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Exploring the Cation Regulation Mechanism for Interfacial Water Involved in the Hydrogen Evolution Reaction by In Situ Raman Spectroscopy

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Nano-Micro Letters 2024年第3期16卷 303-312页

作者： Xueqiu You Dongao zhang xia‑guang zhang xiangyu Li Jing‑Hua Tian Yao‑Hui Wang Jian‑Feng Li School of Ocean Information Engineering Fujian Provincial Key Laboratory of Oceanic Information Perception and Intelligent ProcessingJimei UniversityXiamen 361021People’s Republic of China State Key Laboratory of Physical Chemistry of Solid Surfaces MOE Key Laboratory of Spectrochemical Analysis and InstrumentationiChEMCollege of Chemistry and Chemical EngineeringCollege of MaterialsCollege of EnergyXiamen UniversityXiamen 361005People’s Republic of China Key Laboratory of Green Chemical Media and Reactions Ministry of EducationCollaborative Innovation Center of Henan Province for Green Manufacturing of Fine ChemicalsCollege of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiang 453007People’s Republic of China Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361005People’s Republic of China

Interfacial water molecules are the most important participants in the hydrogen evolution reaction(HER).Hence,understanding the behavior and role that interfacial water plays will ultimately reveal the HER mechanism.Unfortunately,investigating interfacial water is extremely challenging owing to the interference caused by bulk water molecules and complexity of the interfacial environment.Here,the behaviors of interfacial water in different cationic electrolytes on Pd surfaces were investigated by the electrochemistry,in situ core-shell nanostructure enhanced Raman spectroscopy and theoretical simulation techniques.Direct spectral evidence reveals a red shift in the frequency and a decrease in the intensity of interfacial water as the potential is shifted in the positively direction.When comparing the different cation electrolyte systems at a given potential,the frequency of the interfacial water peak increases in the specified order:Li+

关键词： In situ Raman Interfacial water Hydrogen evolution reaction Cations

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Electron transition manipulation under graphene-mediated plasmonic engineering nanostructure

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Nano Research 2023年第4期16卷 5376-5382页

作者： Huaizhou Jin Jing-Yu Wang xia-guang zhang Weiyi Lin Weiwei Cai Yue-Jiao zhang Zhi-Lin Yang Fan-Li zhang Jian-Feng Li College of Optical and Electronic Technology China Jiliang UniversityHangzhou 310018China State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringCollege of EnergySchool of Electronic Science and EngineeringDepartment of PhysicsXiamen UniversityXiamen 361005China Country Key Laboratory of Green Chemical Media and Reactions Ministry of EducationCollaborative Innovation Center of Henan Province for Green Manufacturing of Fine ChemicalsSchool of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiang 453007China

Monolayer graphene has attracted enormous attention owing to its unique electronic and optical properties.However,achieving an effective approach without applying electrical bias for manipulating the charge transfer based on graphene is elusive to date.Herein,we realized the manipulation of excitons’transition from emitter to the graphene surface with plasmonic engineering nanostructures and firstly obtained large enhancements for photon emission on the graphene surface.The localized plasmons generated from the plasmonic nanostructures of shell-isolated nanoparticle coupling to ultra-flat Au substrate would dictate a consistent junction geometry while enhancing the optical field and dominating the electron transition pathways,which may cause obvious perturbations for molecular radiation behaviors.Additionally,the three-dimensional finite-difference time-domain and time-dependent density functional theory were also carried out to simulate the distributions of electromagnetic field and energy levels of hybrid nanostructure respectively and the results agreed well with the experimental data.Therefore,this work paves a novel approach for tunning graphene charge/energy transfer processes,which may hold great potential for applications in photonic devices based on graphene.

关键词： plasmonic nanocavity shell-core isolated nanoparticles electron transition monolayer graphene fluorescence quenching

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Converting CO_(2)to ethanol on Ag nanowires with high selectivity investigated by operando Raman spectroscopy

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Science China Chemistry 2023年第1期66卷 259-265页

作者： Qiong Liu xia-guang zhang Zi-Yu Du Can-Jun Zou Huan-Yu Chen Yu Zhao Jin-Chao Dong Ping-Ping Fang Jian-Feng Li MOE Key Laboratory of Bioinorganic and Synthetic Chemistry The Key Lab of Low-carbon Chem&Energy Conservation of Guangdong ProvinceSchool of ChemistrySun Yat-sen UniversityGuangzhou 510275China State Key Laboratory of Physical Chemistry of Solid Surfaces iChEMCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China Key Laboratory of Green Chemical Media and Reactions Ministry of EducationCollaborative Innovation Center of Henan Province for Green Manufacturing of Fine ChemicalsState Key College of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiang 453007China

