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Metal-Organic Frameworks Housing Active Molecules as Bioinspired Catalysts

CCS Chemistry 2024年第6期6卷 1380-1402页

作者： Yin Zhang Peter e.VanNatta Junyu Ren Shengqian Ma Department of Chemistry University of North TexasDentonTexas 76201 Department of Chemical and Biomolecular engineering National University of SingaporeSingapore 117585

Optimization of activity,selectivity,and stability of catalysts for practical application is a long-soughtafter *** progress in the advancement of rational catalyst design routinely takes queues from ***,enzymes are renowned for their high efficiency and selectivity in diverse and significant reactions under mild *** the well-known merits of enzymes,they often remain unsuitable for industrial catalysis due to issues,including limited environment(solvent/temperature/pH)compatibility,considerable structural uncertainty,and highly specific reaction *** the context of bioinspired catalysis design,the development of synthetic heterogeneous catalyst analogs,which may not only mimic enzymes to reproduce or even surpass their performance but also bypass their intrinsic limitations,is thus,desirable and has been extensively studied in the context of porous *** metal-organic framework(MOF)is a superior candidate for porous materials towards this goal,thanks to facile and modular preparation,explicit crystalline composition/structure,tunable pore size/environment,and excellent *** introduction of active molecular species such as bioactive molecules(e.g.,proteins,enzymes,peptides,amino acids,porphyrins)and chemically active molecules(e.g.,frustrated lewis pairs)into metal-organic frameworks(MOFs)via pore encapsulation,chemical postmodification,or bottom-up construction has been shown to facilitate the cooperative enhancement of catalysis through the enforcement of proximity,enhancement of control/activity,and even inducement of unexpected *** this minireview,we sought to summarize the last 5 years of fruitful progress,exploiting MOFs housing active molecules for substantial catalysis applications,including asymmetric reactions,CO_(2)conversion(reduction,cycloaddition),biocatalytic H_(2)O_(2)/dye degradation,and so on,and discuss challenges and opportunities in the prospective exploration of these system

关键词： metal-organic framework bioinspired catalyst active molecular species

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Development of an active-site titrant for SARS-CoV-2 main protease as an indispensable tool for evaluating enzyme kinetics

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Acta Pharmaceutica Sinica B 2024年第5期14卷 2349-2357页

作者： Rabea Voget Julian Breidenbach Tobias Claff Alexandra Hingst Katharina Sylvester Christian Steinebach Lan Phuong Vu Renato H.Weiße Ulrike Bartz Norbert Sträter Christa e.Müller Michael Gütschow Pharmaceutical Institute Pharmaceutical&Medicinal ChemistryUniversity of BonnBonn 53121Germany Institute of Bioanalytical Chemistry Center for Biotechnology and BiomedicineLeipzig UniversityLeipzig 04103Germany Department of Natural Sciences University of Applied Sciences Bonn-Rhein-SiegRheinbach 53359Germany

A titrant for the SARS-CoV-2 main protease(M^(pro))was developed that enables,for the first time,the exact determination of the concentration of the enzymatically active M^(pro) by active-site *** covalent binding mode of the tetrapeptidic titrant was elucidated by the determination of the crystal structure of the enzyme–titrant *** fluorogenic substrates of M^(pro),including a prototypical,internally quenched Dabcyl-eDANS peptide,were compared in terms of solubility under typical assay *** exploiting the new titrant,key kinetic parameters for the M^(pro)-catalyzed cleavage of these substrates were determined.

关键词： COVID-19 SARS-CoV-2 Main protease Peptide nitriles Fluorogenic substrates Active-site titration X-ray crystallography Inner filter effect

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OsbZIP53 Negatively Regulates Immunity Response by Involving in Reactive Oxygen Species and Salicylic Acid Metabolism in Rice

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Rice science 2024年第2期31卷 190-202,I0022-I0028页

作者： WU Lijuan HAN Cong WANG Huimei He Yuchang LIN Hai WANG Lei CHeN Chen e Zhiguo State.key Laboratory of Rice Biology and Breeding China National Rice Research InstituteHangzhou 310006China Jiangsu key Laboratory of Crop Genetics and Physiology/key Laboratory of Plant Functional Genomics of the Ministry of education/Jiangsu key Laboratory of Crop Genomics and Molecular Breeding/Jiangsu Co-Innovation Center for Modern Production Technology of Grain Crops Agricultural College of Yangzhou UniversityYangzhou 225009China

