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Identifying the Active Site of Water Oxidation Catalyst Based on Defective Fe-Doped Ni Oxyhydroxide

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CCS Chemistry 2024年第2期6卷 365-376页

作者： Yunxuan Ding Jian Du Tao Wang Licheng Sun Institute of natural sciences Westlake Institute for Advanced StudyHangzhou 310024 Center of Artificial Photosynthesis for Solar Fuels Department of ChemistrySchool of ScienceWestlake UniversityHangzhou 310024

Electrochemical water splitting plays a crucial role in storing sustainable energy into H2 as an ideal fuel,in which the anodic oxygen evolution reaction(OER)is the bottleneck.Currently,Fe-doped NiOOH(Ni_(1−x)Fe_(x)OOH)is a promising OER catalyst under alkaline conditions.However,the specific active sites responsible for their good performances remain debatable.Here,we identify a nickel-oxygen radical(Ni–O·)and an iron-oxo(Fe=O)group as two essential states for adsorbed oxygen.Meanwhile,both thermochemical O–O coupling and electrochemical OER elementary steps are considered on the Ni_(1−x)Fe_(x)OOH catalysts.Sophisticated mechanistic studies with a combined density functional theory simulation and experimental analysis unravel that both the Ni and Fe centers can act as the active sites for the defective Ni_(1−x)Fe_(x)OOH to catalyze OER,depending on the nature of the defect.The presence of Fe can benefit the stabilization of the defective surface and influence the electronic property of the nearby Ni site.This work not only identifies the intrinsic active sites of Ni_(1−x)Fe_(x)OOH,but also illustrates the essential roles of defects in catalysis,which sheds light on the design of more efficient OER catalysts in the future.

关键词： defect water nucleophilic attack oxygen evolution reaction heterogeneous catalysis density functional calculations

The first record of a Konservat-Lagerstätten in which early post-settlement stages of fossil archaeobalanids(Cirripedia:Balanomorpha)are preserved

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Integrative Zoology 2024年第2期19卷 200-223页

作者： Tomáš KOCÍ Rok GAŠPARIC John BUCKERIDGE Martina KOCOVÁ VESELSKÁ Aleš ŠOSTER Ivancická581 PragueCzech Republic Palaeontological department Natural History MuseumNational MuseumPragueCzech Republic Oertijdmuseum Bosscheweg 80Boxtel5293 WBThe Netherlands Institute for Palaeobiology and Evolution Novi TrgKamnikSlovenia Earth and Oceanic Systems Group RMIT UniversityMelbourneAustralia Museums Victoria CarltonVictoriaAustralia department of Paleobiology and Paleoecology Institute of Geology of the Czech Academy of SciencesPragueCzech Republic Institute of Geology and Palaeontology Charles UniversityPragueCzech Republic Faculty of natural sciences and Engineering University of LjubljanaLjubljanaSlovenia

A diverse sessile barnacle fauna from a Miocene shallow-water deposit at Dolnja Stara vas in Slovenia is described.It includes the first descriptions of early post settlement juveniles of Actinobalanus sloveniensis attached to mangrove leaves.These represent three distinct growth phases,the earliest being interpreted as being less than 24 h post settlement,the others being 1 to 2 days post settlement.An assessment of their taphonomy is provided.Associated adult balanomorphs are attached to a variety of organic substrates,including mangrove leaves and branches,fragments of the conifers?Taxodioxylon,Carapoxylon,pine cones,molluscs,and cetacean bones.The barnacles include A.sloveniensis,Amphibalanus venustus,and Perforatus perforatus—many with opercula retained within the shells.A.venustus retains some of the original shell color.This is the second record of barnacle–plant associations from the Central Paratethys from Kamnik and Trbovlje.The paleoecology and paleogeography of the site are discussed.

关键词： acorn barnacles barnacle metamorphosis epibiont paleoecology taxonomy

Evaluation of suitability,adaptability,and reserve potential of construction land on the Qinghai-Tibet Plateau

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Journal of Geographical sciences 2024年第1期34卷 41-61页

作者： YANG Hua XU Yong ZHOU Kan WANG Lijia XU Lin Key Laboratory of Regional Sustainable Development Modeling Institute of Geographic Sciences and Natural Resources ResearchCASBeijing 100101China University of Chinese Academy of sciences Beijing 100049China