Electrochemical conversion of CO_(2)into liquid fuels provides an efficient way to store the renewable energy in the production of fuels and chemicals.However,effectively converting CO_(2)to ethanol remains extremely challenging due to the low activity and selectivity.Herein,we achieve a high ethanol Faradaic efficiency(FE)as high as 85%on Ag nanowires(NWs)for CO_(2)electroreduction at-0.95 V.X-ray photoelectron spectroscopy and electrochemical experiments prove that such Ag NWs are partially oxidized.Operando Raman spectroscopy finds the important CO intermediate adsorbed on partially oxidized Ag NWs,facilitating the ethanol formation.Density functional theory calculations prove that the reaction energy of CO coupling with the*CHO to*COCHO intermediate on the partially oxidized Ag NWs is smaller than that on the surface of Cu,which explains why the ethanol FE of such partially oxidized Ag NWs can exceed that of Cu,and therefore is the most favorable pathway for the formation of C_(2)products on partially oxidized Ag NWs.This study provides a new insight to design efficient catalysts and investigate the mechanisms to improve the selectivity.

关键词： surface-enhanced Raman spectroscopy CO_(2)electroreduction electrocatalysis operando spectroscopy ethanol

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Direct Z-scheme WO_(3-x) nanowire-bridged TiO_(2) nanorod arrays for highly efficient photoelectrochemical overall water splitting

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Journal of Energy Chemistry 2021年第8期30卷 721-729,I0015页

作者： Sheng Lin He Ren Zhi Wu Lan Sun xia-guang zhang Yu-Mei Lin Kelvin H.L.zhang Chang-Jian Lin Zhong-Qun Tian Jian-Feng Li State Key Laboratory of Physical Chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Shenzhen Research Institute of xiamen University Shenzhen 518000China Key Laboratory of Green Chemical Media and Reactions Ministry of EducationCollaborative Innovation Center of Henan Province for Green Manufacturing of Fine ChemicalsSchool of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiang 453007China

All-solid-state Z-scheme photocatalysts for overall water splitting to evolve H_(2) is a promising strategy for efficient conversion of solar energy.However,most of these strategies require redox mediators.Herein,a direct Z-scheme photoelectrocatalytic electrode based on a WO_(3-x)nanowire-bridged TiO_(2)nanorod array heterojunction is constructed for overall water splitting,producing H_(2).The as-prepared WO_(3-x)/TiO_(2)nanorod array heterojunction shows photoelectrochemical(PEC)overall water splitting activity evolving both H_(2) and O_(2)under UV-vis light irradiation.An optimum PEC activity was achieved over a 1.67-WO_(3-x)/TiO_(2)photoelectrode yielding maximum H_(2) and O_(2)evolution rates roughly 11 times higher than that of pure TiO_(2)nanorods without any sacrificial agent or redox mediator.The role of oxygen vacancy in WO_(3-x)in affecting the H_(2) production rate was also comprehensively studied.The superior PEC activity of the WO_(3-x)/TiO_(2)electrode for overall water splitting can be ascribed to an efficient Z-scheme charge transfer pathway between the WO_(3-x)nanowires and TiO_(2)nanorods,the presence of oxygen vacancies in WO_(3-x),and a bias potential applied on the photoelectrode,resulting in effective spatial charge separation.This study provides a novel strategy for developing highly efficient PECs for overall water splitting.

关键词： TiO_(2) nanorod arrays WO_(3-x) nanowire Heterostructure Photoelectrochemical Hydrogen production

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Diabetic retinopathy identification based on multi-sourcefree domain adaptation

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International Journal of Ophthalmology(English edition) 2024年第7期17卷 1193-1204页

作者： guang-Hua zhang guang-Ping Zhuo Zhao-xia zhang Bin Sun Wei-Hua Yang Shao-Chong zhang School of Big Data Intelligent Diagnosis&Treatment Industry Taiyuan UniversityTaiyuan 030032Shanxi ProvinceChina Shanxi Key Laboratory of Intelligent Optimization Computing and Blockchain Technology Taiyuan Normal UniversityTaiyuan 030619Shanxi ProvinceChina Shanxi Eye Hospital Taiyuan 030002Shanxi ProvinceChina College of Computer Science and Technology Taiyuan Normal UniversityTaiyuan 030619Shanxi ProvinceChina Shenzhen Eye Institute Shenzhen Eye HospitalJinan UniversityShenzhen 518040Guangdong ProvinceChina

