sciences Center for Soft Matter Science and EngineeringKey Laboratory of Polymer Chemistry and Physics of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China State Key Laboratory of Fine Chemicals Dalian University of TechnologyDalian 116081China

Polythiourethanes(PTU)and polythioesters(PTE)derived from renewable sources are emerging sustainable polymers for their excellent degradability and ***,P(TU-alt-TE)copolymers have been rare and challenging to ***,we report the efficient synthesis of novel P(TU-alt-TE)copolymers via the alternating copolymerization of N-thiocarboxyanhydrides(NTA)/episufides(ES)and provide mechanistic insight into the alternating chain propagation process via density functional theory(DFT)*** incorporation of ESs into traditional peptide backbone is capable of adjusting the glass transition temperature below thermal decomposition temperature,which confers better thermal processability by regulating the rigidity of the backbone and the hydrogen bond interaction among the polymer *** PTUs with tailored properties are accessible by altering the feeding ratio of NTAs and(bifunctional)***,the thiourethane in the backbone can endow interesting underwater adhesion properties to the *** the broad scope of NTA and ES monomers,this method is expected to provide a promising and general route to a wide range of P(TU-alt-TE)copolymers with diverse properties.

关键词： poly(thiourethane-alt-thioester) alternating ring-opening copolymerization N-thiocarboxyanhydrides episulfides

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Comparison of different preoperative objective nutritional indices for evaluating 30-d mortality and complications after liver transplantation

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World Journal of Gastrointestinal Surgery 2024年第1期16卷 143-154页

作者： Chuan Li Hong-Xia Chen Yan-hua lai department of Transplantation People’s Hospital of Guangxi Zhuang Autonomous RegionNanning 530021Guangxi Zhuang Autonomous RegionChina department of Clinical Pharmacy People’s Hospital of Guangxi Zhuang Autonomous RegionNanning 530021Guangxi Zhuang Autonomous RegionChina

BACKGROUND The nutritional status is closely related to the prognosis of liver transplant re-cipients,but few studies have reported the role of preoperative objective nutri-tional indices in predicting liver transplant *** To compare the predictive value of various preoperative objective nutritional indicators for determining 30-d mortality and complications following liver transplantation(LT).METHODS A retrospective analysis was conducted on 162 recipients who underwent LT at our institution from december 2019 to June *** This study identified several independent risk factors associated with 30-d mor-tality,including blood loss,the prognostic nutritional index(PNI),the nutritional risk index(NRI),and the control nutritional *** 30-d mortality rate was 8.6%.Blood loss,the NRI,and the PNI were found to be independent risk factors for the occurrence of severe postoperative *** NRI achieved the highest prediction values for 30-d mortality[area under the curve(AUC)=0.861,Pdex and prealbumin and albumin levels,as well as higher alanine aminotransferase and total bilirubin levels,Model for End-stage Liver Disease scores and prothrombin time(Pdences of intraabdominal bleeding,primary graft nonfunction,and *** The NRI has good predictive value for 30-d mortality and severe complications following *** NRI could be an effective tool for transplant surgeons to evaluate perioperative nutritional risk and develop relevant nutritional therapy.

关键词： Liver transplantation Nutritional indicator Complications Prognosis Nutrition assessment

Coexistence of All-Order Topological States in a Three-Dimensional Phononic Topological Crystalline Insulator

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Research 2024年第2期2023卷 511-518页

作者： hua-Shan lai Hao Chen Chu-Hao Xia Si-Yuan Yu Cheng He Yan-Feng Chen National Laboratory of Solid State Microstructures&department of Materials Science and Engineering Nanjing UniversityNanjng 210093China Collaborative Innovation Center of Advanced Microstructures Nanjing University Nanjng 210093China Jiangsu Key Laboratory of Artificial Functional Materials Nanjing University Nanjing 210093China

Classical-wave topological materials lacking intrinsic half-integer spins are less robust while more ***,we explore a single 3-dimensional phononic topological crystalline insulator that simultaneously exhibits a whole family of first-order quadratic surface,second-order hinge,and third-order corner states within the same *** a topological crystalline insulator hosting all-order phases originates from the different topological nature when hierarchically projected onto different facets and lower dimensions,thus free from trivial cladding *** work offers an ideal platform for either robust wave propagation or localization in on-demand dimensions and may facilitate dimension division multiplexing technology.

