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Atomically dispersed Mn-Nx catalysts derived from Mn-hexamine coordination frameworks for oxygen reduction reaction

Carbon Energy 2024年第5期6卷 114-126页

作者： Guoyu Zhong Liuyong Zou Xiao Chi Zhen Meng Zehong Chen Tingzhen Li yongfa huang Xiaobo Fu Wenbo Liao Shaona Zheng Yongjun Xu Feng Peng Xinwen Peng Guangdong Provincial Key Laboratory of Distributed Energy Systems School of Chemical Engineering and Energy TechnologyDongguan University of TechnologyDongguanChina State Key Laboratory of Pulp and Paper Engineering South China University of TechnologyGuangzhouChina Department of Chemistry Centre for Advanced 2D Materials(CA2DM)National University of SingaporeSingaporeSingapore School of Chemistry and Chemical Engineering Guangzhou UniversityGuangzhouChina

Metal-organic frameworks recently have been burgeoning and used as precursors to obtain various metal-nitrogen-carbon catalysts for oxygen reduction reaction(ORR).Although rarely studied,Mn-N-C is a promising catalyst for ORR due to its weak Fenton reaction activity and strong graphitization catalysis.Here,we developed a facile strategy for anchoring the atomically dispersed nitrogen-coordinated single Mn sites on carbon nanosheets(MnNCS)from an Mn-hexamine coordination framework.The atomically dispersed Mn-N4 sites were dispersed on ultrathin carbon nanosheets with a hierarchically porous structure.The optimized MnNCS displayed an excellent ORR performance in half-cells(0.89 V vs.reversible hydrogen electrode(RHE)in base and 0.76 V vs.RHE in acid in half-wave potential)and Zn-air batteries(233 mW cm^(−2)in peak power density),along with significantly enhanced stability.Density functional theory calculations further corroborated that the Mn-N4-C1_(2)site has favorable adsorption of*OH as the rate-determining step.These findings demonstrate that the metal-hexamine coordination framework can be used as a model system for the rational design of highly active atomic metal catalysts for energy applications.

关键词： carbon nanosheets electrocatalyst metal-organic frameworks Mn-N4 oxygen reduction reaction Zn-air batteries

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Cellulose nanofiber-derived carbon aerogel for advanced room-temperature sodium–sulfur batteries

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Carbon Energy 2023年第1期5卷 1-15页

作者： Wu Yang Wang Yang Ren Zou yongfa huang Haihong Lai Zehong Chen Xinwen Peng State Key Laboratory of Pulp and Paper Engineering South China University of TechnologyGuangzhouChina

Room-temperature sodium–sulfur(RT/Na–S)batteries are regarded as promising large-scale stationary energy storage systems owing to their high energy density and low cost as well as the earth-abundant reserves of sodium and sulfur.However,the diffusion of polysulfides and sluggish kinetics of conversion reactions are still major challenges for their application.Herein,we developed a powerful and functional separator to inhibit the shuttle effect by coating a lightweight three-dimensional cellulose nanofiber-derived carbon aerogel on a glass fiber separator(denoted NSCA@GF).The hierarchical porous structures,favorable electronic conductivity,and three-dimensional interconnected network of N,S-codoped carbon aerogel endow a multifunctional separator with strong polysulfide anchoring capability and fast reaction kinetics of polysulfide conversion,which can act as the barrier layer and an expanded current collector to increase sulfur utilization.Moreover,the hetero-doped N/S sites are believed to strengthen polysulfide anchoring capability via chemisorption and accelerate the redox kinetics of polysulfide conversion,which is confirmed from experimental and theoretical results.As a result,the assembled Na–S coin cells with the NSCA@GF separator showed a high reversible capacity(788.8 mAh g^(−1) at 0.1 C after 100 cycles)and superior cycling stability(only 0.059%capacity decay per cycle over 1000 cycles at 1 C),thereby demonstrating the significant potential for application in high-performance RT/Na–S batteries.

关键词： carbon aerogel cellulose nanofiber N,S codoping redox kinetics sodium–sulfur batteries

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Hydrogen bond-bridged phosphorene flexible film for photodynamic inhibiting Staphylococcus aureus

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Nano Research 2024年第6期17卷 5461-5468页

作者： Ziyu Wei Wenting Li Zhifang Liu yongfa Zhu Huaqiang Cao Department of Chemistry Engineering Research Center of Advanced Rare Earth MaterialsTsinghua UniversityBeijing 100084China

