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Mechanisms of isomerization and hydration reactions of typicalβ-diketone at the air-droplet interface

Journal of Environmental Sciences 2024年第7期141卷 225-234页

作者： Yuemeng Ji Weiyong Luo Qiuju Shi xiaohui ma Ziqi Wu Weina Zhang Yanpeng Gao Taicheng An Guangdong-Hong Kong-macao Joint Laboratory for Contaminants Exposure and Health Guangdong Key Laboratory of Environmental Catalysis and Health Risk ControlInstitute Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China Guangzhou Key Laboratory of Environmental Catalysis and Pollution Control Key Laboratory for City Cluster Environmental Safety and Green Development of the Ministry of EducationSchool of Environmental Science and EngineeringGuangdong University of TechnologyGuangzhou 510006China

Acetylacetone(AcAc)is a typical class ofβ-diketones with broad industrial applications due to the property of the keto-enol isomers,but its isomerization and chemical reactions at the air-droplet interface are still unclear.Hence,using combined molecular dynamics and quantum chemistry methods,the heterogeneous chemistry of AcAc at the air-droplet interface was investigated,including the attraction of AcAc isomers by the droplets,the distribution of isomers at the air-droplet interface,and the hydration reactions of isomers at the air-droplet interface.The results reveal that the preferential orientation of two AcAc isomers(keto-and enol-AcAc)to accumulate and accommodate at the acidic air-droplet interface.The isomerization of two AcAc isomers at the acidic air-droplet interface is more favorable than that at the neutral air-droplet interface because the“water bridge”structure is destroyed by H_(3)O^(+),especially for the isomerization from keto-Ac Ac to enol-AcAc.At the acidic air-droplet interface,the carbonyl or hydroxyl O-atoms of two AcAc isomers display an energetical preference to hydration.Keto-diol is the dominant products to accumulate at the air-droplet interface,and excessive keto-diol can enter the droplet interior to engage in the oligomerization.The photooxidation reaction of AcAc will increase the acidity of the air-droplet interface,which indirectly facilitate the uptake and formation of more keto-diol.Our results provide an insight into the heterogeneous chemistry ofβ-diketones and their influence on the environment.

关键词： Acetylacetone Air-droplet interface Theoretical simulation Isomerization Hydration reaction mechanism

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Stretchable,breathable,and washable epidermal electrodes based on microfoam reinforced ultrathin conductive nanocomposites

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Nano Research 2023年第7期16卷 10412-10419页

作者： Tao ma Yong Lin xiaohui ma Jiaxue Zhang Dongchan Li Desheng Kong School of Chemical Engineering and Technology Hebei University of TechnologyTianjin 300130China College of Engineering and Applied Sciences State Key Laboratory of Analytical Chemistry for Life Scienceand Jiangsu Key Laboratory of Artificial Functional MaterialsNanjing UniversityNanjing 210046China

Stretchable epidermal electronics allow conformal interactions with the human body for emerging applications in wearable health monitoring and therapy.Stretchable devices are commonly constructed on submillimeter-thick elastomer substrates with limited moisture permeability,thereby leading to unpleasant sensations during long-term attachment.Although the ultrathin elastomer membrane may address this problem,the mechanical robustness is essentially lost for direct manipulations and repetitive uses.Here,we report a stretchable,breathable,and washable epidermal electrode of microfoam reinforced ultrathin conductive nanocomposite(MRUCN).The new architecture involves ultrathin conductive silver nanowire nanocomposite features supported on a porous elastomeric microfoam substrate,which exhibits high moisture permeability for pleasant perceptions during epidermal applications.As-prepared epidermal electrodes show excellent electronic conductivity(8440 S·cm^(-1)),high feature resolution(~50μm),decent stretchability,and excellent durability.In addition,the MRUCN retains stable electrical properties during washing to meet the hygiene requirements for repetitive uses.The successful implementation in an integrated electronic patch demonstrates the practical suitability of MRUCN for a broad range of epidermal electronic devices and systems.

