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Accelerated reconstruction of ZIF-67 with significantly enhanced glucose detection sensitivity

Nano Research 2024年第6期17卷 4737-4743页

作者： Huihui jin Weihao Zeng Wei Qian Lun Li pengxia ji Zhengying Li Daping He School of Information Engineering Wuhan University of TechnologyWuhan 430070China Hubei Engineering Research Center of RF-Microwave Technology and Application Wuhan University of TechnologyWuhan 430070China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Research on metal-organic framework(MOF)-based non-enzymatic glucose sensors usually ignores the impact of the surface reconstruction degree of MOF on the activity of catalyzing glucose oxidation.In this work,we choose zeolitic imidazolate framework-67(ZIF-67),which is commonly used in glucose sensing,as a representative to investigate the influence of reconstruction degree on its structure and glucose catalytic performance.By employing the electrochemical activation strategy,the activity of ZIF-67 in catalyzing glucose gradually increased with the prolongation of the activation time,reaching the optimum after 2 h activation.The detection sensitivity of the activated ZIF-67 was 19 times higher than that of the initial ZIF-67,and the limit of detection(LOD)was lowered from 7 to 0.4μM.Our findings demonstrate that the oxidation degree of ZIF-67 deepened rapidly with continuously activation and was basically reconstructed to CoOOH after 2 h activation,accompanied by a morphological change from cuboctahedral to flower-like.Simultaneously,theoretical investigation revealed that ZIF-67 is not suitable as a stable glucose sensor electrode since the adsorbed glucose molecules hasten the dissociation of ligands and the breaking of Co-N bond in ZIF-67.Therefore,our work has important implications for the rational design of next-generation MOF-based glucose sensors.

关键词： zeolitic imidazolate framework-67(ZIF-67) glucose oxidation electrochemical activation reconstruction CoOOH

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Hybrid ionic/electronic interphase enabling uniform nucleation and fast diffusion kinetics for stable lithium metal anode

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Chinese Chemical Letters 2024年第2期35卷 626-633页

作者： Lun Li pengxia ji Meng Huang Zixin Zhang Hong Wang Francis Verpoort jinlong Yang Daping He State Key Laboratory of Advanced Technology for Materials Synthesis and Processing School of Materials Science and EngineeringWuhan University of TechnologyWuhan 430070China Guangdong Research Center for Interfacial Engineering of Functional Materials College of Materials Science and EngineeringShenzhen UniversityShenzhen 518060China Sanya Science and Education Innovation Park of Wuhan University of Technology Sanya 572000China Hubei Engineering Research Center of RF-Microwave Technology and Application Wuhan University of TechnologyWuhan 430070China State Key Laboratory of Silicate Materials for Architectures Wuhan University of TechnologyWuhan 430070China

Lithium(Li)dendrite issue,which is usually caused by inhomogeneous Li nucleation and fragile solid electrolyte interphase(SEI),impedes the further development of high-energy Li metal batteries.However,the integrated construction of a high-stable SEI layer that can regulate uniform nucleation and facilitate fast Li-ion diffusion kinetics for Li metal anode still falls short.Herein,we designed an artificial SEI with hybrid ionic/electronic interphase to regulate Li deposition by in-situ constructing metal Co clusters embedded in LiF matrix.The generated Co and LiF both enable fast Li-ion diffusion kinetics,meanwhile,the lithiophilic properties of Co clusters can serve as Li-ion nucleation sites,thereby contributing to uniform Li nucleation and non-dendritic growth.As a result,a dendrite-free Li deposition with a low overpotential(16.1 mV)is achieved,which enables an extended lifespan over 750 h under strict conditions.The full cells with high-mass-loading LiFePO_(4)(11.5 mg/cm^(2))as cathodes exhibit a remarkable rate capacity of 84.1 mAh/g at 5 C and an improved cycling performance with a capacity retention of 96.4%after undergoing 180 cycles.

