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Exploring the Roles of Single Atom in Hydrogen Peroxide Photosynthesis

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Nano-Micro Letters 2024年第2期16卷 32-67页

作者： Kelin He Zimo Huang chao Chen Chuntian Qiu Yu lin Zhong Qitao Zhang International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education Institute of Microscale OptoelectronicsShenzhen UniversityShenzhen 518000China Queensland Micro‑and Nanotechnology Centre School of Environment and ScienceGriffith UniversityNathanQLD 4222Australia Institute for Sustainable Transformation School of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhou 51006China ZJU‑Hangzhou Global Scientific and Technological Innovation Center Zhejiang UniversityHangzhou 311215China

This comprehensive review provides a deep exploration of the unique roles of single atom catalysts(SACs)in photocatalytic hydrogen peroxide(H_(2)O_(2))production.SACs offer multiple benefits over traditional catalysts such as improved efficiency,selectivity,and flexibility due to their distinct electronic structure and unique properties.The review discusses the critical elements in the design of SACs,including the choice of metal atom,host material,and coordination environment,and how these elements impact the catalytic activity.The role of single atoms in photocatalytic H_(2)O_(2)production is also analysed,focusing on enhancing light absorption and charge generation,improving the migration and separation of charge carriers,and lowering the energy barrier of adsorption and activation of reactants.Despite these advantages,several challenges,including H_(2)O_(2)decomposition,stability of SACs,unclear mechanism,and low selectivity,need to be overcome.Looking towards the future,the review suggests promising research directions such as direct utilization of H_(2)O_(2),high-throughput synthesis and screening,the creation of dual active sites,and employing density functional theory for investigating the mechanisms of SACs in H_(2)O_(2)photosynthesis.This review provides valuable insights into the potential of single atom catalysts for advancing the field of photocatalytic H_(2)O_(2)production.

关键词： Single atom catalysts H_(2)O_(2)photosynthesis Catalyst design and optimization

A bifunctional POM-based Cu-viologen complex with mixed octamolybdate clusters for rapid oxidation desulfurization and effective photogeneration of hydrogen

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Rare Metals 2024年第1期43卷 236-246页

作者： lin Yang Zhong Zhang chao-Nan Zhang Xiu-Li Wang College of Chemistry and Materials Engineering Bohai UniversityJinzhou 121013China Professional Technology Innovation Center of Liaoning Province for Conversion Materials of Solar Cell Bohai UniversityJinzhou 121013China

The design and synthesis of catalysts for the oxidation desulfurization and production of hydrogen are extremely important for solving environmental pollution and energy shortage.Herein,a novel bifunctional [α-Mo_(8)O_(26)]^(4-)/[β-Mo_(8)O_(26)]^(4-)-based Cu-viologen complex H_(4)[Cu_(2)~ⅠCl_(2)(Hbcbpy)_(4)] [α-Mo_(8)O_(26)] [β-Mo8O_(26)]·H_(2)O(BHU-2,Hbcbpy=1-(4-carboxybenzyl)-4,4'-bipyridinium) was synthesized and characterized by single-crystal X-ray diffraction(XRD),infrared radiation spectra,powder X-ray diffraction(PXRD) and X-ray photoelectron spectroscopy(XPS) spectra.The structural characteristic of BHU-2 is the presence of two types of octamolybdate clusters [α-Mo_(8)O_(26)]^(4-)/[β-Mo_(8)O_(26)]^(4-)and a new binuclear Cu~Ⅰ-Hbcbpy complex linked by Cl-bridges[Cu_(2)ⅠCl_(2)(Hbcbpy)_(4)]^(4+).BHU-2 as a heterogeneous catalyst exhibits excellent activities to the oxidation desulfurization and photocatalytic hydrogen production.At room temperature,BHU-2 can catalyze 96% conversion of methyl phenyl sulfide with 98% selectivity,and the process obeys the pseudo-first-order reaction kinetic with the half-life of9.6 min.The notorious 2-chloroethyl ethyl sulfide can achieve 99% conversion with 98% selectivity within only1 min at the presence of BHU-2,and the turnover frequency(TOF) is up to 7400 h^(-1).BHU-2 also exhibits high catalytic activity for the oxidation of other aromatic and aliphatic thioethers within short time at room temperature.Furthermore,BHU-2 shows a high catalytic activity for visible-light-driven hydrogen evolution with an H_(2) evolution rate of 1677.85 μmol·g^(-1)·h^(-1) within 10 h.Moreover,the catalytic activities do not decrease evidently after three cycles,revealing the prominent structural stability and recyclability.

