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Universal insertion of molecules in ionic compounds under pressure

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national Science Review 2024年第1期11卷 120-128页

作者： Feng Peng Yanming ma Chris J.Pickard Hanyu Liu maosheng Miao College of Physics and Electronic Information Luoyang Normal University Department of Chemistry and Biochemistry California State University Northridge State Key Laboratory of Superhard materials & Key Laboratory of material Simulation Methods and Software of Ministry of Education College of Physics Jilin University International Center of Future Science Jilin University Department of materials Science & Metallurgy University of Cambridge Advanced Institute for materials Research Tohoku University Department of Earth Science University of California Santa Barbara

Using first-principles calculations and crystal structure search methods, we found that many covalently bonded molecules such as H2, n2, CO2, nH3, H2O and CH4may react with naC l, a prototype ionic solid,and form stable compounds under pressure while retaining their molecular structure. These molecules,despite whether they are homonuclear or heteronuclear, polar or non-polar, small or large, do not show strong chemical interactions with surrounding na and Cl ions. In contrast, the most stable molecule among all examples, n2, is found to transform into cyclo-n5-anions while reacting with naC l under high pressures. It provides a new route to synthesize pentazolates, which are promising green energy materials with high energy density. Our work demonstrates a unique and universal hybridization propensity of covalently bonded molecules and solid compounds under pressure. This surprising miscibility suggests possible mixing regions between the molecular and rock layers in the interiors of large planets.

关键词： molecule-solid hybrid materials high-pressure crystal structure prediction density functional theory planet interior

Recent advances in solving Li_(2)CO_(3) problems in garnet-based solid-state battery: A systematic review(2020-2023)

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Journal of Energy Chemistry 2024年第3期90卷 58-76,I0004页

作者： Shaoxiong Han Ziqi Wang Yue ma Yanlan Zhang Yongzhen Wang Xiaomin Wang College of materials Science and Engineering Taiyuan University of TechnologyTaiyuan 030024ShanxiChina Shanxi Joint Laboratory of Coal based Solid Waste Resource Utilization and green Ecological Development Taiyuan 030024ShanxiChina

garnet solid electrolytes are one of the most promising electrolytes for solid-state ***,Li_(2)CO_(3) is a critical issue that hinders the practical application of garnet-based solid-state lithium-ion *** are two sources of Li_(2)CO_(3) *** main one is the aging of garnet electrolytes in the *** electrolytes can react with H_(2)O and CO_(2) in the air to form Li_(2)CO_(3),which reduces ion conductivity,increases electrode/garnet electrolyte interface resistance,and deteriorates the electrochemical performance of the *** strategies,such as elemental doping,grain boundary manipulation,and interface engineering,have been suggested to address these *** other is the passivation layer(Li_(2)CO_(3),Li_3n,LiOH,Li_(2)O) formed on the surface of the lithium foil after long-term storage,which is ignored by most *** better understand the current strategies and future trends to address the Li_(2)CO_(3) problem,this perspective provides a systematic review of journals published in this field from 2020-2023.

关键词： Solid-state batteries garnet electrolytes Air stability Interface engineering Lithium foil contamination

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Atomically Dispersed Zinc Active Sites Efficiently Promote the Electrochemical Conversion of n_(2) to nH_(3)

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Energy & Environmental materials 2024年第3期7卷 175-181页

作者： Yanjiao Wei Xinyu Wang Mengjie Sun Min ma Jian Tian Minhua Shao School of materials Science and Engineering Shandong University of Science and TechnologyQingdao 266590China Department of Chemical and Biological Engineering The Hong Kong University of Science and TechnologyClear Water BayKowloonHong Kong 999077China Energy Institute and Chinese National Engineering Research Center for Control&Treatment of Heavy Metal PollutionThe Hong Kong University of Science and TechnologyClear Water BayKowloonHong Kong China

