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Understanding the role of transition metal single-atom electronic structure in oxysulfur radical-mediated oxidative degradation

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Environmental Science and Ecotechnology 2024年第4期20卷 247-258页

作者： Guanshu Zhao Jing Ding Jiayi Ren Qingliang Zhao Chengliang Mao Kun Wang jessica ye Xueqi Chen Xianjie Wang Mingce Long State Key Laboratory of Urban Water Resources and Environment School of EnvironmentHarbin Institute of TechnologyHarbin150090China Solar Fuels Group Department of ChemistryUniversity of Toronto80 St.George StreetTorontoOntarioM5S 3H6Canada School of Physics Harbin Institute of TechnologyHarbin150001China School of Environmental Science and Engineering Key Laboratory of Thin Film and Microfabrication Technology(Ministry of Education)Shanghai Jiao Tong University800 Dongchuan RoadShanghai200240China

The ubiquity of refractory organic matter in aquatic environments necessitates innovative removal *** radical-based advanced oxidation has emerged as an attractive solution,offering high selectivity,enduring efficacy,and anti-interference *** many technologies,sulfite activation,leveraging its cost-effectiveness and lower toxicity compared to conventional persulfates,stands ***,the activation process often relies on transition metals,suffering from low atom *** we introduce a series of single-atom catalysts(SACs)employing transition metals on g-C_(3)N_(4)substrates,effectively activating sulfite for acetaminophen *** highlight the superior performance of Fe/CN,which demonstrates a degradation rate constant significantly surpassing those of Ni/CN and Cu/*** investigation into the electronic and spin polarization characteristics of these catalysts reveals their critical role in catalytic efficiency,with oxysulfur radical-mediated reactions ***,under visible light,the catalytic activity is enhanced,attributed to an increased generation of oxysulfur radicals and a strengthened electron donation-back donation *** proximity of Fe/CN's d-band center to the Fermi level,alongside its high spin polarization,is shown to improve sulfite adsorption and reduce the HOMO-LUMO gap,thereby accelerating photo-assisted sulfite *** work advances the understanding of SACs in environmental applications and lays the groundwork for future water treatment technologies.

关键词： Single-atom catalysts(SACs) Oxysulfur radical Sulfite activation Spin polarization Electronic structure

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Leptogenesis via a varying Weinberg operator:a semi-classical approach

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Chinese Physics C 2019年第3期43卷 22-28页

作者： Silvia Pascoli jessica Turner ye-Ling Zhou Institute for Particle Physics Phenomenology Department of PhysicsDurham UniversitySouth RoadDurham DH1 3LEUnited Kingdom Theoretical Physics Department Fermi National Accelerator LaboratoryP.O.Box 500BataviaIL 60510USA

In this paper, we introduce leptogenesis via a varying Weinberg operator from a semi-classical *** mechanism is motivated by the breaking of an underlying symmetry which triggers a phase transition that causes the coupling of the Weinberg operator to become dynamical. Consequently, a lepton anti-lepton asymmetry arises from the interference of the Weinberg operator at two different spacetime points. Using the semi-classical approach,we treat the Higgs as a background field and show that a reflection asymmetry between leptons and anti-leptons is generated in the vicinity of the bubble wall. We solve the equations of motion of the lepton and anti-lepton quasiparticles to obtain the final lepton asymmetry.

关键词： leptogenesis Weinberg operator phase transition

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Targeting papain-like protease for broad-spectrum coronavirus inhibition

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Protein & Cell 2022年第12期13卷 940-953页