AIM:To address the challenges of data labeling difficulties,data privacy,and necessary large amount of labeled data for deep learning methods in diabetic retinopathy(DR)identification,the aim of this study is to develop a source-free domain adaptation(SFDA)method for efficient and effective DR identification from unlabeled data.METHODS:A multi-SFDA method was proposed for DR identification.This method integrates multiple source models,which are trained from the same source domain,to generate synthetic pseudo labels for the unlabeled target domain.Besides,a softmax-consistence minimization term is utilized to minimize the intra-class distances between the source and target domains and maximize the inter-class distances.Validation is performed using three color fundus photograph datasets(APTOS2019,DDR,and EyePACS).RESULTS:The proposed model was evaluated and provided promising results with respectively 0.8917 and 0.9795 F1-scores on referable and normal/abnormal DR identification tasks.It demonstrated effective DR identification through minimizing intra-class distances and maximizing inter-class distances between source and target domains.CONCLUSION:The multi-SFDA method provides an effective approach to overcome the challenges in DR identification.The method not only addresses difficulties in data labeling and privacy issues,but also reduces the need for large amounts of labeled data required by deep learning methods,making it a practical tool for early detection and preservation of vision in diabetic patients.

关键词： diabetic retinopathy multisource-free domain adaptation pseudo-label generation softmaxconsistence minimization

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Essential Players in Cooperative Games with Graph Communication Structure

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Journal of the Operations Research Society of China 2024年第1期12卷 93-108页

作者： guang zhang Jing-Yi Ge Business School University of Shanghai for Science and TechnologyShanghai200093China

A class of cooperative games with graph communication structure is studied in this paper by considering some important players,namely essential players.Under the assumption that only connected coalitions containing essential players are able to cooperate and obtain their worths,the class of graph games with essential players is proposed as well as an allocation rule.The proposed value follows the spirit of the Myerson value defined by applying the Shapley value on a modified game.Three properties,feasible component efficiency,the inessential component property,and fairness,are provided to fully characterize this value,where feasible component efficiency and fairness follows the same ideas of component efficiency and fairness for classical graph games,and the inessential component property says that the total payoffs of the players in a non-feasible component is zero.Moreover,some computational aspects of the proposed value and comparisons with disjunctive permission value for games with permission structure are also studied,respectively.

关键词： Cooperative game Graph structure Essential player Myerson value Computation Permission structure

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B cell development and antibody responses in human immune system mice:current status and future perspective

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Science China(Life Sciences) 2024年第4期67卷 645-652页

作者： Tao zhang Wentao Liu Yong-guang Yang Key Laboratory of Organ Regeneration&Transplantation of the Ministry of Education The First Hospital of Jilin UniversityChangchun 130061China National-Local Joint Engineering Laboratory of Animal Models for Human Diseases Jilin UniversityChangchun 130061China International Center of Future Science Jilin UniversityChangchun 130061China

Humanized immune system(HIS)mice have been developed and used as a small surrogate model to study human immune function under normal or disease conditions.Although variations are found between models,most HIS mice show robust human T cell responses.However,there has been unsuccessful in constructing HIS mice that produce high-affinity human antibodies,primarily due to defects in terminal B cell differentiation,antibody affinity maturation,and development of primary follicles and germinal centers.In this review,we elaborate on the current knowledge about and previous attempts to improve human B cell development in HIS mice,and propose a potential strategy for constructing HIS mice with improved humoral immunity by transplantation of human follicular dendritic cells(FDCs)to facilitate the development of secondary follicles.

关键词： humanized immune system mouse humoral immunity germinal center B cell follicular dendritic cell

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Significant contribution of carbonyls to atmospheric oxidation capacity(AOC)during the winter haze pollution over North China Plain

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Journal of Environmental Sciences 2024年第5期139卷 377-388页

作者： Xue Yang Gen zhang guang Pan Guolan Fan Houyong zhang Xuan Ge Mingyue Du School of Municipal and Environmental Engineering Shandong Jianzhu UniversityJi’nan 250101China State Key Laboratory of Severe Weather&Key Laboratory of Atmospheric Chemistry of China Meteorological Administration Chinese Academy of Meteorological SciencesBeijing 100081China Shandong Jinan Ecological Environment Monitoring Center Ji’nan 250101China

Atmospheric carbonyl compounds play significant roles in the cycling of radicals and have exhibited surprisingly high levels in winter that were well correlated to particulate matter,for which the reason have not been clearly elucidated.Here we measured carbonyl compounds and other trace gasses together with PM_(2.5)over urban Jinan in North China Plain during the winter.Markedly higher carbonyl concentrations(average:14.63±4.21 ppbv)were found during wintertime haze pollution,about one to three-times relative to those on nonhaze days,with slight difference in chemical composition except formaldehyde(HCHO).HCHO(3.68 ppbv),acetone(3.17 ppbv),and acetaldehyde(CH_3CHO)(2.83 ppbv)were the three most abundant species,accounting for~75% of the total carbonylson both haze and non-haze days.Results from observational-based model(OBM)with atmospheric oxidation capacity(AOC)indicated that AOC significantly increased with the increasing carbonyls during the winter haze events.Carbonyl photolysis have supplied key oxidants such as RO_(2) and HO_(2),and thereby enhancing the formation of fine particles and secondary organic aerosols,elucidating the observed haze-carbonyls inter-correlation.Diurnal variation with carbonyls exhibiting peak values at early-noon and night highlighted the combined contribution of both secondary formation and primary diesel-fuel sources.1-butene was further confirmed to be the major precursor for HCHO.This study confirms the great contribution of carbonyls to AOC,and also suggests that reducing the emissions of carbonyls would be an effective way to mitigate haze pollution in urban area of the NCP region.

