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Enhanced photocatalytic hydrogen production from Co-MOF/CN by nitrogen and sulfur co-doped coal-based carbon quantum dots

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Journal of Rare Earths 2024年第5期42卷 838-850,I0002页

作者： Shiyong Xu Mei Li Yijun Wang Caiyun gao Rongsheng Xu zhiliang jin School of Chemistry and Chemical Engineering North Minzu UniversityYinchuan750021China Ningxia Key Laboratory of Solar Chemical Conversion Technology.North Minzu University.Yinchuan 750021China State Key Laboratory of National Ethnic Affairs Commission Chemical Technology.North Minzu University Yinchuan750021China

A novel composite photocatalyst for photocatalytic decomposition of water for hydrogen evolution was successfully synthesized by in-situ growth of nitrogen and sulfur co-doped coal-based carbon quantum dots(NSCQDs)nanoparticles on the surface of sheet cobalt-based metal-organic framework(Co-MOF)and graphitic carbon nitride(g-C_(3)N_(4),CN).The structure and properties of the obtained catalysts were systematically analyzed.NSCQDs effectively broaden the absorption of Co-MOF and CN in the visible region.The new composite photocatalyst has high hydrogen production activity and the hydrogen production rate reaches 6254μmol/(g·h)at pH=9.At the same time,NSCQDs synergy Co-MOF/CN composites have good stability.After four cycles of hydrogen production,the performance remains relatively stable.The tran sient photocurrent response and Nyquist plot experimental results further demonstrate the improvement of carrier separation efficiency in composite catalysts.The semiconductor type(n-type semico nductor)of the single-phase catalyst was determined by the Mott-Schottky test,and the band structure was analyzed.The conductive and valence bands of CN are-0.99 and 1.72 eV,respectively,and the conduction and valence bands of Co-MOF are-1.85 and 1.33 eV,respectively.Th e mechanism of the photocatalytic reaction can be inferred,that is,Z-type heterojunction is formed between CN an d Co-MOF,and NSCQDs was used as cocatalyst.

关键词： Nitrogen and sulfur co-doped Coal-based carbon quantum dots Co-MOF CN Photocatalytic hydrogen evolution Rare earths

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Reduction in Intrahepatic cccDNA and Integration of HBV in Chronic Hepatitis B Patients with a Functional Cure

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Journal of Clinical and Translational Hepatology 2023年第2期11卷 314-322页

作者： Weiqiang Gan Na gao Lin Gu Zhishuo Mo Xiuqing Pang Ziying Lei zhiliang gao Department of Infectious Diseases The Third Affiliated Hospital of Sun Yat-sen UniversityGuangzhouGuangdongChina Guangdong Key Laboratory of Liver Disease Research The Third Affiliated Hospital of Sun Yat-sen UniversityGuangzhouGuangdongChina Key Laboratory of Tropical Disease Control(Sun Yat-sen University) Ministry of EducationGuangzhouGuangdongChina

Background and Aims:Functional cure(FC)is characterized by the clearance of the hepatitis B surface antigen from the serum of patients with chronic hepatitis B(CHB).However,the level of intrahepatic covalently closed circular DNA(cccDNA)and hepatitis B virus(HBV)integration remains unclear.We conducted this study to determine them and reveal their value in the treatment of CHB.Methods:There were two sessions to elucidate the changes in intrahepatic cccDNA and HBV integration after antiviral therapy.In the first session,116 patients were enrolled and divided into FC,non-functional cure(NFC),and CHB groups,including 48 patients with functionally cured CHB,27 with CHB without functional cure after antiviral treatment,and 41 with treatment-naïve CHB.Patients were tested for both intrahepatic cccDNA and other viral markers.All patients in the FC group were followed up for at least 24 weeks to observe relapse.In the second session,another ten patients were included for in-depth whole-genome sequencing to analyze HBV integration.Results:Thirteen patients in the FC group were negative for intrahepatic cccDNA.Intrahepatic cccDNA was much higher in the CHB group compared with the FC group.Seven patients had HBsAg seroreversion,including two with virological relapse.Integration of HBV was detected in one(33.3%)functionally cured patients and in seven(100%)with CHB.28.0%of the HBV breakpoints were assigned in the 1,500 nt to 1,900 nt range of the HBV genome.Conclusions:After achieving an FC,the rate of intrahepatic cccDNA and HBV integration was significantly reduced in patients with CHB.For those patients who cleared intrahepatic cccDNA,the chances of developing virological relapse were even lower.

