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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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How variable progenitor clones construct a largely invariant neocortex

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National Science Review 2024年第1期11卷 129-144页

作者： Zhongfu Shen Jiajun Yang Qiangqiang Zhang Kuiyu Wang xiaohui Lv Xiaolin Hu Jian ma Song-Hai Shi New Cornerstone Science Laboratory IDG/McG overn Institute for Brain Research Tsinghua-Peking Center for Life Sciences Beijing Frontier Research Center for Biological Structure School of Life Sciences Tsinghua University Department of Computer Sciences Tsinghua University College of Life Sciences Nankai University Chinese Institute for Brain Research

The neocortex contains a vast collection of diverse neurons organized into distinct layers. While nearly all neocortical neurons are generated by radial glial progenitors(RGPs), it remains largely unclear how a complex yet organized neocortex is constructed reliably and robustly. Here, we show that the division behavior and neuronal output of RGPs are highly constrained with patterned variabilities to support the reliable and robust construction of the mouse neocortex. The neurogenic process of RGPs can be well-approximated by a consistent Poisson-like process unfolding over time, producing deep to superficial layer neurons progressively. The exact neuronal outputs regarding layer occupation are variable; yet, this variability is constrained systematically to support all layer formation, largely reflecting the variable intermediate progenitor generation and RGP neurogenic entry and exit timing differences. Together, these results define the fundamental features of neocortical neurogenesis with a balanced reliability and variability for the construction of the complex neocortex.

关键词： neocortex radial glial progenitor intermediate progenitor neurogenesis clonal variability layer formation

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Sensitivity Analysis of Electromagnetic Scattering from Dielectric Targets with Polynomial Chaos Expansion and Method of Moments

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Computer Modeling in Engineering & Sciences 2024年第8期140卷 2079-2102页

作者： Yujing ma Zhongwang Wang Jieyuan Zhang Ruijin Huo xiaohui Yuan College of Architecture and Civil Engineering Xinyang Normal UniversityXinyang464000China Henan International Joint Laboratory of Structural Mechanics and Computational Simulation College of Architecture and Civil EngineeringHuanghuai UniversityZhumadian463000China Academy of Military Sciences Beijing100091China Henan New Environmentally-Friendly Civil Engineering materials Engineering Research Center Xinyang Normal UniversityXinyang464000China

In this paper,an adaptive polynomial chaos expansion method(PCE)based on the method of moments(MoM)is proposed to construct surrogate models for electromagnetic scattering and further sensitivity analysis.The MoM is applied to accurately solve the electric field integral equation(EFIE)of electromagnetic scattering from homogeneous dielectric targets.Within the bistatic radar cross section(RCS)as the research object,the adaptive PCE algorithm is devoted to selecting the appropriate order to construct the multivariate surrogate model.The corresponding sensitivity results are given by the further derivative operation,which is compared with those of the finite difference method(FDM).Several examples are provided to demonstrate the effectiveness of the proposed algorithm for sensitivity analysis of electromagnetic scattering from homogeneous dielectric targets.

关键词： Adaptive polynomial chaos expansion method method of moments radar cross section electromagnetic scattering

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Cobalt-doped TiO_(2)@C hierarchical nanocomposites derived from Ti_(3)C_(2) MXene as cathodes for hybrid magnesium-lithium batteries

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Nano Research 2024年第1期17卷 253-261页

作者： xiaohui Li Yakun Tang Lang Liu Yue Zhang Yang Gao mao Qian Wenjie ma State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources College of ChemistryXinjiang UniversityUrumqi 830017China

TiO_(2)has been explored in hybrid magnesium-lithium batteries(HMLBs)due to the advantages of low self-discharge and small volume expansion during ion insertion.However,how to improve the inherently low ionic and electrical conductivity of TiO_(2)is the problem that needs to be solved.In this work,a smart strategy is adopted to prepare cobalt-doped TiO_(2)@C(Co^(4+)-TiO_(2)@C)hierarchical nanocomposite derived from Co(II)(OH)n@Ti3C2.Compared with TiO_(2)@C(without cobalt doping),Co^(4+)-TiO_(2)@C shows the highest specific capacity(154.7 mah·g^(-1)at 0.1 A·g^(-1)after 200 cycles)and extraordinary rate performance in HMLBs.The excellent electrochemical performance of Co4+-TiO_(2)@C is ascribed to the synergistic effect of the hierarchical structure and cobalt-doping.Both experimental results and density functional theory(DFT)calculation reveal that the cobalt-doping has effectively improved the electronic conductivity and reduced the Li+migration barrier.This work provides a new insight to design TiO_(2)-based cathode materials with high-performance in HMLBs.