关键词： Lithium metal anode Hybrid ionic/electronic interphase Solid electrolyte interphase Fast diffusion kinetics Dendritic growth of lithium

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Trend of Developing Aqueous Liquid and Gel Electrolytes for Sustainable,Safe,and High‑Performance Li‑Ion Batteries

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Nano-Micro Letters 2024年第1期16卷 17-34页

作者： Donghwan ji Jaeyun Kim School of Chemical Engineering Sungkyunkwan University(SKKU)Suwon 16419Republic of Korea Department of Health Sciences and Technology Samsung Advanced Institute for Health Sciences&Technology(SAIHST)Sungkyunkwan University(SKKU)Suwon 16419Republic of Korea Biomedical Institute for Convergence at SKKU(BICS) Sungkyunkwan University(SKKU)Suwon 16419Republic of Korea Institute of Quantum Biophysics(IQB) Sungkyunkwan University(SKKU)Suwon 16419Republic of Korea Present Address:Department of NanoEngineering University of California San DiegoLa JollaSan DiegoCA 92093USA

Current lithium-ion batteries(LIBs)rely on organic liquid electrolytes that pose significant risks due to their flammability and toxicity.The potential for environmental pollution and explosions resulting from battery damage or fracture is a critical concern.Water-based(aqueous)electrolytes have been receiving attention as an alternative to organic electrolytes.However,a narrow electrochemicalstability window,water decomposition,and the consequent low battery operating voltage and energy density hinder the practical use of aqueous electrolytes.Therefore,developing novel aqueous electrolytes for sustainable,safe,high-performance LIBs remains challenging.This Review first commences by summarizing the roles and requirements of electrolytes–separators and then delineates the progression of aqueous electrolytes for LIBs,encompassing aqueous liquid and gel electrolyte development trends along with detailed principles of the electrolytes.These aqueous electrolytes are progressed based on strategies using superconcentrated salts,concentrated diluents,polymer additives,polymer networks,and artificial passivation layers,which are used for suppressing water decomposition and widening the electrochemical stability window of water of the electrolytes.In addition,this Review discusses potential strategies for the implementation of aqueous Li-metal batteries with improved electrolyte–electrode interfaces.A comprehensive understanding of each strategy in the aqueous system will assist in the design of an aqueous electrolyte and the development of sustainable and safe high-performance batteries.

关键词： Lithium-ion battery(LIB) Aqueous electrolyte Gel electrolyte Electrochemical stability window Li dendrite

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Tuning Active Metal Atomic Spacing by Filling of Light Atoms and Resulting Reversed Hydrogen Adsorption-Distance Relationship for Efficient Catalysis

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Nano-Micro Letters 2023年第10期15卷 151-162页

作者： Ding Chen Ruihu Lu Ruohan Yu Hongyu Zhao Dulan Wu Youtao Yao Kesong Yu jiawei Zhu pengxia ji Zonghua Pu Zongkui Kou Jun Yu jinsong Wu Shichun Mu State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070People’s Republic of China NRC(Nanostructure Research Centre) Wuhan University of TechnologyWuhan 430070People’s Republic of China

Precisely tuning the spacing of the active centers on the atomic scale is of great significance to improve the catalytic activity and deepen the understanding of the catalytic mechanism,but still remains a challenge.Here,we develop a strategy to dilute catalytically active metal interatomic spacing(d_(M-M))with light atoms and discover the unusual adsorption patterns.For example,by elevating the content of boron as interstitial atoms,the atomic spacing of osmium(d_(Os-Os))gradually increases from 2.73 to 2.96?.More importantly,we find that,with the increase in dOs-Os,the hydrogen adsorption-distance relationship is reversed via downshifting d-band states,which breaks the traditional cognition,thereby optimizing the H adsorption and H_2O dissociation on the electrode surface during the catalytic process;this finally leads to a nearly linear increase in hydrogen evolution reaction activity.Namely,the maximum dOs-Os of 2.96?presents the optimal HER activity(8 mV@10 mA cm^(-2))in alkaline media as well as suppressed O adsorption and thus promoted stability.It is believed that this novel atomic-level distance modulation strategy of catalytic sites and the reversed hydrogen adsorption-distance relationship can shew new insights for optimal design of highly efficient catalysts.