Antibiotics are a widely used and effective treatment for bacterial infections.However,bacteria can gradually evolve during infection,leading to developing resistance to antibiotics,which renders previously effective treatments ineffective.Finding a useful and convenient manner to treat bacterial infections is a great challenge.Here,we report a flexible hydrogen-bond-bridged phosphorene film with photodynamic antibacterial properties and excellent mechanical properties,fabricated from electrochemical exfoliation of black phosphorus(BP).When illuminated under 700 nm light,the hydrogen bond-bridged phosphorene flexible film is capable of converting ground-state triplet oxygen(O_(2))into excited-state singlet oxygen(^(1)O_(2)),destroying the structure of the membrane of Staphylococcus aureus,and eventually leading to bacterial death,via breaking the C=C of unsaturated fatty acids within the bacterial cell membrane after the reaction between^(1)O_(2)and unsaturated fatty acids,thus realizing a highly efficient antibacterial approach,which is supported by gas chromatography-mass spectrometry(GC-MS)technique.This work establishes an effective phototherapy platform for treating bacterial traumatic infections.

关键词： hydrogen bond-bridged phosphorene flexible film photodynamic Staphylococcus aureus

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Regulating the crystal phase of bismuth-based semiconductors for promoted photocatalytic performance

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Science China Chemistry 2024年第6期67卷 1839-1864页

作者： Zhaohui Wu Mei-Chi Chong Shiying Zhang Junshan Li yongfa Zhu Hunan Key Laboratory of Applied Environmental Photocatalysis Changsha UniversityChangsha410022China Department of Chemistry Tsinghua UniversityBeijing100084China Institute for Advanced Study Chengdu UniversityChengdu610106China

Numerous bismuth-based semiconductors(BBSs)with sophisticated and desirable structures used as photocatalysts for efficient photocatalytic degradation of water organic contaminants have attracted considerable attention.However,regulating the crystal phases and phase transition of BBSs for promoted photocatalytic performance is ignored.Herein,the unique crystal structure and band structure features of each typical BBSs,and the vital roles on phase controlling of each phase were systematically presented based on the classification of BBSs.Notably,the critical factors for the phase transition of BBSs and intrinsic driving forces endowed by phases of BBSs for enhanced photocatalytic performance of organic contaminants removal were also elucidated.This review will provide systematical guidelines and horizons for regulating the crystal phase and phase transition of BBSs,promoting photocatalytic degradation and mineralization of organic contaminants.

关键词： bismuth-based semiconductors phase regulation photocatalytic performances organic contaminants

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Single-cell transcriptional profile of ACE2 in healthy and failing human hearts

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Science China(Life Sciences) 2021年第4期64卷 652-655页

作者： Yitian Zhou yongfa huang Xiaomin Song Xiaoxiao Guo Junling Pang Jing Wang Shuyang Zhang Chen Wang State Key Laboratory of Medical Molecular Biology.Institute of Basic Medical Sciences Chinese Academy of Medical SciencesDeparment of Pathophysiology.Peking Union Medical CollegeBejing 100730China Deparment of Cardiology Peking Union Medlical College HospialPeking Union Medical College and Chinese Academy of Medical SciencesBejing 100730China Slate Key Laboratory of Medical Molecular Biology Institute of Basic Medical SciencesChinese Academy of Medical SciencesDepartment of PlhysiologPeking Union Medical CollegeBeijing 100730China

Dear Editor,The coronavirus disease 2019(COVID-19)pandemic,which is caused by SARS-Co V-2,has gained serious attention from medical practitioners around the world in the past few months.Approximately 20%of critically ill COVID-19 patients were reported to have suffered myocardial injury.The specific mechanism of this pathology requires further investigation(Yang et al.,2020).

关键词： ACE2 al. pathology

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A theoretical study on gaseous pollutant flushing of natural ventilation driven by buoyancy forces in industrial buildings

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Building Simulation 2024年第4期17卷 575-589页

作者： Jiawei Zhuang Genyang Chen Rumeng Yang Kun Han Dongdong Tian yongfa Diao Henggen Shen School of Urban Construction Changzhou UniversityChangzhou213164China School of Petroleum and Natural Gas Engineering School of EnergyChangzhou UniversityChangzhou213164China College of Environmental Science and Engineering Donghua UniversityShanghai201620China School of Architecture and Urban Planning Nanjing UniversityNanjing210093China

The acceleration of industrialization worsening indoor environments of industrial buildings has drawn more attention in recent years.Natural ventilation can improve indoor air quality(IAQ)and reduce carbon emissions.To evaluate gaseous pollutant levels in industrial buildings for the development of buoyancy-driven natural ventilation,two theoretical models of pollutant flushing(Model I and Model II)are developed based on the existing thermal stratification theory in combination with the mixing characteristics of lower pollutant.The results show that indoor pollutant flushing is mainly dependent on the pollution source intensity and effective ventilation area.The mixing characteristics of lower pollutant has an important effect on pollutant stratification and evolution during ventilation,but it does not change the prediction results at steady state.When the dimensionless pollution source intensity is larger than 1,the pollution source should be cleaned up or other ventilation methods should be used instead to improve IAQ.In addition,the comparisons between Model I and Model II on instantaneous pollutant concentration are significantly influenced by the pollution source intensity,and the actual pollutant concentration is more likely to be between the predicted values of Model I and Model II.To reduce pollutant concentration to a required level,the pollution source intensity should be in a certain range.The theoretical models as well as the necessary conditions for ventilation effectiveness obtained can be used for the ventilation optimization design of industrial buildings.

