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Statistical theory for hydrogen bonding fluid system of A_aD_d type (I): The geometrical phase transition

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science china chemistry 2006年第6期49卷 499-506页

作者： wang haijun1,2, hong xiaozhong3, gu fang1 & ba xinwu1 1. college of chemistry and environment science, hebei university, baoding 071002, china 2. International Center for Materials Physics, Chinese Academy of sciences, Shenyang 110016, china 3. college of Physics science and Technology, hebei university, baoding 071002, china 1. college of chemistry and environment science Hebei University Baoding 071002 China 2. International Center for Materials Physics Chinese Academy of Sciences Shenyang 110016 China 3. college of Physics science and Technology Hebei University Baoding 071002 China

The influence of hydrogen bonds on the physical and chemical properties of hydrogen bonding fluid system of AaDd type is investigated from two viewpoints by the principle of statistical mechanics. In detail, we proposed two new ways that can be used to obtain the equilibrium size distribution of the hydrogen bonding clusters, and derived the analytical expression of a relationship between the hydrogen bonding free energy and hydrogen bonding degree. For the nonlinear hydrogen bonding systems, it is shown that the sol-gel phase transition can take place under proper conditions, which is further proven to be a kind of geometrical phase transition rather than a thermodynamic one. Moreover, several problems associated with the geometrical phase transition and liquid-solid phase transition in nonlinear hydrogen bonding systems are discussed.

关键词： hydrogen bonding fluid, equilibrium free energy, geometrical phase transition.

Statistical theory for hydrogen bonding fluid system of A_aD_d type(II):Properties of hydrogen bonding networks

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science china chemistry 2007年第1期50卷 11-17页

作者： wang haijun hong xiaozhong gu fang ba xinwu college of chemistry and environment science Hebei UniversityBaoding 071002China International Center for Materials Physics Chinese Academy of SciencesShenyang 110016China college of Physics science and Technology Hebei UniversityBaoding 071002China

Making use of the invariant property of the equilibrium size distribution of the hydrogen bonding clus- ters formed in hydrogen bonding system of AaDd type,the analytical expressions of the free energy in pregel and postgel regimes are *** the gel free energy and the scaling behavior of the number of hydrogen bonds in gel phase near the critical point are investigated to give the corre- sponding scaling exponents and scaling ***,some properties of intermolecular and in- tramolecular hydrogen bonds in the system,sol and gel phases are *** a result,the explicit relationship between the number of intramolecular hydrogen bonds and hydrogen bonding degree is obtained.

关键词： hydrogen bonding network gel phase scaling law

NiO@Ni nanoparticles embedded in N-doped carbon for efficient photothermal CO_(2) methanation coupled with H_(2)O splitting

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Nano Research 2024年第4期17卷 2283-2290页

作者： Yun Zhou Peng Zheng fang wang fangna gu Wenqing Xu Qinyang Lu Tingyu Zhu Ziyi Zhong guangwen Xu Fabing Su Institute of Process Engineering Chinese Academy of SciencesBeijing 100190China Key Laboratory on Resources Chemicals and Materials of Ministry of Education Shenyang University of Chemical TechnologyShenyang 110142China Institute of Industrial chemistry and Energy Technology Shenyang University of Chemical TechnologyShenyang 110142China School of Ecology and environment Beijing Technology and Business UniversityBeijing 100048China Beijing Key Laboratory of Enze Biomass Fine Chemicals College of New Materials and Chemical EngineeringBeijing Institute of Petrochemical TechnologyBeijing 102617China International School of Beijing 10 An Hua Street Shunyi DistrictBeijing 100048China Department of Chemical Engineering Guangdong Technion Israel Institute of Technology(GTIIT)Shantou 515063China Technion Israel Institute of Technology(IIT) Haifa32000Israel

Photothermal carbon dioxide(CO_(2))methanation has attracted increasing interest in solar fuel synthesis,which employs the advantages of photocatalytic H_(2)O splitting as a hydrogen source and photothermal catalytic CO_(2) *** work prepared three-dimensional(3D)honeycomb N-doped carbon(NC)loaded with core–shell NiO@Ni nanoparticles generated in situ at 500℃(NiO@Ni/NC-500).Under the photothermal catalysis(200℃,1.5 W/cm^(2)),the CH_(4) evolution rate of NiO@Ni/NC-500 reached 5.5 mmol/(g·h),which is much higher than that of the photocatalysis(0.8 mmol/(g·h))and the thermal catalysis(3.7 mmol/(g·h)).It is found that the generated localized surface plasmon resonance enhances the injection of hot electrons from Ni to NiO,while thermal heating accelerates the thermal motion of radicals,thus generating a strong photo-thermal synergistic effect on the *** CO_(2) reduction to CH_(4) follows the*OCH *** work demonstrates the synergistic effect of NiO@Ni and NC can enhance the catalytic performance of photothermal CO_(2) reduction reaction coupled with water splitting reaction.