At present,the research on highly active and stable nitrogen reduction reaction catalysts is still challenging work for the electrosynthesis of ammonia(nH_(3)).Herein,we synthesized atomically dispersed zinc active sites supported on n-doped carbon nanosheets(Zn/nC nSs)as an efficient nitrogen reduction reaction catalyst,which achieves a high ammonia yield of 46.62μg h^(-1)mg^(-1)_(cat).at-0.85 V(vs RHE)and Faradaic efficiency of 95.8%at-0.70 V(vs RHE).In addition,Zn/nC nSs present great stability and selectivity,and there is no significant change in nH_(3)rate and Faradaic efficiencies after multiple *** structural characterization shows that the active center in the nitrogen reduction reaction process is the Zn-n_(4)sites in the *** calculation confirms that Zn/nC with Zn-n_(4)configuration has a lower energy barrier for the formation of^(*)nnH intermediate compared with pure n-doped carbon nanosheets(n-C nSs),thus promoting the hydrogenation kinetics in the whole nitrogen reduction reaction process.

关键词： electrocatalysis nitrogen reduction single-atom catalyst Zn-n_(4)

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Cross-linkedα-amylase aggregates on Fe3O4 magnetic nanoparticles modified with polydopamine/polyethyleneimine for efficient hydrolysis of starch

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Particuology 2024年第7期90卷 98-105页

作者： Jiandong Cui Xiuming Tang Qingqing ma Yuyan Chang Qunli Zhang Shiru Jia State Key Laboratory of Food nutrition and Safety Laboratory of Industrial Fermentation MicrobiologyMinistry of EducationTianjin University of Science and TechnologyTianjin 300457China Key Laboratory of Biomass Chemical Engineering of Ministry of Education Zhejiang UniversityHangzhou 310027China

In this workα-amylase was immobilized on magnetic Fe3O4 nanoparticles with polyethylenimine(PEI)/polydopamine(PDA)coating or 3-aminopropyl triethoxysilane(APTES)for the first time via adsorption–precipitation–*** with the freeα-amylase,the resultant magnetic cross-linkedα-amylase aggregates(PEI/PDA-M-CLEAs and n-M-CLEAs)exhibited excellent thermal and storage stability as well as pH *** storage at 25°C for 60 days,freeα-amylase only retained 60%of its initial activity,while PEI/PDA-M-CLEAs and n-M-CLEAs retained 80%and 78%of their initial activities,***,n-M-CLEAs and PEI/PDA-M-CLEAs showed good *** 6 repeated uses,PEI/PDA-M-CLEAs and n-M-CLEAs still maintained 65%and 62%of their initial activities,***,PEI/PDA-M-CLEAs and n-M-CLEAs exhibited higher starch hydrolysis efficiency than freeα-*** maximum dextrose equivalent(DE)values of starch hydrolysis by PEI/PDA-M-CLEAs and n-M-CLEAs reached 29.24%and 28.79%within 90 min,***,the maximum DE values of starch hydrolysis by the freeα-amylase was only 27.89%even in 150 *** magnetic cross-linkedα-amylase aggregates could be introduced as effective biocatalyst for industrial applications in production of maltose syrups.

关键词： α-amylase magnetic nanoparticles Functional modification magnetic cross-linked enzyme aggregates Hydrolysis of starch

EFFICIEnT SPECTRAL METHODS FOR EIgEnVALUE PROBLEMS OF THE InTEgRAL FRACTIOnAL LAPLACIAn OnABALLOFAnYDIMEnSIOn

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Journal of Computational mathematics 2024年第4期42卷 1032-1062页

作者： Suna ma Huiyuan Li Zhimin Zhang Hu Chen Lizhen Chen College of Science Nanjing University of Posts and TelecommunicationsNanjingChina State Key Laboratory of Computer Science/Laboratory of Parallel Computing Institute of SoftwareChinese Academy of SciencesBeijingChina Department of mathematics Wayne State UniversityDetroitUSA School of mathematical Sciences Ocean University of ChinaQingdaoChina Beijing Computational Science Research Center BeijingChina

An efficient spectral-galerkin method for eigenvalue problems of the integral fractional Laplacian on a unit ball of any dimension is proposed in this *** symmetric positive definite linear system is retained explicitly which plays an important role in the numerical *** a sharp estimate on the algebraic system's condition number is established which behaves as n4s with respect to the polynomial degree n,where 2s is the fractional derivative *** regularity estimate of solutions to source problems of the fractional Laplacian in arbitrary dimensions is firstly investigated in weighted Sobolev *** the regularity of eigenfunctions of the fractional Laplacian eigenvalue problem is readily ***,rigorous error estimates of the eigenvalues and eigenvectors are *** experiments are presented to demonstrate the accuracy and efficiency and to validate the theoretical results.