关键词： Chronic Hepatitis B Virological markers Functional cure cccDNA Integration

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Constructing two-dimensional interfacial ice-like water at room temperature for nanotribology

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Nano Research 2023年第7期16卷 9977-9982页

作者： Yue Hong Deliang Zhang zhiliang gao Yuge Zhang Qiang Li Mingdong Dong Key Laboratory of Colloid and Interface Chemistry of the Ministry of Education School of Chemistry and Chemical EngineeringShandong UniversityJinan 250100China Interdisciplinary Nanoscience Center(iNANO) Aarhus UniversityAarhus C DK-8000Denmark

Water/solid interfaces play crucial roles in a wide range of physicochemical and technological processes.However,our microscopic understanding of the interfacial water under ambient temperature is relatively primitive.Herein,we report the direct experimental construction of two-dimensional(2D)ice-like water layer on hydrophilic surface at room temperature by using environment-controlled atomic force microscopy.In contrast to the prevailing view that nanoscale confinement is needed for the formation of 2D ice-like water,we find that 2D ice-like water can form on mica surface at temperatures above the freezing point without confinement.The 2D ice-like water layer shows epitaxial relation with the underlying mica lattice and good thermostability.In addition,the growth of ice-like water layer can be well controlled by the mechanical force from the scanning tip.Furthermore,the friction properties of 2D ice-like water layer are also probed by friction force microscopy.It is found that the icelike water layer can dramatically reduce the friction.These results provide deep understanding of 2D ice-like water formation on solid surfaces without nanoscale confinement and suggest means of growing 2D ices on surfaces at room temperature.

关键词： two-dimensional ice friction mica surface atomic force microscopy friction force microscopy

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Co-delivery of enzymes and photosensitizers via metal-phenolic network capsules for enhanced photodynamic therapy

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Chinese Chemical Letters 2022年第4期33卷 1917-1922页

作者： Qian Wang zhiliang gao Kaijie Zhao Peiyu Zhang Qi-Zhi Zhong Qun Yu Shumei Zhai Jiwei Cui Key Laboratory of Colloid and Interface Chemistry of the Ministry of Education School of Chemistry and Chemical EngineeringShandong UniversityJi’nan 250100China ARC Centre of Excellence in Convergent Bio-Nano Science and Technology and the Department of Chemical EngineeringThe University of MelbourneParkvilleVIC 3010United States State Key Laboratory of Microbial Technology Shandong UniversityQingdao 266237China

The intrinsic hypoxic tumor microenvironment and limited accumulation of photosensitizers(PSs) result in unsatisfied efficiency of photodynamic therapy(PDT).To enhance the PDT efficiency against solid tumors,a functional oxygen self-supplying and PS-delivering nanosystem is fabricated via the combination of catalase(CAT),chlorin e6(Ce6) and metal-phenolic network(MPN) capsule.It is demonstrated that the CAT encapsulated in the capsules(named CCM capsules) could catalyze the degradation of hydrogen peroxide(H;O;) to produce molecular oxygen(O;),which could be converted into cytotoxicity reactive oxygen species(ROS) by surface-loaded Ce6 under 660 nm laser irradiation,leading to synergistic anticancer effects in vitro and in vivo.Therefore,the application of CCM capsule could be a promising strategy to improve PDT effectiveness.

关键词： Metal-phenolic network(MPN) Photodynamic therapy(PDT) Capsule Oxygen self-supply Drug delivery

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Ensemble of single-atom catalysis and defect engineering in Cu_(1)/CeO_(2) nanozymes for tumor therapy

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中国科学:化学英文版 2023年第9期66卷 2590-2599页

作者： Hao-Xin Liu zhiliang gao Han Yan Shan-Qing Li Wei-Wei Wang Xuetao Qin Hongning Sun Jiwei Cui Chun-Jiang Jia Key Laboratory of Colloid and Interface Chemistry Key Laboratory of Special Aggregated Materials of the Ministry of EducationSchool of Chemistry and Chemical EngineeringShandong UniversityJinan 250100China School of Materials and Environmental Engineering Chizhou UniversityChizhou 247000China

As a class of nanomaterials with natural enzyme-like characteristics, nanozymes have shown their great potential in various applications. Reducible metal oxides featured with defect structures, and single-atom catalysts with isolated metal sites are regarded as two of the most promising nanozymes. However, the strategies to construct highly performed nanozymes by combining these advantages are rarely reported. Herein, we report the coordination-unsaturated single-atomic Cu species supported on sintered CeO_(2), which combines the advantages of defect engineering and single-atom catalysis, exhibiting a largely enhanced peroxidase(POD)-like activity. The high-temperature calcination induces the transformation of inert Cu_(1)O_(4) species into coordination-unsaturated Cu_(1)O_(3) sites. This novel Cu_(1)O_(3) active sites with an unsaturated coordination work as a new type of defect sites to greatly activate the isolated Cu atoms and accelerate the dissociation of H_(2)O_(2) to form hydroxyl radicals(·OH). The obtained nanozyme with a high POD-like activity possesses low cytotoxicity, showing potential applications for the tumor inhibition in vitro and in vivo.