关键词： Ni localized surface plasmon resonance photothermal methanation

Restoring cellular calcium homeostasis to rescue ER stress by 1,2-bis(2-aminophenoxy)ethane-N,N,N’,N’-tetraacetic acid acetoxymethyl ester-loaded lipid-mPLGA hybrid-nanoparticles for acute kidney injury therapy

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Chinese Chemical Letters 2024年第3期35卷 337-345页

作者： Jingwen Zhang Jiahui Yan Yanan wang hong Liu Xueping Sun Yuchao gu Liangmin Yu Changcheng Li Jun Wu Zhiyu He Frontiers science Center for Deep Ocean Multispheres and Earth System and Key Laboratory of Marine Chemistry Theory and TechnologyMinistry of EducationOcean University of ChinaQingdao 266100China college of chemistry and Chemical Engineering Ocean University of ChinaQingdao 266100China School of Medicine and Pharmacy Ocean University of ChinaQingdao 266003China Sanya Oceanographic Institution Ocean University of ChinaQingdao 572024China Bioscience and Biomedical Engineering Thrust The Hong Kong University of Science and Technology(Guangzhou)NanshaGuangzhou 511400China Division of Life science The Hong Kong University of Science and TechnologyHong Kong 999077China

Early pathogenesis of ischemia-reperfusion(I/R)-induced acute kidney injury(AKI)is dominated by intracellular calcium overload,which induces oxidative stress,intracellular energy metabolism disorder,inflammatory activation,and a series of pathologic cascaded reactions that are closely intertwined with self-amplifying and interactive feedback loops,ultimately resulting in cell damage and kidney ***,most nanomedicines originate from the perspective of antioxidant stress,which can only quench existing reactive oxide species(ROS)but cannot prevent the continuous production of ROS,resulting in insufficient *** a safe and promising drug,baPTA-AM is hydrolyzed into baPTA by intracellular esterase upon entering cells,which can rapidly chelate with overloaded Ca^(2+),restoring intracellular calcium homeostasis,thus inhibiting ROS regeneration at the ***,we designed a KTP-targeting peptide-modified yolk-shell structure of liposome–poly(ethylene glycol)methyl ether-block-poly(L-lactide-co-glycolic)(mPLGA)hybrid nanoparticles(100 nm),with the characteristics of high encapsulation rate,high colloid stability,facile modification,and prolonged blood circulation *** the ba/mPLGA@Lipo-KTP was targeted to the site of kidney injury,the cholesteryl hemisuccinate(CHEMS)in the phospholipid bilayer,as an acidic cholesterol ester,was protonated in the simulated inflammatory slightly acidic environment(pH 6.5),causing the liposomes to rupture and release the ba/mPLGA nanoparticles,which were then depolymerized by intracellular *** baPTA-AM was diffused and hydrolyzed to produce baPTA,which can rapidly cut off the malignant loop of calcium overload/ROS generation at its source,blocking the endoplasmic reticulum(ER)apoptosis pathway(ATF4–CHOP–bax/Bcl-2,Casp-12–Casp-3)and the inflammatory pathway(TNF-α–NF-κB–IL-6 axes),thus alleviating pathological changes in kidney tissue,thereby inhibiting the expression of renal tubular marker kidney injury mole

关键词： baPTA-AM Calcium overload Acid-responsive AKI ER stress

Spatial Correlation in Typical Binary Polycondensation Systems: An Essential Extension of the Kirkwood-Buff Theory

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Chemical Research in Chinese Universities 2023年第6期39卷 985-991页

作者： gu fang LI Jiangtao hong xiaozhong wang haijun college of chemistry and Materials science Hebei UniversityBaoding 071002P.R.China college of Physical science and Technology Hebei UniversityBaoding 071002P.R.China Chemical Biology Key Laboratory of hebei Province Hebei UniversityBaoding 071002P.R.China Key Laboratory of Medicinal chemistry and Molecular Diagnosis Ministry of EducationHebei UniversityBaoding 071002P.R.China

We present the isothermal susceptibility(XT)for the typical binary polycondensation system of Af-Bg type,and relate XT to the weight-average degree of polymerization in terms of the Kirkwood-Buff(KB)*** investigation is based on a new expression of XT for mixtures,which is still expressed by the KB integrals(KBIs)but endowed with an explicit physical *** polymerization systems,it is proposed that the KBIs can be further decomposed according to whether there exists a bond between particles when conversions(extents of reaction)of functional groups are incorporated into the *** this way,XT is directly decomposed into its relevant components as *** is especially useful to reveal the relationship between local structures and average properties of various polymerization *** a consequence,the effect of polymerization on XT is greatly simplified in comparison with the free energy ***,we have provided a very simple method to carry out some thermodynamic properties of polymerization systems.