The basic region/leucine zipper(bZIP)transcription factors play important roles in plant development and responses to abiotic and biotic ***53 regulates resistance to Magnaporthe oryzae in rice by analyzing APIP5-RNAi transgenic *** further investigate the biological functions of OsbZIP53,we generated osbzip53 mutants using CRISPR/Cas9 editing and also constructed OsbZIP53 over-expression transgenic *** analysis of phenotypical,physiological,and transcriptional data showed that knocking-out OsbZIP53 not only improved disease resistance by inducing a hypersensitivity response in plants,but also regulated the immune response through the salicylic acid ***,disrupting OsbZIP53 increased H2O2 accumulation by promoting reactive oxygen species generation through up-regulation of several respiratory burst oxidase homologs(Osrboh genes)and weakened H2O2 degradation by directly targeting *** addition,the growth of osbzip53 mutants was seriously impaired,while OsbZIP53 over-expression lines displayed a similar phenotype to the wild type,suggesting that OsbZIP53 has a balancing effect on rice immune response and growth.

关键词： OsbZIP53 hypersensitive response reactive oxygen species metabolism rice immunity salicylic acid transcription factor

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Canonical and noncanonical Wnt signaling: Multilayered mediators, signaling mechanisms and major signaling crosstalk

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Genes & Diseases 2024年第1期11卷 103-134页

作者： Kevin Qin Michael Yu Jiaming Fan Hongwei Wang Piao Zhao Guozhi Zhaoo Wei Zeng Connie Chen Yonghui Wang Annie Wang Zander Schwartz Jeffrey Hong Lily Song William Wagstaff Rex C.Haydon Hue H.Luu Sherwin H.Ho Jason Strelzow Russell R.Reid Tong-Chuan He lewis L.Shi Chicago Medical School Rosalind Franklin University of Medicine and ScienceNorth ChicagoIL 60064USA Molecular Oncology Laboratory Department of Orthopaedic Surgery and Rehabilitation MedicineThe University of Chicago Medical CenterChicagoIL 60637USA Ministry of education key Laboratory of Diagnostic Medicine and Department of Clinical BiochemistryThe School of Laboratory MedicineChongqing Medical UniversityChongqing 400016China Departments of Orthopaedic Surgery and Urology The First Affiliated Hospital of Chongqing Medical UniversityChongqing 400016China Department of Interventional Neurology The First Dongguan Affiliated HospitalGuangdong Medical UniversityDongguanGuangdong 523475China Department of Clinical Laboratory Medicine Shanghai Jiaotong University School of MedicineShanghai 200000China School of Biomedical engineering Vanderbilt UniversityNashvilleTN 37235USA Laboratory of Craniofacial Biology and Development Department of Surgery Section of Plastic SurgeryThe University of Chicago Medical CenterChicagoIL 60637USA

Wnt signaling plays a major role in regulating cell proliferation and *** Wnt ligands are a family of 19 secreted glycoproteins that mediate their signaling effects via binding to Frizzled receptors and LRP5/6 coreceptors and transducing the signal either throughβ-catenin in the canonical pathway or through a series of other proteins in the nonca-nonical *** of the individual components of both canonical and noncanonical Wnt signaling have additional functions throughout the body,establishing the complex interplay between Wnt signaling and other signaling *** crosstalk between Wnt signaling and other pathways gives Wnt signaling a vital role in many cellular and organ ***-regulation of this system has been implicated in many diseases affecting a wide array of organ systems,including cancer and embryological defects,and can even cause embryonic *** complexity of this system and its interacting proteins have made Wnt signaling a target for many therapeutic ***,both stimulatory and inhibitory treatments come with potential risks that need to be *** review synthesized much of the current knowl-edge on the Wnt signaling pathway,beginning with the history of Wnt *** thoroughly described the different variants of Wnt signaling,including canonical,noncanonical Wnt/PCP,and the noncanonical Wnt/Ca2+*** description involved each of its components and their involvement in other cellular ***,this review explained the various other pathways and processes that crosstalk with Wnt signaling.