关键词： stretchable conductor epidermal electronics breathable conductor epidermal electrode

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Competing esterification and oligomerization reactions of typical long-chain alcohols to secondary organic aerosol formation

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Journal of Environmental Sciences 2023年第4期126卷 103-112页

作者： Jiaxin Wang xiaohui ma Yuemeng Ji Yongpeng Ji Yanpeng Gao Yuqi Xiao Guiying Li Taicheng An Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control Guangdong-Hong Kong-Macao Joint Laboratory for Contaminants Exposure and HealthInstitute of Environmental Health and Pollution controlGuangdong University of TechnologyGuangzhou 510006China Guangzhou Key Laboratory of Environmental Catalysis and Pollution Control Key Laboratory of City Cluster Environmental Safety and Green DevelopmentSchool of Environmental Science and EngineeringGuangdong University of TechnologyGuangzhou 510006China

Organosulfate (OSA) nanoparticles,as secondary organic aerosol (SOA) compositions,are ubiquitous in urban and rural environments.Hence,we systemically investigated the mechanisms and kinetics of aqueous-phase reactions of 1-butanol/1-decanol (BOL/DOL) and their roles in the formation of OSA nanoparticles by using quantum chemical and kinetic calculations.The mechanism results show that the aqueous-phase reactions of BOL/DOL start from initial protonation at alcoholic OH^(-)groups to form carbenium ions (CBs),which engage in the subsequent esterification or oligomerization reactions to form OSAs/organosulfites (OSIs) or dimers.The kinetic results reveal that dehydration to form CBs for BOL and DOL reaction systems is the rate-limiting step.Subsequently,about 18%of CBs occur via oligomerization to dimers,which are difficult to further oligomerize because all reactive sites are occupied.The rate constant of BOL reaction system is one order of magnitude larger than that of DOL reaction system,implying that relative short-chain alcohols are more prone to contribute OSAs/OSIs than long-chain alcohols.Our results reveal that typical long-chain alcohols contribute SOA formation via esterification rather than oligomerization because OSA/OSI produced by esterification engages in nanoparticle growth through enhancing hygroscopicity.

关键词： Long-chain alcohols Organosulfates Aqueous phase reaction Reaction mechanisms Secondary organic aerosol

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Radiomic-based machine learning model for predicting the surgical risk in children with abdominal neuroblastoma

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World Journal of Pediatric Surgery 2023年第3期6卷 188-195页

作者： Xuan Jia Jiawei Liang xiaohui ma Wenqi Wang Can Lai Department of Radiology Children's HospitalZhejiang University School of MedicineHangzhouChina

Background Preoperative imaging assessment of surgical risk is very important for the prognosis of these children.To develop and validate a radiomics-based machine learning model based on the analysis of radiomics features to predict surgical risk in children with abdominal neuroblastoma(NB).Methods A retrospective study was conducted from April 2019 to march 2021 among 74 children with abdominal NB.A total of 1874 radiomic features in MR images were extracted from each patient.Support vector machines(SVMs)were used to establish the model.Eighty percent of the data were used as the training set to optimize the model,and 20%of the data were used to validate its accuracy,sensitivity,specificity and area under the curve(AUC)to verify its effectiveness.Results Among the 74 children with abdominal NB,55(65%)had surgical risk and 19(35%)had no surgical risk.A t test and Lasso identified that 28 radiomic features were associated with surgical risk.After developing an SVMbased model using these features,predictions were made about whether children with abdominal NB had surgical risk.The model achieved an AUC of 0.94(a sensitivity of 0.83 and a specificity of 0.80)with 0.890 accuracy in the training set and an AUC of 0.81(a sensitivity of 0.73 and a specificity of 0.82)with 0.838 accuracy in the test set.Conclusions Radiomics and machine learning can be used to predict the surgical risk in children with abdominal NB.The model based on 28 radiomic features established by SVM showed good diagnostic efficiency.