作者： Shuofeng Yuan Xiaopan Gao Kaiming Tang Jian-Piao Cai Menglong Hu Peng Luo Lei Wen Zi-Wei ye Cuiting Luo jessica Oi-Ling Tsang Chris Chun-Yiu Chan Yaoqiang Huang Jianli Cao Ronghui Liang Zhenzhi Qin Bo Qin Feifei Yin Hin Chu Dong-Yan Jin Ren Sun Jasper Fuk-Woo Chan Sheng Cui Kwok-Yung Yuen State Key Laboratory of Emerging Infectious Diseases Li Ka Shing Faculty of MedicineThe University of Hong KongPokfulamHong Kong SARChina Department of Microbiology Li Ka ShingFaculty of MedicineThe University of Hong KongPokfulamHong Kong SARChina NHC Key Laboratory of Systems Biology of Pathogens Institute of Pathogen BiologyChinese Academy of Medical Sciences and Peking Union Medical CollegeBeijing 100730China School of Biomedical Sciences Li Ka Shing Faculty of MedicineThe University of Hong KongPokfulamHong Kong SARChina Department of Molecular and Medical Pharmacology David Geffen School of MedicineUniversity of California Los AngelesLos AngelesCAUSA Key Laboratory of Tropical Translational Medicine of Ministry of Education Hainan Medical UniversityHaikou 571199China Academician Workstation of Hainan Province Hainan Medical UniversityHaikou 571199China Hainan Medical University-The University of Hong Kong Joint Laboratory of Tropical Infectious Diseases The University of Hong KongPokfulamHong Kong Special Administrative RegionChina Guangzhou Laboratory Guangzhou 510320China Department of Clinical Microbiology and Infection Control The University of Hong Kong-Shenzhen HospitalShenzhen 518053China

The emergence of SARS-CoV-2 variants of concern and repeated outbreaks of coronavirus epidemics in the past two decades emphasize the need for next-generation pan-coronaviral *** the multi-functional papain-like protease(PLpro)domain of the viral nsp3 holds ***,none of the known coronavirus PLpro inhibitors has been shown to be in vivo ***,we screened a structurally diverse library of 50,080 compounds for potential coronavirus PLpro inhibitors and identified a noncovalent lead inhibitor F0213 that has broad-spectrum anti-coronaviral activity,including against the Sarbecoviruses(SARSCoV-1 and SARS-CoV-2),Merbecovirus(MERS-CoV),as well as the Alphacoronavirus(hCoV-229E and hCoVOC43).Importantly,F0213 confers protection in both SARS-CoV-2-infected hamsters and MERS-CoV-infected human DPP4-knockin mice.F0213 possesses a dual therapeutic functionality that suppresses coronavirus replication via blocking viral polyprotein cleavage,as well as promoting antiviral immunity by antagonizing the PLpro deubiquitinase *** the significant difference of substrate recognition,mode of inhibition studies suggest that F0213 is a competitive inhibitor against SARS2-PLpro via binding with the 157K amino acid residue,whereas an allosteric inhibitor of MERSPLpro interacting with its 271E *** proof-ofconcept findings demonstrated that PLpro is a valid target for the development of broad-spectrum anticoronavirus *** orally administered F0213 may serve as a promising lead compound for combating the ongoing COVID-19 pandemic and future coronavirus outbreaks.

关键词： protease inhibitor coronavirus Nsp3 antiviral

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Baseline gut microbiota and metabolome predict durable immunogenicity to SARS-CoV-2 vaccines

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Signal Transduction and Targeted Therapy 2023年第10期8卷 5085-5095页

作者： ye Peng Lin Zhang Chris K.P.Mok jessica Y.L.Ching Shilin Zhao Matthew K.L.Wong Jie Zhu Chunke Chen Shilan Wang Shuai Yan Biyan Qin Yingzhi Liu Xi Zhang Chun Pun Cheung Pui Kuan Cheong Ka Long Ip Adrian C.H.Fung Kenneth K.Y.Wong David S.C.Hui Francis K.L.Chan Siew C.Ng Hein M.Tun Microbiota I-Center(MaglC) Hong KongChina Jockey Club School of Public Health and Primary Care The Chinese University of Hong KongHong KongChina Li Ka Shing Institute of Health Sciences Faculty of MedicineThe Chinese University of Hong KongHong KongChina Department of Medicine and Therapeutics The Chinese University of Hong KongHong KongChina Department of Surgery LKS Faculty of MedicineThe University of Hong KongHong KongChina Stanley Ho Centre for Emerging Infectious Diseases Faculty of MedicineThe Chinese University of Hong KongHong KongChina Centre for Gut Microbiota Research The Chinese University of Hong KongHong KongChina

The role of gut microbiota in modulating the durability of cOVID-19 vaccine immunity is yet to be *** this cohort study,we collected blood and stool samples of 121 BNT162b2 and 40 CoronaVac vaccinees at baseline,1 month,and 6 months post vaccination(p.v).Neutralisation antibody,plasma cytokine and chemokines were measured and associated with the gut microbiota and metabolome composition.