关键词： β-catenin Canonical Wnt Noncanonical Wnt Signal transduction Signaling crosstalk

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extractable and kerogen-bound hopanoids from typical eocene oil shales in China

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energy Geoscience 2024年第2期5卷 171-179页

作者： Changbo Zhai Zhirong Zhang John K.Volkman Hong Lu Yan'e Chen SINOPeC key Laboratory of Petroleum Accumulation Mechanisms Wuxi Institute of Petroleum GeologySINOPEC2060 Lihu RoadWuxiJiangsu213126China SINOPeC Petroleum exploration and Production Research Institute 31 Xueyuan RoadBeijing100083China State.key Laboratory of Organic Geochemistry Guangzhou Institute of GeochemistryChinese Academy of ScienceGuangzhou510640GuangdongChina

This study conducted a comparative analysis of extractable hopanoid hydrocarbons and those released via stepwise pyrolysis of typical eocene immature oil shales in China,namely the Huadian,Maoming,and Fushun *** the Huadian and Maoming shales exhibit immature indicators in extractable and kerogen-bound hopanoids(notably,high abundance of C_(29)to C_(32)17β,21β-hopanes and unsaturated hopenes).In contrast,the Fushun oil shale's hopanoids from extracts and pyrolyzates suggest a higher maturity *** absence of neohopenes in the pyrolyzates of the shales underpins that the kerogenbound hopanoid skeletons resist ***,the Huadian oil shale's asymmetric distribution of C_(29)and C_(30)hopenes and neohopenes hints at the presence of an additional *** unsaturated hopenes,such as hop-20(21)-enes,identified in pyrolyzates of the three kerogens at various pyrolysis temperatures,reveal the occurrence of double bonds in kerogen-bound hopanoid skeletons without methyl *** absence of hop-20-(21)-ene in extracts suggests that it might act as an intermediate of these novel hopenes during the epimerization of hopanoid skeletons within *** extractable and pyrolytic hopanoids'stereochemical alignment indicates that epimerization may occur in both ring systems and alkyl side chains of kerogen-bound hopanoid *** stepwise pyrolysis proves to be a quick screening method for geological hopanoids without causing any significant alteration to the original skeletons even when cracking multiple covalent bonds is necessary.

关键词： Hopanoid Hopane Hopene Neohopene Stepwise pyrolysis Kerogen eocene oil shale

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An inulin-type fructan CP-A from Codonopsis pilosula attenuates experimental colitis in mice by promoting autophagy-mediated inactivation of NLRP3 inflammasome

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Chinese Journal of Natural Medicines 2024年第3期22卷 249-264页

作者： ZHOU Jiangtao WANG Jun WANG Jiajing LI Deyun HOU Jing LI Jiankuan BAI Yun’e GAO Jianping School of Pharmaceutical Science Shanxi Medical UniversityJinzhong 030600China

Inulin-type fructan CP-A,a predominant polysaccharide in Codonopsis pilosula,demonstrates regulatory effects on immune activity and *** efficacy of CP-A in treating ulcerative colitis(UC)is,however,not *** study employed an in vitro lipopolysaccharide(LPS)-induced colonic epithelial cell model(NCM460)and an in vivo dextran sulfate sodium(DSS)-induced colitis mouse model to explore CP-A’s protective effects against experimental colitis and its underlying *** monitored the clinical symptoms in mice using various parameters:body weight,disease activity index(DAI),colon length,spleen weight,and histopathological ***,molecular markers were assessed through enzyme-linked immunosorbent assay(eLISA),quantitative real-time polymerase chain reaction(qRT-PCR),immunofluorescence(IF),immunohistochemistry(IHC),and Western blotting *** showed that CP-A significantly reduced reactive oxygen species(ROS),tumor necrosis factor-alpha(TNF-α),and interleukins(IL-6,IL-1β,IL-18)in LPS-induced cells while increasing IL-4 and IL-10 levels and enhancing the expression of Claudin-1,ZO-1,and occludin proteins in NCM460 ***,in vivo findings revealed that CPA administration markedly improved DAI,reduced colon shortening,and decreased the production of myeloperoxidase(MPO),malondialdehyde(MDA),ROS,IL-1β,IL-18,and NOD-like receptor protein 3(NLRP3)inflammasome-associated genes/proteins in UC ***-A treatment also elevated glutathione(GSH)and superoxide dismutase(SOD)levels,stimulated autophagy(LC3B,P62,Beclin-1,and ATG5),and reinforced Claudin-1 and ZO-1 expression,thereby aiding in intestinal epithelial barrier repair in colitis ***,the inhibition of autophagy via chloroquine(CQ)diminished CP-A’s protective impact against colitis in *** findings elucidate that CP-A’s therapeutic effect on experimental colitis possibly involves mitigating intestinal inflammation through autophagymediated N