关键词： surgical specificity neuroblastoma

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Preparation of Y^(3+)-doped Bi-_(2)MoO_(6) nanosheets for improved visible-light photocatalytic activity: Increased specific surface area, oxygen vacancy formation and efficient carrier separation

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International Journal of Minerals,Metallurgy and materials 2023年第9期30卷 1824-1834页

作者： Hong Qiu Shujing Liu xiaohui ma Yajie Li Yueyan Fan Wenjun Li Hualei Zhou Department of Chemistry and Chemical Engineering School of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China College of Applied Science and Technology Beijing Union UniversityBeijing 100012China BGRIMM MTC Technology Co. Ltd.Beijing 102680China

Although Bi_(2)Mo O_(6)(BMO) has recently received extensive attention, its visible-light photocatalytic activity remains poor due to its limited photoresponse range and low charge separation efficiency. In this work, a series of visible-light-driven Y^(3+)-doped BMO(Y-BMO) photocatalysts were synthesized via a hydrothermal method. Degradation experiments on Rhodamine B and Congo red organic pollutants revealed that the optimal degradation rates of Y-BMO were 4.3 and 5.3 times those of pure BMO, respectively. The degradation efficiency of Y-BMO did not significantly decrease after four cycle experiments. As a result of Y^(3+)doping, the crystal structure of BMO changed from a thick layer structure to a thin flower-like structure with an increased specific surface area. X-ray photoelectron spectroscopy showed the presence of highintensity peaks for the O 1s orbital at 531.01 and 530.06 eV, confirming the formation of oxygen vacancies in Y-BMO. Photoluminescence(PL) and electrochemical impedance spectroscopy measurements revealed that the PL intensity and interface resistances of composites decreased significantly, indicating reduced electron–hole pair recombination. This work provides an effective way to prepare high-efficiency Bibased photocatalysts by doping rare earth metal ions for improved photocatalytic performance.

关键词： photocatalysts dye sensitization bismuth molybdate yttrium-doped

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New class of high-entropy pseudobrookite titanate with excellent thermal stability,low thermal expansion coefficient,and low thermal conductivity

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Journal of Advanced Ceramics 2022年第10期11卷 1654-1670页

作者： Jinyu WU xiaohui ma Xiaoxia HU Liwen YAN Feng HOU Jiachen LIU Anran GUO School of materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin UniversityTianjin 300072China

As a type of titanate,the pseudobrookite(MTi_(2)O_(5)/M_(2)TiO_(5))exhibits a low thermal expansion coefficient and thermal conductivity,as well as excellent dielectric and solar spectrum absorption properties.However,the pseudobrookite is unstable and prone to decomposing below 1200℃,which limits the practical application of the pseudobrookite.In this paper,the high-entropy pseudobrookite ceramic is synthesized for the first time.The pure high-entropy(Mg,Co,Ni,Zn)Ti_(2)O_(5) with the pseudobrookite structure and the biphasic high-entropy ceramic composed of the highentropy pseudobrookite(Cr,Mn,Fe,Al,Ga)_(2)TiO_(5) and the high-entropy spinel(Cr,Mn,Fe,Al,Ga,Ti)_(3)O_(4) are successfully prepared by the in-situ solid-phase reaction method.The comparison between the theoretical crystal structure of the pseudobrookite and the aberration-corrected scanning transmission electron microscopy(AC-STEM)images of high-entropy(Mg,Co,Ni,Zn)Ti_(2)O_(5) shows that the metal ions(M and Ti ions)are disorderly distributed at the A site and the B site in high-entropy(Mg,Co,Ni,Zn)Ti_(2)O_(5),leading to an unprecedentedly high configurational entropy of high-entropy(Mg,Co,Ni,Zn)Ti_(2)O_(5).The bulk high-entropy(Mg,Co,Ni,Zn)Ti_(2)O_(5) ceramics exhibit a low thermal expansion coefficient of 6.35×10^(−6) K^(−1) in the temperature range of 25-1400℃ and thermal conductivity of 1.840 W·m^(−1)·K^(−1) at room temperature,as well as the excellent thermal stability at 200,600,and 1400℃.Owing to these outstanding properties,high-entropy(Mg,Co,Ni,Zn)Ti_(2)O_(5) is expected to be the promising candidate for high-temperature thermal insulation.This work has further extended the family of different crystal structures of high-entropy ceramics reported to date.