关键词： industrial buildings buoyancy-driven natural ventilation gaseous pollutants evolution model pollution sources

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SARS-CoV-2 leads to myocardial injury in rhesus macaque

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Signal Transduction and Targeted Therapy 2021年第10期6卷 2957-2959页

作者： Yufan Feng Xiaomin Song yongfa huang Wei Deng Man Li Xiaoxiao Guo Chuan Qin Wei-Min Tong Jiangning Liu Jing Wang Institute of Basic Medical Sciences Chinese Academy of Medical SciencesSchool of Basic Medicine Peking Union Medical CollegeBeijingChina Department of Cardiology Peking Union Medical College HospitalPeking Union Medical College and Chinese Academy of Medical SciencesBeijingChina NHC Key Laboratory of Human Disease Comparative Medicine Beijing Key Laboratory for Animal Models of Emerging and Remerging Infectious DiseasesInstitute of Laboratory Animal ScienceChinese Academy of Medical Sciences and Comparative Medicine CenterPeking Union Medical CollegeBeijingChina Department of Pathology Beijing Ditan HospitalCapital Medical UniversityBeijingChina Department of Pathology Institute of Basic Medical SciencesChinese Academy of Medical Sciences and Peking Union Medical CollegeMolecular Pathology Research CenterChinese Academy of Medical SciencesBeijingChina

Dear Editor,Coronavirus disease 2019(COVID-19)is caused by severe acute respiratory syndrome coronavirus 2(SARS-CoV-2)infection,which induces multiple cardiovascular complications including acute myocardial injury resulting from acute coronary syndrome,myocarditis,stress-cardiomyopathy,arrhythmias,cardiogenic shock,and cardiac arrest.The incidence of myocardial injury in COVID-19 patients was up to 20%or higher in the subpopulation with existing cardiovascular diseases,accounting for 69.4%of mortality.1 Although the presence of angiotensin-converting enzyme 2(ACE2)in cardiomyocytes could result in viral myocarditis in COVID-19 patients,the cardiopathology involved in COVID-19 is still unclear.

关键词： acute cardiovascular myocardial

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Unraveling the role of iron on Ni-Fe alloy nanoparticles during the electrocatalytic ethanol-to-acetate process

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Nano Research 2024年第4期17卷 2328-2336页

作者： Junshan Li Luming Li Xinyu Ma Jun Wang Jun Zhao Yu Zhang Ren He Yaoyue Yang Andreu Cabot yongfa Zhu Institute for Advanced Study Chengdu University610106 ChengduChina State Key Laboratory of Environmental-Friendly Energy Materials Southwest University of Science and TechnologyMianyang 621010China College of Food and Biological Engineering Chengdu UniversityChengdu 610106China School of Chemistry and Environment Southwest Minzu UniversityChengdu 610041China Hebei Key Laboratory of Photoelectric Control on Surface and Interface College of ScienceHebei University of Science and TechnologyShijiazhuang 050018China Catalonia Institute for Energy Research-IREC Sant Adriàde BesòsBarcelona 08930CataloniaSpain ICREA Pg.Lluís Companys 23Barcelona 08010CataloniaSpain Department of Chemistry Tsinghua UniversityBeijing 100084China

The anodic electrooxidation of ethanol to value-added acetate is an excellent example of replacing the oxygen evolution reaction to promote the cathodic hydrogen evolution reaction and save energy.Herein,we present a colloidal strategy to produce Ni-Fe bimetallic alloy nanoparticles(NPs)as efficient electrocatalysts for the electrooxidation of ethanol in alkaline media.Ni-Fe alloy NPs deliver a current density of 100 mA·cm^(-2) in a 1.0 M KOH solution containing 1.0 M ethanol merely at 1.5 V vs.reversible hydrogen electrode(RHE),well above the performance of other electrocatalysts in a similar system.Within continuous 10 h testing at this external potential,this electrode is able to produce an average of 0.49 mmol·cm^(-2)·h^(-1) of acetate with an ethanol-to-acetate Faradaic efficiency of 80%.A series of spectroscopy techniques are used to probe the electrocatalytic process and analyze the electrolyte.Additionally,density functional theory(DFT)calculations demonstrate that the iron in the alloy NPs significantly enhances the electroconductivity and electron transfer,shifts the rate-limiting step,and lowers the energy barrier during the ethanol-to-acetate reaction pathway.