关键词： Inulin-type fructan CP-A Codonopsis pilosula Ulcerative colitis NLRP3 inflammasome Autophagy

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Challenges and countermeasures for developing countries in addressing loss and damage caused by climate change

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Advances in Climate Change Research 2024年第2期15卷 353-363页

作者： Shuo LIU Yu-e LI Bin WANG An-Dong CAI Chao FeNG Hua LAN Ruo-Chen ZHAO Institute of environment and Sustainable Development in Agriculture Chinese Academy of Agricultural SciencesBeijing 100081China key Laboratory of Agricultural environment Ministry of Agriculture and Rural AffairsBeijing 100081China China Clean Development Mechanism Fund Management Center Beijing 100045China School of International Law China University of Political Science and LawBeijing 100088China

Loss and damage caused by extreme climate events have attracted increasing *** 28th Conference of the Parties to the United Nations Framework Convention on Climate Change(hereinafter referred to as the Convention)has agreed to adopt Loss and Damage Fund agreement,which identified the source of funding and the funds to be entrusted to the World ***,there is still ambiguous that how to allocate the funds could accelerate the effectiveness of meeting the needs for developing ***-disaster prevention and preparedness is one of the most effective measures to deal with loss and damage,which closely related to *** studies rarely analyzed quantitatively the financial needs of pre-disaster prevention and preparedness relating to adaptation to reduce loss and *** on the official reports submitted by countries under the Convention,this study analyzes the annual change in the total financial support provided by developed countries to developing countries,the proportion of pre-disaster prevention and preparedness in the adaptation needs of developing countries,and the progress in raising the current annual funding target of 100 billion USD for developed countries,to reveal the financial and technical challenges facing by developing countries on addressing loss and *** results show that by 2030,the total adaptation financial needs of developing countries are estimated to be about 3.8 trillion USD,of which pre-disaster prevention matters account for about 9%.Therefore,by 2030,developing countries will need about 342 billion USD in pre-disaster prevention and preparedness finance to withstand loss and *** addition,developing countries face a lack of technical methods to quantify information about their *** on the above analysis,this study puts forward countermeasures and suggestions,including strengthening the allocation amount of loss and damage fund on pre-disaster warning,prevention and control actions,and

关键词： Loss and damage Funding mechanism Pre-disaster warning and preparedness Convention negotiations Countermeasures

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Paleoclimatic application of spectral parameters to the eolian red clay of the Jianzha Basin,northeastern margin of the Tibetan Plateau

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Science China earth Sciences 2024年第6期67卷 1952-1966页

作者： Chaofeng FU Ju’e TIAN Xinwen XU Yougui SONG Jun ZUO Feng WANG Lin CHeN Pengfei LI Xiaoke QIANG The School of earth Science and Resources Chang’an UniversityXi’an 710054China State.key Laboratory of Loess and Quaternary Geology Institute of Earth and EnvironmentCASXi’an 710061China College of Urban and environmental Science Northwest UniversityXi’an 710069China CAS Center for excellence in Quaternary Science and Global Change Xi’an 710061China