关键词： topological dimensions crystalline

Predictive value of intracranial high-density areas in neurological function

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World Journal of Psychiatry 2024年第7期14卷 1080-1086页

作者： Zhi-Juan Lu Jin-Xing lai Jing-Ru huang Shu-hua Xie Zhao-Hui lai department of Neurology Ganzhou People’s HospitalGanzhou 341000Jiangxi ProvinceChina

BACKGROUND Intracranial high-density areas(HDAs)have attracted considerable attention for predicting clinical outcomes;however,whether HDAs predict worse neurological function and mental health remains controversial and unclear,which requires further *** this prospective study,96 patients with acute ischemic stroke(AIS)who accepted endovascular mechanical thrombectomy(EMT)were *** enrolled patients underwent cranial computed tomography(CT)examination within 24 hours after *** data in terms of National Institutes of Health Stroke Scale(NIHSS),the 3-month modified Rankin Scale(mRS),self-rating depression scale(SDS),and self-rating anxiety scale(SAS)scores were collected and compared between patients with HDAs and non-HDAs and between patients with good and poor clinical *** to patients without HDAs,patients with HDAs presented severe neurological deficits(admission NIHSS score:18±3 vs 19±4),were more likely to have post-stroke disabilities(mRSdepression(SDS score:58±16 vs 64±13)and anxiety disorder(SAS score:52±8 vs 59±10).Compared to patients with a good prognosis,patients with a poor prognosis presented severe neurological deficits(admission NIHSS score:17±4 vs 20±3),were more likely to have HDAs on CT images(64%vs 33%),and suffered more severe depression(SDS score:55±19 vs 65±11)and anxiety(SAS score:50±8 vs 58±12).Multivariate analysis revealed that HDAs were independent nega-tive prognostic *** In conclusion,HDAs on CT images predicted poor prognosis and severe depressive and anxiety symptoms in patients with AIS who underwent EMT.

关键词： Acute ischemic stroke Endovascular mechanical thrombectomy High-density areas depressive disorder Anxiety disorder

Prognostic Nutritional Index Associates with the Severity of Silicosis:A Study from a Tertiary Class A Prevention and Treatment Institute for Occupational Diseases in China

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Biomedical and Environmental Sciences 2024年第1期37卷 122-126页

作者： HE La Gu LIANG Yun lai YANG Lu Qi YUAN hua Min Medical laboratory department Hunan Prevention and Treatment Institute for Occupational DiseasesChangsha 410000HunanChina Laboratory Medicine department Xiangya HospitalCentral South UniversityChangsha 410013HunanChina

Pneumoconiosis is a group of heterogeneous fibrotic lung diseases caused by inorganic mineral dust and includes coal workers’pneumoconiosis and *** involves diffuse or nodular interstitial pulmonary fibrosis caused by exposure to asbestos or silica *** is thought to have the highest number of silicosis cases,with 6,000 new cases reported annually^([1]).Currently,the clinical diagnosis and monitoring of silicosis relies mainly on a history of occupational exposure and radiological abnormalities^([2]).Therefore,determining further indicators is crucial to reflect the severity of silicosis.

关键词： diagnosis lung diseases

Boosting rate performance of layered lithium-rich cathode materials by oxygen vacancy induced surface multicomponent integration

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Journal of Energy Chemistry 2024年第5期92卷 250-262页

作者： Youyou Fang Yuefeng Su Jinyang Dong Jiayu Zhao Haoyu Wang Yun Lu Bin Zhang hua Yan Feng Wu lai Chen Beijing Key Laboratory of Environmental Science and Engineering School of Material Science and EngineeringBeijing Institute of TechnologyBeijing 100081China Chongqing Innovation Center Beijing Institute of TechnologyChongqing 401120China Yibin Libode New Materials Co. Ltd.Yibin 64400SichuanChina School of Metallurgy and Environment Central South UniversityChangsha 410083HunanChina Engineering Research Center of the Ministry of Education for Advanced Battery Materials Central South UniversityChangsha 410083HunanChina

The rapid development of electric vehicles and portable energy storage systems demands improvements in the energy density and cost-effectiveness of lithium-ion batteries,a domain in which Lithium-rich layered cathode(LLO)materials inherently ***,these materials face practical challenges,such as low initial Coulombic efficiency,inferior cycle/rate performance,and voltage decline during cycling,which limit practical *** study introduces a surface multi-component integration strategy that incorporates oxygen vacancies into the pristine LLO material Li1.2Mn_(0.6)Ni_(0.2)O_(2).This process involves a brief citric acid treatment followed by calcination,aiming to explore rate-dependent degradation *** induced surface oxygen vacancies can reduce surface oxygen partial pressure and diminish the generation of O_(2)and other highly reactive oxygen species on the surface,thereby facilitating the activation of Li ions trapped in tetrahedral sites while overcoming transport ***,the formation of a spinel-like phase with 3D Li+diffusion channels significantly improves Li^(+)diffusion kinetics and stabilizes the surface *** optimally modified sample boasts a discharge capacity of 299.5 mA h g^(-1)at a 0.1 C and 251.6 mA h g^(-1)at a 1 C during the initial activation cycle,with an impressive capacity of 222.1 mA h g^(-1)at a 5 *** notably,it retained nearly 70%of its capacity after 300 cycles at this elevated *** straightforward,effective,and highly viable modification strategy provides a crucial resolution for overcoming challenges associated with LLO materials,making them more suitable for practical application.