关键词： Polyoxometalate Metal-organic complex Viologen Oxidation desulfurization Photocatalytic hydrogen production

Intake of tobacco nitrosamines of smokers in various provinces of China and their cancer risk:A meta-analysis

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Journal of Environmental Sciences 2024年第7期141卷 249-260页

作者： Xiao Li Zhiwei Ye Jun Wang Pengfei lin Xiaojin Zhang Shuguang Xie chao Chen Research Institute for Environmental Innovation(Suzhou) TsinghuaSuzhouJiangsu 215163China State Key Joint Laboratory of Environmental Simulation and Pollution Control School of EnvironmentTsinghua UniversityBeijing 100084China Shenzhen Key Laboratory of Organic Pollution Prevention and Control State Key Laboratory of Urban Water Resource and EnvironmentHarbin Institute of TechnologyShenzhen 518055China State Key Joint Laboratory of Environmental Simulation and Pollution Control College of Environmental Science and EngineeringPeking UniversityBeijing 100871China

Nitrosamines are a class of carcinogens which have been detected widely in food,water,some pharmaceuticals as well as tobacco.The objectives of this paper include reviewing the basic information on tobacco consumption and nitrosamine contents,and assessing the health risks of tobacco nitrosamines exposure to Chinese smokers.We searched the publications in English from“Web of Science”and those in Chinese from the“China National Knowledge Infrastructure”in 2022 and collected 151 literatures with valid information.The content of main nitrosamines in tobacco,including 4-(methylnitrosoamino)-1-(3-pyridyl)-1-butanone(NNK),N-nitrosonornicotine(NNN),N-nitrosoanatabine(NAT),N-nitrosoanabasine(NAB),total tobacco-specific nitrosamines(TSNA),and N-nitrosodimethylamine(NDMA)were summarized.The information of daily tobacco consumption of smokers in 30 provinces of China was also collected.Then,the intakes of NNN,NNK,NAT,NAB,TSNAs,and NDMA via tobacco smoke were estimated as 1534ng/day,591 ng/day,685 ng/day,81 ng/day,2543 ng/day,and 484 ng/day by adult smokers in30 provinces,respectively.The cancer risk(CR)values for NNN and NNK inhalation intake were further calculated as 1.44×10^(-5)and 1.95×10^(-4).The CR value for NDMA intake via tobacco smoke(inhalation:1.66×10^(-4))indicates that NDMA is similarly dangerous in tobacco smoke when compared with the TSNAs.In China,the CR values caused by average nitrosamines intake via various exposures and their order can be estimated as the following:smoke(3.75×10^(-4))>food(1.74×10^(-4))>drinking water(1.38×10^(-5)).Smokers in China averagely suffer 200%of extra cancer risk caused by nitrosamines in tobacco when compared with non-smokers.

关键词： N-nitrosamine Tobacco Cancer risk Tobacco specific nitrosamines(TSNAs) N-nitrosodimethylamine(NDMA)

linear paired electrolysis of furfural to furoic acid at both anode and cathode in a multiple redox mediated system

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Green Energy & Environment 2024年第1期9卷 104-113页

作者： Xinxin Li linchuan Cong Haibo lin Fangbing Liu Xiangxue Fu Hai-chao Xu Nan lin State Key Laboratory of Inorganic Synthesis and Preparative Chemistry Jilin UniversityChangchun 130012JilinChina State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina

Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future.Here,we report a multiple redox-mediated linear paired electrolysis system,combining the hydrogen peroxide mediated cathode process with the I2 mediated anode process,and realize the conversion of furfural to furoic acid in both side of the dividedﬂow cell simultaneously.By reasonably controlling the cathode potential,the undesired water splitting reaction and furfural reduction side reactions are avoided.Under the galvanostatic electrolysis,the two-mediated electrode processes have good compatibility,which reduce the energy consumption by about 22%while improving the electronic efﬁciency by about 125%.This system provides a green electrochemical synthesis route with commercial prospects.