关键词： Ti_(3)C_(2)MXene TiO_(2) hybrid magnesium-lithium batteries hierarchical structure cobalt-doping

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Electrostatic and hydrophobic interaction cooperative nanochaperone regulates protein folding

Aggregate

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Aggregate 2024年第1期5卷 419-426页

作者： xiaohui Wu Fei Deng Yujie Chen Mengchen Xu Feihe ma Linqi Shi Key Laboratory of Functional Polymer materials of Ministry of Education State Key Laboratory of Medicinal Chemical BiologyInstitute of Polymer Chemistry and College of ChemistryNankai UniversityTianjinP.R.China School of materials Science and Engineering and State Key Laboratory of Separation Membranes and Membrane Processes Tiangong UniversityTianjinP.R.China

Natural molecular chaperones utilize spatially ordered multiple molecular forces to effectively regulate protein folding.However,synthesis of such molecules is a big challenge.The concept of“aggregate science”provides insights to construct chemical entities(aggregates)beyond molecular levels to mimic both the structure and function of natural chaperone.Inspired by this concept,herein we fabricate a novel multi-interaction(i.e.,electrostatic and hydrophobic interaction)cooperative nanochaperone(multi-co-nChap)to regulating protein folding.This multi-co-nChap is fabricated by rationally introducing electrostatic interactions to the surface(corona)and confined hydrophobic microdomains(shell)of traditional single-hydrophobic interaction nanochaperone.We demonstrate that the corona electrostatic attraction facilitates the diffusion of clients into the hydrophobic microdomains,while the shell electrostatic interaction balances the capture and release of clients.By finely synergizing corona electrostatic attraction with shell electrostatic repulsion and hydrophobic interaction,the optimized multi-co-nChap effectively facilitated de novo folding of nascent polypeptides.Moreover,the synergy between corona electrostatic attraction,shell electrostatic attraction and shell hydrophobic interaction significantly enhanced the capability of multi-co-nChap to protect native proteins from denaturation at harsh temperatures.This work provides important insights for understanding and design of nanochaperone,which is a kind of ordered aggregate with chaperone-like activity that beyond the level of single molecule.

关键词： chaperone-like activity cooperative effect nanochaperones ordered aggregates protein folding

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Aqueous-phase formation of N-containing secondary organic compounds affected by the ionic strength

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Journal of Environmental Sciences 2024年第4期138卷 88-101页

作者： Yuqi Gan xiaohui Lu Shaodong Chen Xinghua Jiang Shanye Yang Xiewen ma Mei Li Fan Yang Yewen Shi Xiaofei Wang Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention Department of Environmental Science and EngineeringFudan UniversityShanghai 200433China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China Guangdong Provincial Observation and Research Station for Coastal Atmosphere and Climate of the Great Bay Area Southern University of Science and TechnologyShenzhen 518055China Institute of mass Spectrometry and Atmospheric Environment Guangdong Provincial Engineering Research Center for On-line Source Apportionment System of Air PollutionJinan UniversityGuangzhouChina Environmental Monitoring Station of Pudong New District Shanghai 201200China Shanghai Municipal Center for Disease Control&Prevention Shanghai 200336China

The reaction of carbonyl-to-imine/hemiaminal conversion in the atmospheric aqueous phase is a critical pathway to produce the light-absorbing N-containing secondary organic compounds(SOC).The formation mechanism of these compounds has been wildly investigated in bulk solutions with a low ionic strength.However,the ionic strength in the aqueous phase of the polluted atmosphere may be higher.It is still unclear whether and to what extent the inorganic ions can affect the SOC formation.Here we prepared the bulk solution with certain ionic strength,in which glyoxal and ammonium were mixed to mimic the aqueous-phase reaction.Molecular characterization by High-resolution mass Spectrometry was performed to identify the N-containing products,and the light absorption of the mixtures was measured by ultraviolet-visible spectroscopy.Thirty-nine N-containing compounds were identified and divided into four categories(N-heterocyclic chromophores,high-molecular-weight compounds with N-heterocycle,aliphatic imines/hemiaminals,and the unclassified).It was observed that the longer reaction time and higher ionic strength led to the formation of more N-heterocyclic chromophores and the increasing of the lightabsorbance of the mixture.The added inorganic ions were proposed to make the aqueous phase somewhat viscous so that the molecules were prone to undergo consecutive and intramolecular reactions to form the heterocycles.In general,this study revealed that the enhanced ionic strength and prolonged reaction time had the promotion effect on the lightabsorbing SOC formation.It implies that the aldehyde-derived aqueous-phase SOC would contribute more light-absorbing particulate matter in the industrial or populated area where inorganic ions are abundant.