关键词： high-entropy pseudobrookite (Mg,Co,Ni,Zn)Ti_(2)O_(5) (Cr,Mn,Fe,Al,Ga)_(2)TiO_(5) high conformational entropy thermal expansion coefficient thermal conductivity

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Multiple evaluations of atmospheric behavior between Criegee intermediates and HCHO: Gas-phase and air-water interface reaction

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Journal of Environmental Sciences 2023年第5期127卷 308-319页

作者： Tianlei Zhang Mingjie Wen Chao Ding Yongqi Zhang xiaohui ma Zhuqing Wang makroni Lily Junhai Liu Rui Wang Institute of Theoretical and Computational Chemistry Shaanxi Key Laboratory of CatalysisSchool of Chemical&Environment ScienceShaanxi University of TechnologyHanzhong 723001China School of Environmental Science and Engineering Institute of Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China Shandong Key Laboratory of Biophysics Institute of BiophysicsDezhou UniversityDezhou 253023China Environmental Research Institute Shandong UniversityQingdao 266237China Qinba Mountains of Bio-Resource Collaborative Innovation Center of Southern Shaanxi Province Shaanxi University of TechnologyHanzhong 723001China

Given the high abundance of water in the atmosphere,the reaction of Criegee intermediates(CIs)with(H_(2)O)_(2) is considered to be the predominant removal pathway for CIs.However,recent experimental findings reported that the reactions of CIs with organic acids and carbonyls are faster than expected.At the same time,the interface behavior between CIs and carbonyls has not been reported so far.Here,the gas-phase and air-water interface behavior between Criegee intermediates and HCHO were explored by adopting high-level quantum chemical calculations and Born-Oppenheimer molecular dynamics(BOMD)simulations.Quantum chemical calculations evidence that the gas-phase reactions of CIs+HCHO are submerged energy or low energy barriers processes.The rate ratios speculate that the HCHO could be not only a significant tropospheric scavenger of CIs,but also an inhibitor in the oxidizing ability of CIs on SO_(x) in dry and highly polluted areas with abundant HCHO concentration.The reactions of CH_(2)OO with HCHO at the droplet’s surface follow a loop structure mechanism to produce i)SOZ(■),ii)BHMP(HOCH_(2)OOCH_(2)OH),and iii)HMHP(HOCH_(2)OOH).Considering the harsh reaction conditions between CIs and HCHO at the interface(i.e.,the two molecules must be sufficiently close to each other),the hydration of CIs is still their main atmospheric loss pathway.These results could help us get a better interpretation of the underlying CIs-aldehydes chemical processes in the global polluted urban atmospheres.

关键词： Criegee intermediates HCHO Atmospheric behavior Air-water interface Chemical processes

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North Atlantic subtropical mode water formation controlled by Gulf Stream fronts

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National Science Review 2023年第9期10卷 214-223页

作者： Bolan Gan Jingjie Yu Lixin Wu Gokhan Danabasoglu R.Justin Small Allison H.Baker Fan Jia Zhao Jing xiaohui ma Haiyuan Yang Zhaohui Chen Frontier Science Center for Deep Ocean Multispheres and Earth System(FDOMES) and Physical Oceanography Laboratory Ocean University of China 2. Laoshan Laboratory National Center for Atmospheric Research CAS Key Laboratory of Ocean Circulation and Waves Institute of Oceanology Chinese Academy of Sciences

The North Atlantic Ocean hosts the largest volume of global subtropical mode waters(STMWs) in the world,which serve as heat,carbon and oxygen silos in the ocean interior.STMWs are formed in the Gulf Stream region where thermal fronts are pervasive and result in feedback with the atmosphere.However,their roles in STMW formation have been overlooked.Using eddy-resolving global climate simulations,we find that suppressing local frontal-scale ocean-to-atmosphere(FOA) feedback leads to STMW formation being reduced almost by half.This is because FOA feedback enlarges STMW outcropping,attributable to the mixed layer deepening associated with cumulative excessive latent heat loss due to higher wind speeds and greater air-sea humidity contrast driven by the Gulf Stream fronts.Such enhanced heat loss overshadows the stronger restratification induced by vertical eddies and turbulent heat transport,making STMW colder and he avier.With more realistic representation of FOA feedback,the eddy-present/rich coupled global climate models reproduce the observed STMWs much better than the eddy-free ones.Such improvement in STMW production cannot be achieved,even with the oceanic resolution solely refined but without coupling to the overlying atmosphere in oceanic general circulation models.Our findings highlight the need to resolve FOA feedback to ameliorate the common severe underestimation of STMW and associated heat and carbon uptakes in earth system mo dels.