Construction land is the leading carrier of human activities such as production and living.Evaluating the construction land suitability(CLS)on the Qinghai-Tibet Plateau(QTP)holds significant implications for harmonizing the relationship between ecological protection and human activity and promoting population and industry layout optimization.However,no relevant studies provide a complete CLS assessment of the QTP.In this study,we developed a model-based CLS evaluation framework coupling of pattern and process to calculate the global CLS on the QTP based on a previously developed CLS evaluation model.Then,using the land-use data of 1990,2000,2010,and 2020,we examined the adaptability of existing construction land(ECL)to the CLS assessment result through the adaptability index and vertical gradient index and further analyzed the limitations of maladaptive construction land.Finally,we calculated the potential area of reserve suitable construction land.This article includes four conclusions:(1)The highly suitable,suitable,moderately suitable,marginally suitable,and unsuitable CLS classes cover areas of 0.33×10^(4)km^(2),10.42×10^(4)km^(2),18.06×10^(4)km^(2),24.12×10^(4)km^(2),and 205.29×10^(4)km^(2),respectively.Only approximately 11%of the study area on the QTP is suitable for large-scale permanent construction land,and approximately 79.50%of the area is unsuitable under current economic and technological conditions.(2)The ECL adaptability index is 85.16%,85.93%,85.18%,and 78.01%during 1990–2020,respectively,with an average adaptability index exceeding 80%on the QTP.The ECL distribution generally conforms to construction land suitable space characteristics but with a significant spatial difference.(3)From 1990 to 2020,the maladaptive ECL was dominated by rural settlement land,transport land,and special land,with a rapidly increasing proportion of urban and other construction land.The maladaptive ECL is constrained by both elevation and slope in the southern Qinghai Plateau,the Hengduan Mountains,and the Qilian Mount

关键词： land resource construction land suitability existing construction land adaptability human activity Qinghai-Tibet Plateau

A fungal CYP from Beauveria bassiana with promiscuous steroid hydroxylation capabilities

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Chinese Chemical Letters 2024年第5期35卷 218-222页

作者： Yu Peng Yue Wang Tian-Jiao Chen Jing-Jing Chen Jin-Ling Yang Ting Gong Ping Zhu State Key Laboratory of Bioactive Substance and Function of natural Medicines NHC Key Laboratory of Biosynthesis of Natural ProductsCAMS Key Laboratory of Enzyme and Biocatalysis of Natural DrugsInstitute of Materia MedicaChinese Academy of Medical Sciences&Peking Union Medical CollegeBeijing 100050China

Hydroxylation of steroid core is critical to the synthesis of steroid drugs.Direct sp^(3) C-H hydroxylation is challenging through chemical catalysis,alternatively,fungal biotransformation offers a possible solution to this problem.However,mining and metabolic engineering of cytochrome P450 monooxygenases(CYPs)is usually regarded as a more eco-friendly and efficient strategy.Herein,we report the mining and identification of a new steroid CYP(CYP68BE1)from Beauveria bassiana by transcriptomics,heterologous expression,in vivo and in vitro functional characterization.The catalytic promiscuity of CYP68BE1 was explored,and CYP68BE1 showed promiscuously and catalytically versatile,which is qualified for monohydroxylation on C11α,C1α,C6βand dihydroxylation on C1β,11αand C6β,11αof six steroids,leading to the production of key steroid intermediates required in the industrial synthesis of some indispensable steroid drugs.Molecular dynamics simulations were performed,revealing the molecular basis of different binding orientations of CYP68BE1 with different substrates.The discovery of CYP68BE1 offers a promising biocatalyst for enriching the steroid structural and functional diversity,which also can be applied to biosynthesize valuable steroid drug intermediates.

关键词： Fungal CYPs Steroid hydroxylase Beauveria bassiana Promiscuous biocatalyst Molecular dynamics

There is more to the knee joint than just the quadriceps:A systematic review with meta-analysis and evidence gap map of hamstring strength,flexibility,and morphology in individuals with gradual-onset knee disorders

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Journal of Sport and Health Science 2024年第4期13卷 521-536页

作者： Helder S.Lopes Marina C.Waiteman Liliam B.Priore Neal R.Glaviano David M.Bazett-Jones Ronaldo V.Briani Fabio M.Azevedo School of Science and Technology Physical Therapy DepartmentSao Paulo State University(UNESP)Presidente Prudente 19060-900Brazil department of Kinesiology College of AgricultureHealth and Natural ResourcesUniversity of ConnecticutStorrsCT 06269USA School of Exercise and Rehabilitation sciences College of Health and Human ServicesUniversity of ToledoToledoOH 43606USA