关键词： Ionic strength Carbonyl-to-imine/hemiaminal Heterocyclic Brown carbon mass spectrometry Aqueous-phase reaction

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Antagonism effect of residual S triggers the dual-path mechanism for water oxidation

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Journal of Energy Chemistry 2024年第6期93卷 568-579,I0014页

作者： Li Liu Jinming Cao Siqi Hu Tinghui Liu Can Xu Wensheng Fu Xinguo ma xiaohui Yang Chongqing Key Laboratory of Green Catalytic materials and Technology College of ChemistryChongqing Normal UniversityChongqing 401331China School of Science Hubei University of TechnologyWuhan 430068HubeiChina Chongqing Institute of Green and Intelligent Technology Chinese Academy of SciencesChongqing 400714China

Transition metal chalcogenides(TMCs)are recognized as pre-catalysts,and their(oxy)hydroxides derived from electrochemical reconstruction are the active species in the water oxidation.However,understanding the role of the residual chalcogen in the reconstructed layer is lacking in detail,and the corresponding catalytic mechanism remains controversial.Here,taking Cu_(1-x)Co_(x)S as a platform,we explore the regulating effect and existence form of the residual S doped into the reconstructive layer for oxygen evolution reaction(OER),where a dual-path OER mechanism is proposed.First-principles calculations and operando~(18)O isotopic labeling experiments jointly reveal that the residual S in the reconstructive layer of Cu_(1-x)Co_(x)S can wisely balance the adsorbate evolution mechanism(AEM)and lattice oxygen oxidation mechanism(LOM)by activating lattice oxygen and optimizing the adsorption/desorption behaviors at metal active sites,rather than change the reaction mechanism from AEM to LOM.Following such a dual-path OER mechanism,Cu_(0.4)Co_(0.6)S-derived Cu_(0.4)Co_(0.6)OSH not only overcomes the restriction of linear scaling relationship in AEM,but also avoids the structural collapse caused by lattice oxygen migration in LOM,so as to greatly reduce the OER potential and improved stability.

关键词： Electrochemical reconstruction Adsorbate evolution mechanism Lattice oxygen oxidation mechanism Oxygen evolution reaction Residual sulfur

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CD36 promotes tubular ferroptosis by regulating the ubiquitination of FSP1 in acute kidney injury

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Genes & Diseases 2024年第1期11卷 449-463页

作者： Yixin ma Lili Huang Zheng Zhang Pengfei Yang Qingsong Chen Xujia Zeng Fangyan Tan Chunxia Wang Xiongzhong Ruan xiaohui Liao Department of Nephrology The Second Affiliated HospitalChongqing Medical UniversityChongqing 400010China Department of Cell Biology and Genetics Chongqing Medical UniversityChongqing 400016China Centre for Nephrology Royal Free and University College Medical SchoolUniversity College LondonRoyal Free CampusRowland Hill StreetLondon NW32PFUnited Kingdom Centre for Lipid Research Key Laboratory of Molecular Biology on Infectious DiseasesMinistry of EducationChongqing Medical UniversityChongqing 400016China Kuanren Laboratory of Translational Lipidology Centre for Lipid ResearchSecond Affiliated Hospital of Chongqing Medical UniversityChongqing 400010China

Reactive oxidative species(ROos)production-driven ferroptosis plays a role in acute kidney injury(Akl).However,its exact molecular mechanism is poorly understood.Scavenger receptor CD36 has important roles in oxidizing lipids,lipid accumulation,metabolic syndrome,and insulin resistance in chronic kidney disease,but its roles remain unexplored in AKl.The present study investigated the role and mechanism of CD36 in regulating proximal tubular cell ferroptosis and AKl.The expression of CD36 was found to be significantly up-regulated in AKI renal tissues and correlated with renal function,which might serve as an independent biomarker for AKl patients.Moreover,in adult mice subjected to AKl,deletion of CD36(CD36-/-)induced tubular cell Ros accumulation,ferroptosis activation,and renal injury.Mechanistically,combining LC-MS/MS,co-IP,and ubiquitination analyses revealed that CD36 could specifically bind to ferroptosis suppressor protein 1(FSP1)and regulate its ubiquitination at sites K16 and K24,leading to FSP1 degradation and progression of ferroptosis in AKl.The present results emphasize a novel mechanism of CD36 in cisplatin-induced AKl.The discovery of the special CD36 roles in promoting ferroptosis and AKI development by regulating the ubiquitination of FSP1 in proximal tubular cells may be potential therapeutic targets for AKl.Moreover,CD36 may play a key role in the progression of AKl.Therefore,targeting CD36 may provide a promising treatment option for AKI.