关键词： Electrocatalysis DFT calculation Interstitial filling Hydrogen evolution Structure–activity relationships

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Photocatalytic activation of sulfite by N-doped porous biochar/MnFe_(2)O_(4) interface-driven catalyst for efficient degradation of tetracycline

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Green Energy & Environment 2024年第3期9卷 481-494页

作者： Long Cheng Yuanhui ji jiangsu Province Hi-Tech Key Laboratory for Biomedical Research School of Chemistry and Chemical EngineeringSoutheast UniversityNanjing211189China

A novel photo-catalytic system composed of N-doped biochars(NBCs),MnFe_(2)O_(4) and sulfite activation under ultraviolet(NBCs/MnFe_(2)O_(4)/sulfite/UV)was constructed to realize the efficient eliminate of tetracycline(TC).As the carrier of MnFe_(2)O_(4),NBCs were synthesized from alfalfa,which has large specific surface area,graphite like structure and hierarchical porous structure.The adsorption isotherm indicated that NBCs/MnFe_(2)O_(4)-2:1 had the best adsorption performance for TC(347.56 mg g^(-1)).Through synergistic adsorption and photocatalysis,the removal rate of TC reached 84%,which was significantly higher than that of MnFe_(2)O_(4).Electrochemical impedance spectroscopy(EIS)and Photoluminescence(PL)characterization results showed that the introduction of NBCs improved the separation efficiency of photogenerated electron and hole pairs and enhanced the photocatalytic performance.Moreover,the adsorption,degradation mechanism and degradation path of TC by the catalyst were systematically analyzed by coupling HPLC–MS measurement with the theoretical calculation.Considering the advantages of excellent degradation performance,low cost,easy separation and environmental friendliness of NBCs/MnFe_(2)O_(4),this work was expected to provide a new path for the practical application of biochar.

关键词： Biochar MnFe_(2)O_(4) Sulfite Adsorption Photocatalysis

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Small Cycles Property of Some Cremer Rational Maps and Polynomials

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Chinese Annals of Mathematics,Series B 2024年第1期45卷 123-136页

作者： Rong FU ji ZHOU Faculty of Science Yibin UniversityYibin 644000SichuanChina Department of Mathematical Sciences Sichuan Normal UniversityChengdu 610066China

This paper concerns the linearization problem on rational maps of degree d≥2 and polynomials of degree d>2 from the perspective of non-linearizability.The authors introduce a set l_(∞) of irrational numbers and show that if α∈l_(∞),then any rational map is not linearizable and has infinitely many cycles in every neighborhood of the fixed point with multiplier λ=e^(2πiα),Adding more constraints to cubic polynomials,they discuss the above problems by polynomial-like maps.For the family of polynomials,with the help of Yoccoz's method,they obtain its maximum dimension of the set in which the polynomials are non-linearizable.

关键词： Irrationally indifferent fixed point Linearization problem Small cycles property

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Soft coarse-grained particle model for particle-fluid systems

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Particuology 2024年第1期84卷 178-193页

作者： Yanhao Ye ji Xu Wei Ge State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing100049China Innovation Academy for Green Manufacture Chinese Academy of SciencesBeijing100190China

By modeling a group of neighboring real particles as a single coarse-grained particle(CGP),discrete particle method(DPM)is now capable of simulating industrial-scale particle-fluid systems.However,a systematic approach to determine the CGP properties and develop their interaction models is still lacking,which casts uncertainty on the predictivity of the method.In this study,collisions between predefined particle groups are analyzed to construct kernel functions for modeling the CGPs and then the model parameters are determined by equating the statistical properties of the CGPs and the real particles in the physical process studied.This approach is implemented for homogeneous cooling of granular gas,then demonstrated effective in simulating experimental fluidized beds.

关键词： Coarse-grain(CG) Discrete particle method(DPM) Fluidized bed Multi-scale simulation

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Semi-derived Ringel-Hall algebras and Hall algebras of odd-periodic relative derived categories

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Science China Mathematics 2024年第8期67卷 1735-1760页

作者： ji Lin Liangang Peng Department of Mathematics and Statistics Fuyang Normal University School of Mathematics Sichuan University

Let t be a positive integer and A be a hereditary abelian category satisfying some finiteness conditions. We define the semi-derived Ringel-Hall algebra of A from the category CZ/t（A） of Z/t-graded complexes and obtain a natural basis of the semi-derived Ringel-Hall algebra. Moreover, we describe the semiderived Ringel-Hall algebra by the generators and defining relations. In particular, if t is an odd integer, we show an embedding of the derived Hall algebra of the odd-periodic relative derived category in the extended semi-derived Ringel-Hall algebra.