关键词： single-atom catalysis oxygen defect Cu/CeO_(2) peroxidase-like activity tumor inhibition

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抗病毒治疗后慢性乙型肝炎HBsAg阴转的预测因子

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中华肝脏病杂志 2024年第2期32卷 186-192页

作者：吴丽丽高志良中山大学附属第三医院感染科广州510630

乙型肝炎表面抗原(HBsAg)阴转(HBsAg<0.05 IU/ml)是现阶段肝炎领域的研究热点,达到HBsAg阴转的患者其肝脏相关的并发症明显减少。目前关于HBsAg阴转的研究较多,但临床中用于预测HBsAg阴转的指标仍偏少。基线低HBsAg定量及治疗过程中的... 详细信息

乙型肝炎表面抗原(HBsAg)阴转(HBsAg<0.05 IU/ml)是现阶段肝炎领域的研究热点,达到HBsAg阴转的患者其肝脏相关的并发症明显减少。目前关于HBsAg阴转的研究较多,但临床中用于预测HBsAg阴转的指标仍偏少。基线低HBsAg定量及治疗过程中的动态下降是目前公认的预测HBsAg阴转的最佳指标,其他的因素如病毒基因型、治疗过程中的转氨酶升高、免疫细胞功能及细胞因子水平、宿主因素等均可以影响HBsAg阴转,现就HBsAg阴转的相关指标及潜在预测因子进行综述。

关键词：慢性乙型肝炎乙型肝炎表面抗原临床治愈预测因子

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Double Plasma Molecular Adsorption System with Sequential Low-dose Plasma Exchange in Patients with Hepatitis B Virus-related Acute-on-chronic Liver Failure:A Prospective Study

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Journal of Clinical and Translational Hepatology 2023年第4期11卷 908-917页

作者： Lu Wang Wenxiong Xu Shu Zhu Guoli Lin Jing Lai Yufeng Zhang Ying Liu Lihua Zheng Qiumin Luo zhiliang gao Chan Xie Liang Peng Second School of Clinical Medicine Binzhou Medical UniversityYantaiShandongChina Department of Infectious Diseases Third Affiliated Hospital of Sun Yat-Sen UniversityGuangzhouGuangdongChina Key Laboratory of Tropical Disease Control(Sun Yat-sen University) Ministry of EducationGuangzhouGuangdongChina

Background and Aims:To investigate the safety and efficacy of double plasma molecular adsorption system(DPMAS)with sequential low-dose plasma exchange(LPE)in treating early hepatitis B virus-related acute-on-chronic liver failure(HBV-ACLF).Methods:Clinical data of patients with HBVACLF were prospectively collected,including patients in a DPMAS with sequential LPE(DPMAS+LPE)group and those in a standard medical treatment(SMT)group.The primary endpoint was death or liver transplantation(LT)at 12 weeks of follow-up.Propensity-score matching was performed to control the effects of confounding factors on prognosis between the two groups.Results:After 2 weeks,total bilirubin,alanine aminotransferase,blood urea nitrogen levels,and Chinese Group on the Study of Severe Hepatitis B score,were significantly lower in the DPMAS+LPE group than those in the SMT group(p<0.05).After 4 weeks,laboratory parameters of the two groups were similar.The cumulative survival rate of the DPMAS+LPE group was significantly higher than that of the SMT group at 4 weeks(97.9%vs.85.4%,p=0.027),but not at 12 weeks(85.4%vs.83.3%,p=0.687).Cytokine levels were significantly lower in 12-week survival group than in the death-or-LT group(p<0.05).Functional enrichment analysis showed that downregulated cytokines were mainly involved in positive regulation of proliferation and activation of lymphocytes and monocytes,regulation of immune effect response,regulation of endotoxin response,and glial cell proliferation.Conclusion:DPMAS+LPE significantly improved the 4-week cumulative survival rate,and ameliorated the inflammatory response in patients.DPMAS+LPE may be a promising modality for patients with early HBV-ACLF.