关键词： Lithium-ion battery Layered lithium rich cathode Surface multicomponent integration Rate-dependent degradation and Li^(+) diffusion kinetics

Enhanced thermoelectric performance enabled by compositing ZrO_(2)in n-type SiGe alloy with low thermal conductivity

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Rare Metals 2024年第3期43卷 1167-1176页

作者： Meng-Fei Wang hua-Jun lai Ji-Sheng Liang Jun-Liang Chen Wang-Yang Ding Qi Zhou Ying Peng Cheng-Yan Liu Lei Miao Guangxi Key Laboratory for Relativity Astrophysics State Key Laboratory of Featured Metal Materials and Life-Cycle Safety for Composite StructuresSchool of Physical Science and TechnologyGuangxi UniversityNanning530004China Guangxi Academy of Sciences Nanning530007China Key Laboratory of Information Material Engineering Research Center of Electronic Information Materials and DevicesGuilin University of Electronic TechnologyMinistry of EducationGuilin541004China Guangxi Key Laboratory of Precision Navigation Technology and Application School of Information and CommunicationGuilin University of Electronic TechnologyGuilin541004China

SiGe-based thermoelectric(TE)materials have gained increasing interests due to their low maintenance costs,environmental friendliness and long ***,the intrinsically high thermal conductivity of Si-based materials also results in poor TE *** this investigation,a zirconia(ZrO_(2))composite strategy was applied to an n-type SiGe alloy,tremendously elevating its TE *** mechanical alloying and spark plasma sintering(SPS)processes,the ZrO_(2)induced the formation of nanopores in the SiGe matrix via phosphorus ***,such increase in porosity enhanced the phonon scattering and dramatically suppressed lattice thermal conductivity,from 2.83 to 1.59 W·m^(-1)·K^(-1)at 873 ***,reduced phosphorus doping led to an increase in Seebeck coefficients and a relatively minor decrease in electrical conductivity,The power factor didn't deteriorate significantly,either,as its maximum of~3.43 mW·m^(-1-)K^(-2)was achieved at 873 K with(Si_(0.8)Ge_(0.2))_(0.097)P_(0.03)(ZrO_(2))_(0.003).In short,a peak figure of merit(ZT)of~1.27 at 873 K and an average ZT~0.7 from 323 to 873 K were *** study demonstrates that the electrical and thermal transportation of SiGe material can be synergistically tuned by compositing ZrO_(2),illustrating a novel strategy to optimize the TE properties of bulk materials.

关键词： Thermoelectric SiGe alloy ZrO2 composting P element adsorption nanopores

Progress and prospects of graphene-based materials in lithium batteries

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Rare Metals 2024年第5期43卷 1886-1905页

作者： Shen lai Tao huang Pei Liu Hong-Bin Wang Shi-Chun Yang Xin-hua Liu Kai Yang Qian-Ling Zhang Jian-Hong Liu Jiang-Tao Hu Graphene Composite Research Center College of Chemistry and Environmental EngineeringShenzhen UniversityShenzhen 518060China College of Physics and Optoelectronic Engineering Shenzhen UniversityShenzhen 518060China Shenzhen Eigen-Equation Graphene Technology Co.Ltd Shenzhen518060China School of Transportation Science and Engineering Beihang UniversityBeijing 100191China department of Electrical and Electronic Engineering Advanced Technology InstituteUniversity of SurreyGuildfordSurrey GU27XHUK

Reasonable design and applications of graphene-based materials are supposed to be promising ways to tackle many fundamental problems emerging in lithium batteries,including suppression of electrode/electrolyte side reactions,stabilization of electrode architecture,and improvement of conductive ***,extensive fundamental research on this aspect has been performed so ***,when it comes to large-scale industrial applications,the utilization of graphene-based materials progresses at a very slow ***,there presents a severe technological decoupling between academic research and industrial application,and there is an urgent need to link ***,in order to address current issues of graphene-based materials used in lithium batteries,we present their latest advancements with stateof-the-art *** applications of graphenebased materials in practical lithium batteries are highlighted and predicted to bridge the gap between the academic progress and industrial manufacture,thereby paving the way for accelerating the development of graphenebased material as well as lithium battery industry.

关键词： Lithium batteries Graphene-based materials Academic research Industrial application development direction