Reflectance spectroscopy is rapid,inexpensive,and non-destructive and can provide important information about the mineralogy of rocks and *** measured the reflectance spectroscopy of Miocene red clay deposits on the northeastern margin of the Tibetan Plateau,with the aim of developing a rapid methodology for detecting paleoclimatic *** obtained visible/near-infrared(VNIR)and short-wave infrared(SWIR)spectroscopy data from the red clay in the Jianzha Basin,and analyzed their relationship with independent paleoclimatic records,including mineral contents and environmental magnetic *** results show that the VNIR parameters,including D500,D900,R500,and R900(where D and R represent the depth and reflectance of the absorption peaks around 500 and 900 nm,respectively)are temperature-sensitive and correlated with the magnetic susceptibility,frequency-dependent magnetic susceptibility,and the marine δ^(18)O *** results of frequency-domain analysis of the VNIR parameters show that they reflect climate change on orbital *** parameters,such as AS1400,D1400/D1900 and D1900(where AS represents the asymmetry of the absorption peaks around1400 nm),are correlated with the illite and montmorillonite content,and they are sensitive to the weathering *** spectral parameters of the eolian red clay in the Jianzha Basin reflect regional climatic changes caused by the uplift of the Tibetan Plateau at~8.5 Ma and global climatic cooling at~7.2 Ma,and thus they are applicable as both regional and global paleoenvironmental indicators.

关键词： Visible/near-infrared spectroscopy Short-wave infrared spectroscopy Paleoclimatic indicators Red clay Tibetan Plateau

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3D Printed Polyimide/Silica Composite Aerogels for Customizable Thermal Insulation from-50℃ to 1300℃

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Chinese Journal of Polymer Science 2024年第7期42卷 936-945,I0007页

作者： Dingyi Yu Tiantian Xue Zhuocheng Ma Zaiyin Hu Lijuan Long Yue-e Miao Wei Fan Tianxi Liu State.key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghai201620China key Laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi214122China Guizhou Aerospace Wujiang electro-Mechanical equipment Co. Ltd.Zunyi563000China School of Materials and Architectural engineering Guizhou Normal UniversityGuiyang550025China

Aerogels are widely used as thermal insulation materials because of their high porosity and low bulk ***,the insulation performance of aerogels is limited to a narrow temperature ***,the preparation of aerogel materials with precisely controlled and complex architectures is still ***,we report 3D printed polyimide/silica aerogel particle(PI/SAP)composite aerogels for thermal insulation in a wide range of temperature with customized *** printability and shape fidelity of 3D printed composite aerogels is improved by adding hydrophilic SAP as a rheology *** resulting PI/SAP composite aerogel exhibits excellent flame-retardant properties and thermal insulation from-50℃ to 1300℃.Moreover,the PI/SAP composite aerogel with customized shape can be applied for battery insulation at subzero temperatures,promising to be used as customizable and stable insulating materials in a variety of complex and extreme applications.

关键词： 3D printing Polyimide Aerogel Silica Thermal insulation

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Ultrafast magneto-optical dynamics in nickel(111)single crystal studied by the integration of ultrafast reflectivity and polarimetry probes

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Chinese Physics B 2024年第3期33卷 65-69页

作者：匡皓余军潇陈洁 H.e.elsayed-Ali 李润泽 Peter M.Rentzepis School of Physical Science and Technology ShanghaiTech UniversityShanghai 201210China Center for Transformative Science ShanghaiTech UniversityShanghai 201210China Center for Ultrafast Science and Technology Key Laboratory for Laser Plasmas (Ministry of Education)Collaborative Innovation Center of IFSA (CICIFSA)School of Physics and AstronomyShanghai Jiao Tong UniversityShanghai 200240China Department of electrical and Computer engineering Old Dominion UniversityNorfolkVirginia 23529USA Department of electrical and Computer engineering Texas A&M UniversityCollege StationTexas 77843USA

With the integration of ultrafast reflectivity and polarimetry probes,we observed carrier relaxation and spin dynamics induced by ultrafast laser excitation of Ni(111)single *** carrier relaxation time within the linear excitation range reveals that electron-phonon coupling and dissipation of photon energy into the bulk of the crystal take tens of *** the other hand,the observed spin dynamics indicate a longer time of about 120 *** further understand how the lattice degree of freedom is coupled with these dynamics may require the integration of an ultrafast diffraction probe.

关键词： ultrafast spin dynamics non-equilibrium dynamics multi-probe

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