关键词： Multiple redox mediated system linear paired electrolysis Furfural Furoic acid

Hemoglobin loss method calculates blood loss during pancreaticoduodenectomy and predicts bleeding-related risk factors

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World Journal of Gastrointestinal Surgery 2024年第2期16卷 419-428页

作者： chao Yu Yi-Min lin Guo-Zhe Xian Department of Hepatobiliary Surgery Shandong Provincial Hospital Affiliated to Shandong First Medical UniversityJinan 250021Shandong ProvinceChina

BACKGROUND The common clinical method to evaluate blood loss during pancreaticoduoden-ectomy(PD)is visual inspection,but most scholars believe that this method is extremely subjective and inaccurate.Currently,there is no accurate,objective me-thod to evaluate the amount of blood loss in PD patients.We retrospectively analyzed the clinical data of 341 patients who underwent PD in Shandong Provincial Hospital from March 2017 to February 2019.According to different surgical methods,they were divided into an open PD(OPD)group and a laparoscopic PD(LPD)group.The differences and correlations between the in-traoperative estimation of blood loss(IEBL)obtained by visual inspection and the intraoperative calculation of blood loss(ICBL)obtained using the Hb loss method were analyzed.ICBL,IEBL and perioperative calculation of blood loss(PCBL)were compared between the two groups,and single-factor regression analysis was performed.RESULTS There was no statistically significant difference in the preoperative general patient information between the two groups(P>0.05).PD had an ICBL of 743.2(393.0,1173.1)mL and an IEBL of 100.0(50.0,300.0)mL(P200μmol/L(95%CI:7.09-644.26;P=0.045)were independent risk factors for PCBL.The ICBLs of the LPD group and OPD group were 767.7(435.4,1249.0)mL and 663.8(347.7,1138.2)mL,respectively(P>0.05).The IEBL of the LPD group 200.0(50.0,200.0)mL was slightly greater than that of the OPD group 100.0(50.0,300.0)mL(P>0.05).PCBL was greater in the LPD group than the OPD group[1061.6(612.3,1632.3)mL vs 806.1(375.9,1347.6)mL](P<0.05).CONCLUSION The ICBL in patients who underwent PD was greater than the IEBL,but there is a certain correlation bet

关键词： Pancreaticoduodenectomy Hemoglobin loss Calculated blood loss Estimated blood loss

Tracing of Multi-Site Acetal Reactions at Metal Clusters by HR-ESI-TOF-MS

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Tracing of Multi-Site Acetal Reactions at Metal Clusters by ...

C-reactive protein to albumin ratio predict responses to programmed cell death-1 inhibitors in hepatocellular carcinoma patients

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作者：韩英姿 Jing（Jeanne） Yang Hai-Feng Su shui-chao lin Zi-chao Tang Lan-Sun Zheng State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen University

In this work, using the post-modified metal clusters as molecular reactors, the progress of aldehyde ligands with methanol molecules forming hemiacetals and acetals under the catalysis of concentrated sulfuric acids was precisely traced with high resolution ESI-TOF Mass Spectrometry（HR-ESI-TOF-MS）. It is indicated that as an effective tool to track chemical reactions, mass spectroscopy could provide some instructions in the designing of molecular reactors, and shows the ability to study the chemical reaction mechanisms.