关键词： electrocatalysis ethanol oxidation reaction alloy nanoparticle acetate biorefinery

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Efficient ammonia production over e_(g)-occupancy-optimized perovskite electrocatalysts

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Nano Research 2024年第6期17卷 4682-4686页

作者： Mingfa Chen Yu Zhang Fulong Liu Zhenbao Zhang Yuming Dong yongfa Zhu Heqing Jiang Jiawei Zhu Key Laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi 214122China Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266101China School of Chemistry and Chemical Engineering Linyi UniversityLinyi 276005China Department of Chemistry Tsinghua UniversityBeijing 100084China

Renewable-energy-driven nitrate(NO_(3)^(−))electroreduction to ammonia(NH_(3))(NERA)has been an attractive technology for decarbonizing NH_(3)production and wastewater treatment.Improving NERA efficiency requires electrocatalysts that are earth-abundant and show fantastic performance.Here we report a semiempirical activity descriptor of eg occupancy(of surface B-site cations)for identifying inexpensive perovskite oxides with extremely high efficacy toward NERA.We establish the descriptor by systematic investigations of more than 10 perovskite oxides.These investigations demonstrate that their intrinsic NERA activities display a volcano-shaped dependence on eg occupancy and the optimized intrinsic activities are accessible at near-1 eg occupancies.This could plausibly be attributed to the favorable overlaps between surface adsorbates and vertically-oriented eg orbitals.More importantly,utilizing this descriptor,we predict a highly active,selective,and durable NERA electrocatalyst with a composition of Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3−δ)(BSCF).Because of its close-to-1 e_(g)occupancy(i.e.~1.2),the BSCF features a superior NH_(3)production rate of 0.12 g·h^(−1)·mg_(cat.)^(−1)(Faradaic efficiency of 97.8%)that is at top of the volcano plot,and substantially outperforms most NERA electrocatalysts reported in literature.

关键词： perovskite oxide nitrate electroreduction ammonia electrosynthesis eg occupancy

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Associations of daily sedentary behavior,physical activity,and sleep with irritable bowel syndrome:A prospective analysis of 362,193 participants

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Journal of Sport and Health Science 2024年第1期13卷 72-80页

作者： Xu Gao Sifan Tian Ninghao huang Gang Sun Tao huang Department of Occupational and Environmental Health Sciences School of Public HealthPeking UniversityBeijing 100191China Department of Epidemiology and Biostatistics School of Public HealthPeking UniversityBeijing 100191China Department of Gastroenterology and Hepatology First Medical Center of People's Liberation Army General HospitalBeijing 100853China

Background:Irritable bowel syndrome(IBS)substantially affects quality of life and requires early prevention.This study aimed to elucidate the relationships between IBS and daily behaviors,including sedentary behavior(SB),physical activity(PA),and sleep.In particular,it seeks to identify healthy behaviors to reduce IBS risk,which previous studies have rarely addressed.Methods:Daily behaviors were retrieved from self-reported data of 362,193 eligible UK Biobank participants.Incident cases were determined by self-report or health care data according to RomeⅣcriteria.Results:A total of 345,388 participants were IBS-free at baseline,during a median follow-up of 8.45 years,19,885 incident IBS cases were recorded.When examined individually,SB and shorter(≤7 h/day)or longer(>7 h/day)sleep duration were each positively associated with increased IBS risk,and PA was associated with lower IBS risk.The isotemporal substitution model suggested that replacing SB with other activities could provide further protective effects against IBS risk.Among people sleeping≤7 h/day,replacing 1 h of SB with equivalent light PA,vigorous PA,or sleep was associated with 8.1%(95%confidence interval(95%CI):0.901-0.937),5.8%(95%CI:0.896-0.991),and 9.2%(95%CI:0.885-0.932)reduced IBS risk,respectively.For people sleeping>7 h/day,light and vigorous PA were associated with a 4.8%(95%CI:0.926-0.978)and a 12.0%(95%CI:0.815-0.949)lower IBS risk,respectively.These benefits were mostly independent of genetic risk for IBS.Conclusion:SB and unhealthy sleep duration are risk factors for IBS.A promising way to mitigate IBS risk for individuals sleeping≤7 h/day and for those sleeping>7 h/day appears to be by replacing SB with adequate sleep or vigorous PA,respectively,regardless of the genetic predisposition of IBS.

关键词： Irritable bowel syndrome Isotemporal substitution model Physical activity Sedentary behavior Sleep

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