关键词： Acute kidney injury CD36 Ferroptosis FSP1 Ubiquitin-dependent degradation

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Selective leaching of lithium from spent lithium-ion batteries using sulfuric acid and oxalic acid

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International Journal of Minerals,Metallurgy and materials 2024年第4期31卷 688-696页

作者： Haijun Yu Dongxing Wang Shuai Rao Lijuan Duan Cairu Shao xiaohui Tu Zhiyuan ma Hongyang Cao Zhiqiang Liu Institute of Advanced Wear&Corrosion Resistant and Functional materials Jinan UniversityGuangzhou 510632China Institute of Resources Utilization and Rare Earth Development Guangdong Academy of SciencesGuangzhou 510650China State Key Laboratory of Separation and Comprehensive Utilization of Rare Metals Guangzhou 510650China Guangdong Province Key Laboratory of Rare Earth Development and Application Guangzhou 510650China

Traditional hydrometallurgical methods for recovering spent lithium-ion batteries(LIBs)involve acid leaching to simultaneously extract all valuable metals into the leachate.These methods usually are followed by a series of separation steps such as precipitation,extraction,and stripping to separate the individual valuable metals.In this study,we present a process for selectively leaching lithium through the synergistic effect of sulfuric and oxalic acids.Under optimal leaching conditions(leaching time of 1.5 h,leaching temperature of 70°C,liquid-solid ratio of 4 mL/g,oxalic acid ratio of 1.3,and sulfuric acid ratio of 1.3),the lithium leaching efficiency reached89.6%,and the leaching efficiencies of Ni,Co,and Mn were 12.8%,6.5%,and 21.7%.X-ray diffraction(XRD)and inductively coupled plasma optical emission spectrometer(ICP-OES)analyses showed that most of the Ni,Co,and Mn in the raw material remained as solid residue oxides and oxalates.This study offers a new approach to enriching the relevant theory for selectively recovering lithium from spent LIBs.

关键词： selective leaching oxalic acid sulfuric acid spent lithium-ion batteries

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Designing ABC-6 family small pore zeolites by epitaxial growth approach

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Chinese Chemical Letters 2024年第3期35卷 508-512页

作者： xiaohui Cui Jia Lv Chao ma Yujiao Wang Zhenghao Jia Daliang Zhang Peng Guo Zhongmin Liu Henan Institute of Advanced Technology Zhengzhou UniversityZhengzhou 450001China National Engineering Research Center of Lower-Carbon Catalysis Technology Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Multi-scale Porous materials Center Institute of Advanced Interdisciplinary Studies&School of Chemistry EngineeringChongqing UniversityChongqing 400044China University of Chinese Academy of Sciences Beijing 100049China Division of Energy Research Resources Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China

Aluminosilicate small pore zeolites belonging to ABC-6 family play crucially important roles in the high methanol conversion with the high selectivity of light olefins,gas separation and storage,and selective catalytic reduction of NO_(x).In this work,we report a general method,called the epitaxial growth approach,for designing ABC-6 family small pore zeolites.It is mainly realized through the epitaxial growth on the nonporous SOD-type zeolite in the presence of inorganic cations(Na^(+)and K^(+))combined with a variety of organic structure directing agents(OSDAs).In this case,a series of ABC-6 family small pore zeolites such as ERI-,SWY-,LEV-,AFX-,and PTT-type zeolites have been successfully synthesized within a few hours.More importantly,the advanced focused ion beam(FIB)and the low-dose high-resolution transmission electron microscopy(HRTEM)imaging technique have been utilized for unraveling the zeolite heterojunction at the atomic level during the epitaxial growth process.It turns out(222)crystallographic planes of the SOD-type zeolite substrate provide unique pre-building units,which facilitate the growth of targeted ABC-6 family small pore zeolites along its c-axis.Moreover,the morphologies of ERI-type zeolite can also be tuned through the epitaxial growth approach,achieving a longer lifetime in the methanol conversion.

关键词： Zeolite structure Zeolite synthesis Structural characterizations Low-dose imaging Focused ion beam

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