关键词： hemiacetal acetal metal cluster reaction mass spectrometry

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World Journal of Gastrointestinal Oncology 2024年第1期16卷 61-78页

作者： Bai-Bei Li Lei-Jie Chen Shi-Liu Lu Biao Lei Gui-lin Yu shui-Ping Yu Department of Hepatobiliary Surgery The First Affiliated Hospital of Guangxi Medical UniversityNanning 530021Guangxi Zhuang Autonomous RegionChina Key Laboratory of Early Prevention and Treatment for Regional High Frequency Tumor(Guangxi Medical University) Ministry of EducationNanning 530021Guangxi Zhuang Autonomous RegionChina Guangxi Key Laboratory of Immunology and Metabolism for Liver Diseases Guangxi Medical UniversityNanning 530021Guangxi Zhuang Autonomous RegionChina Department of Gastroenterology The Second Xiangya Hospital of Central South UniversityNanning 410011Guangxi Zhuang Autonomous RegionChina Department of Emergency The First Affiliated Hospital of Guangxi Medical UniversityNanning 530021Guangxi Zhuang Autonomous RegionChina

BACKGROUND Over the years,programmed cell death-1(PD-1)inhibitors have been routinely used for hepatocellular carcinoma(HCC)treatment and yielded improved survival outcomes.Nonetheless,significant heterogeneity surrounds the outcomes of most studies.Therefore,it is critical to search for biomarkers that predict the efficacy of PD-1 inhibitors in patients with HCC.AIM To investigate the role of the C-reactive protein to albumin ratio(CAR)in evaluating the efficacy of PD-1 inhibitors for HCC.METHODS The clinical data of 160 patients with HCC treated with PD-1 inhibitors from January 2018 to November 2022 at the First Affiliated Hospital of Guangxi Medical University were retrospectively analyzed.RESULTS The optimal cut-off value for CAR based on progression-free survival(PFS)was determined to be 1.20 using x-tile software.Cox proportional risk model was used to determine the factors affecting prognosis.Eastern Cooperative Oncology Group performance status[hazard ratio(HR)=1.754,95%confidence interval(95%CI)=1.045-2.944,P=0.033],CAR(HR=2.118,95%CI=1.057-4.243,P=0.034)and tumor number(HR=2.932,95%CI=1.246-6.897,P=0.014)were independent prognostic factors for overall survival.CAR(HR=2.730,95%CI=1.502-4.961,P=0.001),tumor number(HR=1.584,95%CI=1.003-2.500,P=0.048)and neutrophil to lymphocyte ratio(HR=1.120,95%CI=1.022-1.228,P=0.015)were independent prognostic factors for PFS.Two nomograms were constructed based on independent prognostic factors.The C-index index and calibration plots confirmed that the nomogram is a reliable risk prediction tool.The ROC curve and decision curve analysis confirmed that the nomogram has a good predictive effect as well as a net clinical benefit.CONCLUSION Overall,we reveal that the CAR is a potential predictor of short-and long-term prognosis in patients with HCC treated with PD-1 inhibitors.If further verified,CAR-based nomogram may increase the number of markers that predict individualized prognosis.

关键词： C-reactive protein to albumin ratio Hepatocellular carcinoma Programmed cell death-1 inhibitors Prognosis Nomogram

Association of daily sitting time and leisure-time physical activity with body fat among U.S.adults

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Journal of Sport and Health Science 2024年第2期13卷 195-203页

作者： Jingwen Liao Min Hu Kellie Imm Clifton J.Holmes Jie Zhu chao Cao lin Yang Guangdong Provincial Key Laboratory of Physical Activity and Health Promotion Guangzhou Sport UniversityGuangzhou 510500China Scientific Research Center Guangzhou Sport UniversityGuangzhou 510500China Division of Epidemiology&Genetics Department of Population and Public Health SciencesKeck School of Medicine of the University of Southern CaliforniaLos AngelesCA 90033USA Program in Physical Therapy Washington University School of MedicineSt.LouisMO 63110USA Center for Human Nutrition Washington University School of MedicineSt.LouisMO 63110USA Department of Plastic and Reconstructive Surgery Shanghai East HospitalTongji UniversityShanghai 200070China Department of Cancer Epidemiology and Prevention Research Alberta Health ServicesCalgary T2S 3C3Canada Department of Oncology and Community Health Sciences University of CalgaryCalgary T2N 1N4Canada