关键词： Carbonyls Haze Observation-based model Source apportionment Atmospheric oxidation capacity

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Conduction-convection coupled heat transfer around a hollow cylinder under different buoyancy forces

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Chinese Journal of Aeronautics 2024年第4期37卷 216-228页

作者： Wanyu zhang Jingyi WU guang YANG Institute of Refrigeration and Cryogenics Shanghai Jiao Tong UniversityShanghai 200240China

In order to clarify the effect of a buoyancy force on conduction–convection coupled heat transfer in a hollow cylinder, the flow and thermal characteristics were analyzed using an RNG k-ε turbulence model. The Reynolds number was fixed at 1.014 × 10^(6), and the Rayleigh number varied from 1.122 × 10^(10)to 1.088 × 10^(11). Results have shown that, when considering the effect of an opposed buoyancy force, increasing the Rayleigh number has a positive impact on the rate of change and uniformity of the cylinder temperature. The temperature distributions along the axial and circumferential directions are similar for different Rayleigh numbers, but extreme values differ.Along the axial direction, the maximum temperature is obtained at the interface between the variable-diameter part and the constant-diameter part. The maximum dimensionless temperature value decreases to 0.12 when the Rayleigh number increases to 1.088 × 10^(11). Along the circumferential direction, the temperature distribution is affected by the buoyancy force, which results in the temperature of the upper part being higher than that of the lower part. After nondimensionalization of the temperature and time, a correlation was proposed to illustrate the transient heat transfer process quantitatively. The standard deviation of the maximum relative temperature, representing the temperature uniformity, was also calculated. It was found that the difference in the direction of the buoyancy force made a huge difference. Compared with the opposed buoyancy force, the maximum dimensionless temperature is almost two times higher with an assisted buoyancy force. Similarly, the heat transfer coefficient with an assisted buoyancy force is half of that with an opposed buoyancy force. Overall, an assisted buoyancy force plays a negative role in terms of thermal characteristics. The flow field around the hollow cylinder was also illustrated to reveal the mechanism of the buoyancy force on magnitude and direction aspects.

关键词： Buoyancy Conduction-convection heat transfer Transient analysis Hollow cylinder Non-dimensionalization

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Hydrogel loaded with bone marrow stromal cell-derived exosomes promotes bone regeneration by inhibiting inflammatory responses and angiogenesis

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World Journal of Stem Cells 2024年第5期16卷 499-511页

作者： Shuai zhang Chuan Lu Sheng Zheng guang Hong Division for International Collaborative and Innovative Dentistry Tohoku University Graduate School of DentistrySendai 980-8575MiyagiJapan School of Stomatology Zhejiang Chinese Medical UniversityHangzhou 310053Zhejiang ProvinceChina

BACKGROUND Bone healing is a complex process involving early inflammatory immune regu-lation,angiogenesis,osteogenic differentiation,and biomineralization.Fracture repair poses challenges for orthopedic surgeons,necessitating the search for efficient healing methods.AIM To investigate the underlying mechanism by which hydrogel-loaded exosomes derived from bone marrow mesenchymal stem cells(BMSCs)facilitate the process of fracture healing.METHODS Hydrogels and loaded BMSC-derived exosome(BMSC-exo)gels were charac-terized to validate their properties.In vitro evaluations were conducted to assess the impact of hydrogels on various stages of the healing process.Hydrogels could recruit macrophages and inhibit inflammatory responses,enhance of human umbilical vein endothelial cell angiogenesis,and promote the osteogenic differen-tiation of primary cranial osteoblasts.Furthermore,the effect of hydrogel on fracture healing was confirmed using a mouse fracture model.RESULTS The hydrogel effectively attenuated the inflammatory response during the initial repair stage and subsequently facilitated vascular migration,promoted the formation of large vessels,and enabled functional vascularization during bone repair.These effects were further validated in fracture models.CONCLUSION We successfully fabricated a hydrogel loaded with BMSC-exo that modulates macrophage polarization and angiogenesis to influence bone regeneration.

关键词： Hydrogel Bone marrow mesenchymal stem cells Macrophage polarization Angiogenesis Bone regeneration

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