关键词： Plasma exchange Double plasma molecular adsorption system Acute-on-chronic liver failure Prognosis

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Ensemble of single-atom catalysis and defect engineering in Cu/CeOnanozymes for tumor therapy

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Science China Chemistry 2023年

作者： Haoxin Liu zhiliang gao Han Yan Shanqing Li Weiwei Wang Xuetao Qin Hongning Sun Jiwei Cui Chunjiang Jia Key Laboratory of Colloid and Interface Chemistry Key Laboratory of Special Aggregated Materials of the Ministry of Education School of Chemistry and Chemical Engineering Shandong University School of Materials and Environmental Engineering Chizhou University

As a class of nanomaterials with natural enzyme-like characteristics, nanozymes have shown their great potential in various applications. Reducible metal oxides featured with defect structures, and single-atom catalysts with isolated metal sites are regarded as two of the most promising nanozymes. However, the strategies to construct highly performed nanozymes by combining these advantages are rarely reported. Herein, we report the coordination-unsaturated single-atomic Cu species supported on sintered CeO2, which combines the advantages of defect engineering and single-atom catalysis, exhibiting a largely enhanced peroxidase(POD)-like activity. The high-temperature calcination induces the transformation of inert Cu1O4species into coordination-unsaturated Cu1O3sites. This novel Cu1O3active sites with an unsaturated coordination work as a new type of defect sites to greatly activate the isolated Cu atoms and accelerate the dissociation of H2O2to form hydroxyl radicals(·OH). The obtained nanozyme with a high POD-like activity possesses low cytotoxicity, showing potential applications for the tumor inhibition in vitro and in vivo.

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Hsa-miR-637 inhibits human hepatocyte proliferation by targeting Med1-interacting proteins

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Liver Research 2021年第2期5卷 88-96页

作者： Jing Liu Jianyun Zhu Xiaohong Zhang Yuzhi Jia Xuejun Lee zhiliang gao Department of Infectious Diseases The Third Affiliated Hospital of Sun Yat-sen UniversityGuangzhouChina Department of Pathology Northwestern University Feinberg School of MedicineChicagoILUSA

Background:Recent studies have shown that mediator complex subunit 1(Med1)can significantly affect hepatocyte proliferation and differentiation.Acting as a tumor suppressor,microRNA-637(hsa-miR-637)can inhibit the growth of hepatocarcinoma cells and further induce cell apoptosis.However,the function of hsa-miR-637 and its target genes during liver regeneration remains to be elucidated.Methods:This study used co-immunoprecipitation(Co-IP)assay,transfection,luciferase reporter assay,functional assay by cell counting kit-8(CCK-8),Annexin V-FITC/propidium iodide apoptosis assay,and quantitative polymerase chain reaction analysis of chromatin immunoprecipitation(ChIP)for analysis.Results:Hsa-miR-637 has been suggested to suppress the expression of two Med1-interacting nuclear receptors,identified as the peroxisome proliferator-activated receptor alpha(PPARA)and thyroid hormone receptor alpha(THRA)at the transcriptional and translational levels in the human liver HL-7702 cell line.The interaction between Med1 and PPARA/THRA in HL-7702 cells was then confirmed.The transcriptional repression of hsa-miR-637 on PPARA and THRA was also demonstrated.Moreover,hsamiR-637 has been determined to suppress the proliferation of HL-7702 cells.Furthermore,cell cycle arrest of HL-7702 cells was induced by transfection of hsa-miR-637 at the S phase,but its apoptosis failed.Finally,PPARA was indicated to directly bind to the promoter of some transcription factors,like bcatenin,mouse double minute 2(MDM2),and p53.Conclusions:This study has confirmed that hsa-miR-637 plays an antiproliferative role during liver regeneration,which may contribute in understanding the regenerative process of the liver.

关键词： Liver regeneration Hsa-miR-637 Peroxisome proliferator-activated receptor alpha(PPARA) Thyroid hormone receptor alpha(THRA) Mediator complex subunit 1(Med1)

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Tunable morphologies of polymer capsules templated from cuprous oxide particles for control over cell association

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Chinese Chemical Letters 2020年第2期31卷 505-508页

作者： Hongyan Pei Yanyan Bai Jianman Guo zhiliang gao Qiong Dai Qun Yu Jiwei Cui Key Laboratory of Colloid and Interface Chemistry of the Ministry of Education School of Chemistry and Chemical EngineeringShandong UniversityJi'nan 250100China

Over the past two decades,layer-by-layer(LbL) assembly of micro/nanocapsules has been of interest for the investigation of bio-nano interactions to explore bio-applications,such as drug delivery.The choice of an appropriate template that can be easily dissolved under mild conditions is one of the challenges for the assembly of LbL capsules.Herein,we report the engineering of LbL capsules with tunable morphologies using cuprous oxide(Cu_2O) particles as templates.Cu_2O particles with cubic,tetradecahedral or spherical morphologies were synthesized via hydrothermal processes,which can be dissolved under mild condition(e.g.,sodium thiosulfate solution).The influence of capsule morphologies on cell association was investigated,which indicates that LbL capsules with cubic geometry promoted cell association up to 4 and 9-fold than tetradecahedral and spherical capsules,respectively.The reported method provides a new avenue for the assembly of LbL capsules with different morphologies,which has the potential for better understanding of biological interactions of LbL capsules.

关键词： Layer-by-layer Cuprous oxide Polymer capsules Cell association Polyphenol

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