Background:Prolonged sitting and reduced physical activity lead to low energy expenditures.However,little is known about the joint impact of daily sitting time and physical activity on body fat distribution.We investigated the independent and joint associations of daily sitting time and physical activity with body fat among adults.Methods:This was a cross-sectional analysis of U.S.nationally representative data from the National Health and Nutrition Examination Survey2011-2018 among adults aged 20 years or older.Daily sitting time and leisure-time physical activity(LTPA)were self-reported using the Global Physical Activity Questionnaire.Body fat(total and trunk fat percentage)was determined via dual X-ray absorptiometry.Results:Among 10,808 adults,about 54.6%spent 6 h/day or more sitting;more than one-half reported no LTPA(inactive)or less than 150 min/week LTPA(insufficiently active)with only 43.3%reported 150 min/week or more LTPA(active)in the past week.After fully adjusting for sociodemographic data,lifestyle behaviors,and chronic conditions,prolonged sitting time and low levels of LTPA were associated with higher total and trunk fat percentages in both sexes.When stratifying by LTPA,the association between daily sitting time and body fat appeared to be stronger in those who were inactive/insuufficiently active.In the joint analyses,inactive/insuufficiently active adults who reported sitting more than 8 h/day had the highest total(female:3.99%(95%confidence interval(95%CI):3.09%-4.88%);male:3.79%(95%CI:2.75%-4.82%))and trunk body fat percentages(female:4.21%(95%CI:3.09%-5.32%);male:4.07%(95%CI:2.95%-5.19%))when compared with those who were active and sitting less than 4 h/day.Conclusion:Prolonged daily sitting time was associated with increased body fat among U.S.adults.The higher body fat associated with 6 h/day sitting may not be offset by achieving recommended levels of physical activity.

关键词： Adults Body fat distribution Physical activity Sitting time

Efficient removal of natural organo-chromium(Ⅲ)through selfcirculating decomplex and immobilization with nanoscale zerovalent iron

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Nano Research 2024年第1期17卷 364-371页

作者： Zhicheng Dong Yunyun Xu Can Wu Jin chao Chen Tian Zhang lin School of Metallurgy and Environment Central South UniversityChangsha 410083China Chinese National Engineering Research Center for Control&Treatment of Heavy Metal Pollution Changsha 410083China College of Ecology and Environment Chengdu University of TechnologyChengdu 610059China School of Environment and Energy The Key Laboratory of Pollution Control and Ecosystem Restoration in Industry Clusters(Ministry of Education)South China University of TechnologyGuangzhou 510006China

Organo-chromium(III)complex is one of the chromium contaminant species,which would transform to high-toxic Cr(VI)during migrating in the environment.Such natural organo-chromium(III)(NOCr)is difficult to remove by traditional degradation or precipitation methods,due to its high stability and solubility.Herein,we demonstrated a novel NOCr removing method by transforming it to certain structures similar to Cr-Fe minerals in nature,through a self-circulating decomplex and immobilization mechanism with nano zero-valent iron(nZVI).Taking chromium glycinate(Cr-Gly)as a probe,nZVI showed a high Cr removal efficiency of 99.4%under ambient conditions.The removal process included three stages of adsorption,decomplexation,and re-immobilization.Cr-Gly was first adsorbed on the surface of nZVI by chemisorption of the oxide shell.Then,the adsorbed Cr-Gly was decomplexed and oxidized to Cr(VI)by·OH and 1O_(2),which were generated from molecular oxygen activated by nZVI.Meanwhile,the released Cr(VI)could be in-situ adsorbed and re-reduced to Cr(III),which was further immobilized in form of Cr-O-Fe complex.As the Cr-O-Fe complexing structure was similar to that of Cr-Fe minerals(such as chromohercynite)in nature,this work explored a novel and efficient NOCr removing method that was potential to weaken chromium pollution in the environment.

关键词： organo-chromium(III) zero-valent iron adsorption decomplexation Cr immobilization