Background:Impairments in hamstring strength,flexibility,and morphology have been associated with altered knee biomechanics,pain,and function.Determining the presence of these impairments in individuals with gradual-onset knee disorders is important and may indicate targets for assessment and rehabilitation.This systematic review aimed to synthesize the literature to determine the presence of impairments in hamstring strength,flexibility,and morphology in individuals with gradual-onset knee disorders.Methods:Five databases(MEDLINE,Embase,CINAHL,SPORTDiscus,and Web of Science)were searched from inception to September 2022.Only studies comparing hamstring outcomes(e.g.,strength,flexibility,and/or morphology)between individuals with gradual-onset knee disorders and their unaffected limbs or pain-free controls were included.Meta-analyses for each knee disorder were performed.Outcome-level certainty was assessed using the Grading of Recommendations Assessment,Development,and Evaluation,and evidence gap maps were created.Results:Seventy-nine studies across 4 different gradual-onset knee disorders(i.e.,knee osteoarthritis(OA),patellofemoral pain(PFP),chondromalacia patellae,and patellar tendinopathy)were included.Individuals with knee OA presented with reduced hamstring strength compared to pain-free controls during isometric(standard mean difference(SMD)=-0.76,95%confidence interval(95%CI):-1.32 to-0.21)and concentric contractions(SMD=-0.97,95%CI:-1.49 to-0.45).Individuals with PFP presented with reduced hamstring strength compared to painfree controls during isometric(SMD=-0.48,95%CI:-0.82 to-0.14),concentric(SMD=-1.07,95%CI:-2.08 to-0.06),and eccentric contractions(SMD=-0.59,95%CI:-0.97 to-0.21).No differences were observed in individuals with patellar tendinopathy.Individuals with PFP presented with reduced hamstring flexibility when compared to pain-free controls(SMD=-0.76,95%CI:-1.15 to-0.36).Evidence gap maps identified insufficient evidence for chondromalacia patellae and hamstring morphology across all gradual-

关键词： Chondromalacia patellae Knee flexors Knee osteoarthritis Patellar tendinopathy Patellofemoral pain

A naturally derived small molecule compound suppresses tumor growth and metastasis in mice by relieving p53-dependent repression of CDK2/Rb signaling and the Snail-driven EMT

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Chinese Journal of natural Medicines 2024年第2期22卷 112-126页

作者： REN Boxue LI Yang DI Lei CHENG Ranran LIU Lijuan LI Hongmei LI Yi TANG Zhangrui YAN Yongming LU Tao FU Rong CHENG Yongxian WU Zhaoqiu State Key Laboratory of natural Medicines Department of PharmacologySchool of PharmacyChina Pharmaceutical UniversityNanjing 211198China Institute for Inheritance-Based Innovation of Chinese Medicine School of Pharmaceutical SciencesShenzhen University Health Science CenterShenzhen 518060China

The tumor suppressor protein p53 is central to cancer biology,with its pathway reactivation emerging as a promising therapeutic strategy in oncology.This study introduced LZ22,a novel compound that selectively inhibits the growth,migration,and metastasis of tumor cells expressing wild-type p53,demonstrating ineffectiveness in cells devoid of p53 or those expressing mutant p53.LZ22’s mechanism of action involves a high-affinity interaction with the histidine-96 pocket of the MDM2 protein.This interaction disrupted the MDM2-p53 binding,consequently stabilizing p53 by shielding it from proteasomal degradation.LZ22 impeded cell cycle progression and diminished cell proliferation by reinstating the p53-dependent suppression of the CDK2/Rb signaling pathway.Moreover,LZ22 alleviated the p53-dependent repression of Snail transcription factor expression and its consequent EMT,effectively reducing tumor cell migration and distal metastasis.Importantly,LZ22 administration in tumor-bearing mice did not manifest notable side effects.The findings position LZ22 as a structurally unique reactivator of p53,offering therapeutic promise for the management of human cancers with wild-type TP53.

关键词： LZ22 Wild-type p53 p53 Reactivator Snail-driven EMT Tumor growth and metastasis

Novel phenanthrene/bibenzyl trimers from the tubers of Bletilla striata attenuate neuroinﬂammation via inhibition of NF-κB signaling pathway

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Chinese Journal of natural Medicines 2024年第5期22卷 441-454页

作者： SHAO Siyuan SUN Mohan MA Xianjie JIANG Jianwei TIAN Jinying ZHANG Jianjun YE Fei LI Shuai State Key Laboratory of Bioactive Substance and Function of natural Medicines Institute of Materia MedicaChinese Academy of Medical Sciences and Peking Union Medical CollegeBeijing 100050China