关键词： Integral fractional Laplacian Spectral method Eigenvalue problem Regularity analysis Error estimate

Regulating the oxidation state of Pd to enhance the selective hydrogenation for 5-hydroxymethylfurfural

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Chinese Journal of Chemical Engineering 2024年第8期72卷 60-68页

作者： Xin Li Yue ma Xuning Wang Jianguo Wu Dong Cao Daojian Cheng State Key Laboratory of Organic-Inorganic Composites and College of Chemical Engineering Beijing University of Chemical TechnologyBeijing 100029China

The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an important reaction in the field of biomass hydrogenation,because it is a bridge between biomass resources and chemical ***,we precisely constructed carbon nitride supported Pd-based catalysts by a simple impregnation-reduction *** changing the reduction temperature,catalysts with different oxidation state could be precisely ***,the important correlation between the ratio of Pd^(0)/Pd^(2+)and catalytic activity is revealed during the selective hydrogenation of *** Pd/g—C_(3)n_(4)—300 catalyst with a Pd^(0)/Pd^(2+)ratio of 3/2 showed the highest catalytic activity,which could get 96.9%5-hydroxymethylfurfural conversion and 90.3%2,5-dihydroxymethylfuran *** density functional theory calculation revealed that the synergistic effect between Pd0and Pd2+in Pd/g—C_(3)n_(4)—300 system could boost the adsorption of the substrate and the dissociation of *** this work,we highlight the important correlation between metal oxidation state and catalytic activity,which provides valuable insights for the rational design of precious metal catalysts for hydrogenation reactions.

关键词： Pd/g-C_(3)n_(4) Selective hydrogenation 5-hydroxymethylfurfural 2,5-dihydroxymethylfuran Oxidation state

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Effects of Lactobacillus paracasei n1115 on gut microbial imbalance and liver function in patients with hepatitis B-related cirrhosis

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World Journal of gastroenterology 2024年第11期30卷 1556-1571页

作者： Yan-Chao Hu Xiang-Chun Ding Hui-Juan Liu Wan-Long ma Xue-Yan Feng Li-na ma Department of Infectious Disease General Hospital of Ningxia Medical UniversityYinchuan 750004Ningxia Hui Autonomous RegionChina Infectious Disease Clinical Research Center of ningxia Yinchuan 750004Ningxia Hui Autonomous RegionChina

BACKgROUnD Hepatitis B cirrhosis(HBC)is a chronic disease characterized by irreversible diffuse liver damage and aggravated by intestinal microbial imbalance and metabolic *** the relationship between certain single probiotics and HBC has been explored,the impact of the complex ready-to-eat Lactobacillus paracasei n1115(LP n1115)supplement on patients with HBC has not been *** To compare the changes in the microbiota,inflammatory factor levels,and liver function before and after probiotic treatment in HBC *** This study included 160 HBC patients diagnosed at the general Hospital of ningxia Medical University between October 2018 and December *** were randomly divided into an intervention group that received LP n1115 supplementation and routine treatment and a control group that received routine treatment *** samples were collected at the onset and conclusion of the 12-wk intervention *** structure of the intestinal microbiota and the levels of serological indicators,such as liver function and inflammatory factors,were *** Following LP n1115 intervention,the intestinal microbial diversity significantly increased in the intervention group(Pnd the structure of the intestinal microbiota was characterized by an increase in the proportions of probiotic microbes and a reduction in harmful ***,the intervention group demonstrated notable improvements in liver function indices and significantly lower levels of inflammatory factors(PnCLUSIOn LP n1115 is a promising treatment for ameliorating intestinal microbial imbalance in HBC patients by modulating the structure of the intestinal microbiota,improving liver function,and reducing inflammatory factor levels.