关键词： North Atlantic subtropical mode water Gulf Stream thermal fronts frontal-scale ocean-to-atmosphere feedback eddy-resolving coupled global climate model

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CT manifestations of childhood pancreatoblastoma

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World Journal of Pediatric Surgery 2022年第3期5卷 187-191页

作者： Meijun Sheng Ruifang Zhang xiaohui ma Haichun Zhou Surgical Intensive Care Unit Zhejiang University School of Medicine Children's HospitalHangzhouZhejiangChina Department of Radiology Zhejiang University School of Medicine Children's HospitalHangzhouZhejiangChina

Pancreatoblastoma is the most common type of malignant pancreatic tumor in children under 10 years old,accounting for 25%of pancreatic tumors.1 The imaging findings of pancreatoblastoma are non-specific,and most of tumors are lobulated masses with well-circumscribed or partially circumscribed margins,accompanied by necrosis and enhancing septations on contrast-enhanced CT.2 When a large tumor originates in the pancreas,pancreatoblastoma is one of the top differential diagnoses in children because of its relative frequency in this age group.

关键词： tumor pancreas finding

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Passivating buried interface with multifunctional novel ionic liquid containing simultaneously fluorinated anion and cation yielding stable perovskite solar cells over 23% efficiency

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Journal of Energy Chemistry 2022年第6期31卷 659-666,I0018页

作者： Deyu Gao Liqun Yang xiaohui ma Xueni Shang Chen Wang Mengjia Li Xinmeng Zhuang Boxue Zhang Hongwei Song Jiangzhao Chen Cong Chen School of material Science and Engineering State Key Laboratory of Reliability and Intelligence of Electrical EquipmentHebei University of TechnologyTianjin 300130China State Key Laboratory of Integrated Optoelectronics College of Electronic Science and EngineeringJilin UniversityChangchun 130012JilinChina Chimie ParisTech PSL Research UniversityCNRSInstitut de Recherche de Chimie Paris(IRCP)UMR824711 rue P.et M.CurieF-75005 ParisFrance Key Laboratory of Optoelectronic Technology&Systems(Ministry of Education) College of Optoelectronic EngineeringChongqing UniversityChongqing 400044China

Interfacial defects and energy barrier would result in serious interfacial non-radiative recombination losses.In addition,the quality of perovskite films is highly dependent on deposition substrates.Consequently,there is an urgent desire to develop multifunctional interface modulators to manage the interface between electron transport layer and perovskite layer.Here,we report a multifunctional buried interface modulation strategy that 4-fluoro-phenylammonium tetrafluoroborate (FBABF_(4)) consisting of simultaneously fluorinated anion and cation is inserted between SnO_(2)layer and perovskite layer.It is uncovered by time-of-flight secondary ion mass spectroscopy that the anion and cation in modifier are mainly located at this interface,which is put down to coordination bond of the fluorine atom on BF_(4)^(-) with SnO_(2),and the hydrogen bond of the fluorine atom on FBA^(+) with formamidinium.This suggests that simultaneous fluorination of anion and cation in the ionic liquid molecule is of crucial importance to ameliorate interfacial contact through chemical linker.The interface modification approach enables the realization of interfacial defect passivation,interfacial energy band alignment modulation,and perovskite crystallization manipulation,which are translated into enhanced efficiency and stability as well as significantly suppressed hysteresis.The multiple functions of FBABF_(4) endow the modified solar cells excellent photovoltaic performance with an efficiency exceeding 23%along with appealing long-term stability.This work highlights the critical role of fluorination strategy in engineering multifunctional organic salt modulators for improving interfacial contact.

关键词： Perovskite solar cells Interface engineering Buried interface Ionic liquid Multifunctional

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