Five novel(9,10-dihydro)phenanthrene and bibenzyl trimers,as well as two previously identified biphenanthrenes and bibenzyls,were isolated from the tubers of Bletilla striata.Their structures were elucidated through comprehensive analyses of NMR and HRESIMS spectroscopic data.The absolute configurations of these compounds were determined by calculating rotational energy barriers and comparison of experimental and calculated ECD curves.Compounds 5b and 6 exhibited inhibitory effects on LPS-induced NO production in BV-2 cells,with IC_(50) values of 12.59±0.40 and 15.59±0.83μmol·L^(-1),respectively.A mechanistic study suggested that these compounds may attenuate neuroinflammation by reducing the activation of the AKT/IκB/NF-κB signaling pathway.Additionally,compounds 3a,6,and 7 demonstrated significant PTP1B inhibitory activities,with IC_(50) values of 1.52±0.34,1.39±0.11,and 1.78±0.01μmol·L^(-1),respectively.Further investigation revealed that compound 3a might inhibit LPS-induced PTP1B overexpression and NF-κB activation,thereby mitigating the neuroinflammatory response in BV-2 cells.

关键词： Bletilla striata Phenanthrene/bibenzyl trimer NO inhibition AKT/IκB/NF-κB signaling pathway PTP1B inhibitory effect

Centennial Analysis of Human Activity Intensity and Associated Historical Events in Heilongjiang River Sino-Russo Watershed

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Chinese Geographical Science 2024年第2期34卷 280-293页

作者： SONG Chaoxue LI Xiaoling HE Hongshi Michael SUNDE School of Geographical sciences Northeast Normal UniversityChangchun 130024China School of natural Resources University of MissouriColumbia 65211USA

Human activities in a transborder watershed are complex under the influence of domestic policies,international relations,and global events.Understanding the forces driving human activity change is important for the development of transborder watershed.In this study,we used global historical land cover data,the hemeroby index model,and synthesized major historical events to analyze how human activity intensity changed in the Heilongjiang River(Amur River in Russia)watershed(HLRW).The results showed that there was a strong spatial heterogeneity in the variation of human activity intensity in the HLRW over the past century(1900-2016).On the Chinese side,the human activity intensity change shifted from the plain areas for agricultural reclamation to the mountainous areas for timber extraction.On the Russian side,human activity intensity changes mostly concentrated along the Trans-Siberian Railway and the Baikal-Amur Mainline.Localized variation of human activity intensity tended to respond to regional events while regionalized variation tends to reflect national policy change or broad international events.The similarities and differences between China and Russia in policies and positions in international events resulted in synchronous and asynchronous changes in human activity intensity.Meanwhile,policy shifts were often confined by the natural features of the watershed.These results reveal the historical origins and fundamental connotations of watershed development and contribute to formulating regional management policies that coordinate population,eco-nomic,social,and environmental activities.

关键词： human activity intensity changes hemeroby index centennial scale Heilongjiang River(Amur River in Russia)watershed China Russia

STING signaling in islet macrophages impairs insulin secretion in obesity

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Science China(Life sciences) 2024年第2期67卷 345-359页

作者： Ze Hong Saihua Chen Jing Sun Dan Cheng Hanli Guo Jiahao Mei Xiang Zhang Munire Maimaiti Haiping Hao Peng Cao Haiyang Hu Chen Wang School of Pharmacy Nanjing University of Chinese MedicineNanjing 210023China State Key Laboratory of natural Medicines Department of Life Science and TechnologyChina Pharmaceutical UniversityNanjing 211198China School of Life sciences Westlake UniversityHangzhou 310012China

The innate immune regulator stimulator of interferon genes(STING)mediates self-DNA sensing and leads to the induction of type I interferons and inflammatory cytokines,which promotes the progression of various inflammatory and autoimmune diseases.Innate immune system plays a critical role in regulating obesity-induced islet dysfunction,whereas the potential effect of STING signaling is not fully understood.Here,we demonstrate that STING is mainly expressed and activated in islet macrophages upon high-fat diet(HFD)feeding.Sting^(-/-)alleviates HFD-induced islet inflammation by inhibiting the expression of pro-inflammatory cytokines and the infiltration of macrophages.Mechanically,palmitic acid incubation promotes mitochondrial DNA leakage into the cytosol and subsequently activates STING pathway in macrophages.Additionally,STING activation in macrophages impairs glucose-stimulated insulin secretion by mediating the engulfment ofβcell insulin secretory granules.Pharmacologically inhibiting STING activation enhances insulin secretion to control hyperglycemia.Together,our results reveal a regulatory mechanism in controlling the islet inflammation and insulin secretion in dietinduced obesity and suggest that selective blocking of the STING activation may be a promising strategy for treating type 2 diabetes.

关键词： STING obesity type 2 diabetes insulin macrophages islet