关键词： Hepatitis B cirrhosis n1115 ready-to-eat lactobacillus Inflammation Liver function Lachnospiraceae incertae sedis Probiotic

Covalent Organic Framework with Predesigned Single-Ion Traps for Highly Efficient Palladium Recovery from Wastes

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CCS Chemistry 2024年第8期6卷 1908-1919页

作者： Yinghui Xie Qiuyu Rong Caimei Wen Xiaolu Liu Mengjie Hao Zhongshan Chen Hui Yang geoffrey I.n.Waterhouse Shengqian ma Xiangke Wang College of Environmental Science and Engineering North China Electric Power UniversityBeijing 102206 School of Chemical Sciences The University of AucklandAuckland 1142 Department of Chemistry University of North TexasDentonTexas 76201

The recovery of palladium from waste streams is of importance for metal recycling and environmental ***,we present a“single-ion trap”strategy for efficiently recovering Pd(II)from superacidic solutions and laboratory *** was realized by rational design and synthesis of an antiparallel stacked covalent organic framework(ACOF)with hydrazine-carbonyl sites and pyridine sites for cooperative Pd(II)*** single-ion traps provided Lewis base sites with a high Pd(II)binding affinity,enabling the trapping of Pd(II)ions under a wide range of *** developed ACOF-1 adsorbent demonstrated fast kinetics,excellent selectivity,and a high adsorption capacity of 412.9±14.2 mg/g for Pd(II)in a 3M HnO_(3) *** applied in a packed column,ACOF-1 dynamically captured Pd(II)from3M HnO_(3) solutions or laboratorywastes containing trace amounts of palladium and many other metals,realizing extraction efficiencies of 232.9 and 320.9 mg/g,*** experimental and theoretical studies revealed that the single-ion traps offered exceptionally strong binding of Pd(II)under both acidic and high ionic strength conditions,enabling selective adsorptive behavior not accessible using traditional ***,the general design strategy reported here could be used to create porous adsorbents for the capture of other precious metals.

关键词： antiparallel stacking covalent organic frameworks binding affinity selective adsorption Pd(II)recovery

Promoted non-enzymatic glucose Sensor Based on Synergistic Effect of Hydrothermal Synthesized ni(OH)_(2)-graphene nanocomposite

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Chemical Research in Chinese Universities 2024年第5期40卷 914-921页

作者： CAI Yuqing CUI Qingyan ZHAng Huanrong ma Xinlei XUE Mianqi School of Chemistry and Life Resources Renmin University of ChinaBeijing100872P.R.China Technical Institute of Physics and Chemistry Chinese Academy of ScienceBeijing100190P.R.China

Although glucose electrochemical sensors based on enzymes play a dominant role in market,their stability remains a problem due to the inherent nature of ***,glucose sensors that are independent on enzymes have attracted more attention for the development of stable detection *** we present an enzyme-free glucose sensor based on ni(OH)_(2)and reduced graphene oxide(rgO).The as-fabricated sensor still exhibits excellent electrocatalytic activity for detecting glucose under enzyme independent *** enhanced catalytic performance may due to synergistic effect as follows:(i)the interaction between the ni2+andπelectron of graphene induces the formation of theβ-phase ni(OH)_(2)with higher catalytic activity;(ii)the frozen dry process works as a secondary filtration,getting rid of poorly formed ni(OH)_(2)particles with low catalytic activity;(iii)the rgO network with good conductivity provides a good electronic pathway for promoting electron transfer to reduce the response *** on the synergistic effect,the sensor exhibits a wide linear detection range from 0.2µmol/L to 1.0µmol/L and a low detection limit(0.1µmol/L,S/n=3).The excellent detection performance,as well as the easy and low-cost preparation method,suggests the promising applicability of the sensor in the glucose detection market.

关键词： glucose sensing non-enzyme sensor graphene 2D material ni(OH)_(2)nanosheet