关键词： vaccine immunity vaccines

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Identification of novel small-molecule inhibitors of SARS-CoV-2 by chemical genetics

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Acta Pharmaceutica Sinica B 2024年第9期14卷 4028-4044页

作者： Chris Chun-Yiu Chan Qian Guo Jasper Fuk-Woo Chan Kaiming Tang Jian-Piao Cai Kenn Ka-Heng Chik Yixin Huang Mei Dai Bo Qin Chon Phin Ong Allen Wing-Ho Chu Wan-Mui Chan Jonathan Daniel Ip Lei Wen jessica Oi-Ling Tsang Tong-Yun Wang Yubin Xie Zhenzhi Qin Jianli Cao Zi-Wei ye Hin Chu Kelvin Kai-Wang To Xing-Yi Ge Tao Ni Dong-Yan Jin Sheng Cui Kwok-Yung Yuen Shuofeng Yuan State Key Laboratory of Emerging Infectious Diseases Carol Yu Centre for InfectionDepartment of MicrobiologySchool of Clinical MedicineLi Ka Shing Faculty of Medicinethe University of Hong KongPokfulamHong Kong SAR 999077China Department of Infectious Diseases and Microbiology the University of Hong Kong-Shenzhen HospitalShenzhen 518000China Centre for Virology Vaccinology and TherapeuticsHong Kong Science and Technology ParkHong Kong SAR 999077China Academician Workstation of Hainan Province Hainan Medical University-the University of Hong Kong Joint Laboratory of Tropical Infectious DiseasesHaikou 571100China School of Biomedical Sciences Li Ka Shing Faculty of Medicinethe University of Hong KongPokfulamHong Kong SAR 999077China NHC Key Laboratory of Systems Biology of Pathogens Institute of Pathogen Biology Chinese Academy of Medical Sciences&Peking Union Medical CollegeBeijing 100730China College of Biology Hunan Provincial Key Laboratory of Medical VirologyHunan UniversityChangsha 410082China

There are only eight approved small molecule antiviral drugs for treating *** them,four are nucleotide analogues(remdesivir,JT001,molnupiravir,and azvudine),while the other four are protease inhibitors(nirmatrelvir,ensitrelvir,leritrelvir,and simnotrelvir-ritonavir).Antiviral resistance,unfavourable drug‒drug interaction,and toxicity have been reported in previous *** there is a dearth of new treatment options for *** this work,a three-tier cell-based screening was employed to identify novel compounds with anti-SARS-CoV-2 *** compound,designated 172,demonstrated broad-spectrum antiviral activity against multiple human pathogenic coronaviruses and different SARS-CoV-2 variants of *** studies validated by reverse genetics showed that compound 172 inhibits the 3-chymotrypsin-like protease(3CLpro)by binding to an allosteric site and reduces 3CLpro dimerization.A drug synergistic checkerboard assay demonstrated that compound 172 can achieve drug synergy with nirmatrelvir in *** vivo studies confirmed the antiviral activity of compound 172 in both Golden Syrian Hamsters and K18 humanized ACE2 ***,this study identified an alternative druggable site on the SARS-CoV-23CLpro,proposed a potential combination therapy with nirmatrelvir to reduce the risk of antiviral resistance and shed light on the development of allosteric protease inhibitors for treating a range of coronavirus diseases.

关键词： SARS-CoV-2 High throughput screening Broad-spectrum antiviral treatment 3CLpro inhibitor Allosteric-site inhibitor Animal models Chemical genetics Reverse genetics

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