关键词： hereditary abelian categories the categories of $\mathbb{Z}/t$-graded complexes semi-derived Ringel-Hall algebras derived Hall algebras

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Boosting electrocatalytic nitrate reduction to ammonia via Cu_(2)O/Cu(OH)_(2)heterostructures promoting electron transfer

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Nano Research 2024年第6期17卷 4898-4907页

作者： jing Geng Sihan ji Anhui Province International Research Center on Advanced Building Materials School of Materials Science and Chemical EngineeringAnhui Jianzhu UniversityHefei 230601China Anhui Province Key Laboratory of Advanced Building Materials Anhui Jianzhu UniversityHefei 230601China School of Energy Materials and Chemical Engineering Hefei UniversityHefei 230601China

Electrocatalytic nitrate(NO_(3)^(−))reduction to ammonia(NH_(3))offers a viable approach for sustainable NH_(3)production and environmental denitrification.Copper(Cu)possesses a distinctive electronic structure,which can augment the reaction kinetics of NO_(3)^(−)and impede hydrogen evolution reaction(HER),rendering it a promising contender for the electrosynthesis of NH_(3)from NO_(3)^(−).Nevertheless,the role of Cu_(2)O in copper-based catalysts still requires further investigation for a more comprehensive understanding.Herein,the Cu_(2)O/Cu(OH)_(2)heterostructures are successfully fabricated through liquid laser irradiation using CuO nanoparticles as a precursor.Experimental and theoretical researches reveal that Cu_(2)O/Cu(OH)_(2)heterostructure exhibits enhanced electrocatalytic performance for NO_(3)^(−)to NH_(3)because Cu(OH)_(2)promotes electron transfer and reduces the valence state of Cu active site in Cu_(2)O.At−0.6 V(vs.reversible hydrogen electrode(RHE)),the NH_(3)yield reaches its maximum at 1630.66±29.72μg·h^(−1)·mgcat^(−1),while the maximum of Faraday efficiency(FE)is 76.95%±5.51%.This study expands the technical scope of copper-based catalyst preparation and enhances the understanding of the electrocatalytic mechanism of NO_(3)^(−)to NH_(3).

关键词： Cu_(2)O/Cu(OH)_(2)heterostructures electron transfer ammonia synthesis electrocatalysts nitrate

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Detection and analysis of serum bile acid profile in patients with colonic polyps

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World Journal of Clinical Cases 2024年第13期12卷 2160-2172页

作者： Xin ji Hong Chen School of Medicine Southeast UniversityNanjing 210009Jiangsu ProvinceChina Department of Gastroenterology Zhongda Hospital Southeast UniversityNanjing 210009Jiangsu ProvinceChina

BACKGROUND Analyzing the variations in serum bile acid(BA)profile can provide a certain biological basis for early warning and prevention of various diseases.There is currently no comprehensive study on the relationship between the serum BA profile and colonic polyps.AIM To study the serum BA profile detection results of patients with colonic polyps,and analyze the correlation between BA and colonic polyps.METHODS From January 1,2022,to June 1,2023,204 patients with colonic polyps who were diagnosed and treated at Zhongda Hospital Southeast University were chosen as the study subjects,and 135 non-polyp people who underwent physical examination were chosen as the control group.Gathering all patients'clinical information,typical biochemical indicators,and BA profile.RESULTS Compared with the control group,the serum levels of taurocholic acid,glycocholic acid,glycochenodeoxycholic acid,and taurochenodeoxycholic acid in the colonic polyp group were significantly higher than those in the control group,while the content of deoxycholic acid(DCA)was lower than that in the control group(P<0.05).When colonic polyps were analyzed as subgroups,it was shown that there was a strong correlation between changes in the BA profile and polyp diameter,location,morphology,pathological kind,etc.CONCLUSION The serum BA profile showed significant changes in patients with colonic polyps,with a significant increase in primary conjugated BA content and a decrease in secondary free bile acid DCA content.There is a certain correlation between primary free BA and pathological parameters of polyps.

关键词： Serum Bile acid profile Colonic polyps Bile acid metabolism

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