关键词： Isothermal compressibility Polycondensation Kirkwood-Buff theory Radial distribution function Spatial correlation

Tuning the exciton binding energy of covalent organic frameworks for efficient photocatalysis

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Chinese Chemical Letters 2024年第2期35卷 577-583页

作者： Zhangjie gu Zhen Shan Yulan wang Jinjian wang Tongtong Liu Xiaoming Li Zhiyang Yu Jian Su Gen Zhang Key Laboratory for Soft chemistry and Functional Materials of Ministry of Education School of Chemistry and Chemical EngineeringNanjing University of Science and TechnologyNanjing 210094China State Key Laboratory of Photocatalysis on Energy and environment College of ChemistryFuzhou UniversityFuzhou 350002China MIIT Key Laboratory of Advanced Display Material and Devices School of Materials Science and EngineeringNanjing University of Science and TechnologyNanjing 210094China Key Laboratory of Preclinical Study for New Drugs of Gansu Province School of Basic Medical SciencesLanzhou UniversityLanzhou 730000China

Owing to the large exciton binding energy(>100 meV)of most organic materials,the process of exciton dissociation into free electrons and holes is seriously hindered,which plays a key role in the photocatalytic *** this study,a series of chalcogen(S,Se)-substituted mesoporous covalent organic frameworks(COFs)have been synthesized for enhanced photocatalytic organic *** measurements indicate that the introduction of semi-metallic Se atom and the enlargement of conjugation degree can not only reduce the exciton binding energy accelerating the charge separation,but also reduce the band gap of *** a result,the COF-NUST-36 with the lowest exciton binding energy(39.5 meV)shows the highest photocatalytic performance for selective oxidation of amines(up to 98%*** 97.5%Sel.).This work provides a feasible method for designing COFs with high photocatalytic activity by adjusting exciton binding energy.

关键词： Covalent organic frameworks Exciton binding energy Atom substitution Extended conjugation Photocatalysis

Is the polydispersity exponent of the hyperbranched polymers the 3/2 or 5/2?

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Chinese science Bulletin 2006年第12期51卷 1526-1528页

作者： ba xinwu LIU Ying wang Sujuan wang haijun college of chemistry and environment science Hebei University Baoding 071002 China Department of chemistry Hebei Normal University of Science and Technology Qinhuangdao 066600 China

The number of the hyperbranched polymers in the system is investigated for the polymerization process to give the asymptotic form of the concentration of the n-mer. The polydispersity exponent is calculated, which coincides with that of the classical result. Finally, the asymptotic forms of the number, the weight and the z-average degrees of the polymerization were evaluated analytically to obtain polydispersity index, which is close to 1 as the reaction is quantitatively completed.

关键词：超分支聚合体多分散指数聚合过程渐近形式

Statistical and thermodynamic properties of binary self-condensing vinyl polymerization

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science china chemistry 2011年第3期54卷 438-445页

作者： gu fang wang haijun ZHAO ZuoFei college of chemistry and environment science Hebei University Baoding 071002 China International Centre for Materials Physics Chinese Academy of Sciences Shenyang 110016 China Key Laboratory of Medicinal chemistry and Molecular Diagnosis Ministry of Education hebei university Baoding 071002 China

The thermodynamic properties of a binary self-condensing vinyl polymerization system consisting of monomers and inimers are investigated by the principle of statistical *** detail,in terms of two types of canonical partition functions constructed from different viewpoints,the equilibrium free energy,the law of mass action and the size distribution of hyperbranched polymers are *** an application,the specific heat,equation of state and isothermal compressibility concerning the polymerization are given as *** study the dimension of hyperbranched polymers in the system,a recursion formula satisfied by the(k+1)-th and k-th mean square radius of gyration is derived,and then the first,second and third radius of gyration under different solvent conditions are *** influences of the fraction of inimers,the conversion of vinyl groups and the solvent effect on the average dimension of hyperbranched polymers are discussed.

关键词： self-condensing vinyl polymerization law of mass action mean square radius of gyration solvent effect

Dynamic tracking of exsolved PdPt alloy/perovskite catalyst for efficient lean methane oxidation

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Chinese Chemical Letters 2024年第4期35卷 170-175页

作者： Yanling Yang Zhenfa Ding Huimin wang Jianhui Li Yanping Zheng hongquan guo Li Zhang Bing Yang Qingqing gu Haifeng Xiong Yifei Sun college of Energy Xiamen UniversityXiamen 361005China School of environment and Civil Engineering Dongguan University of TechnologyDongguan 523808China Department of chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China State Key Laboratory of Physical chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China CAS Key Laboratory of science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China Innovation Laboratory for sciences and Technologies of Energy Materials of Fujian Province(IKKEM) Xiamen 361102China

Supported Pd based catalysts are considered as the efficient candidates for low-carbon alkane oxidation for their outstanding capability to break C-H bond. Whereas, the irreversible deactivation of Pd based catalysts was still frequently observed. Herein, we reinforced the extruded Pd nanoparticles with quantitive Pt to assemble the evenly distributed Pd Pt nanoalloy onto ferrite perovskite(Pd Pt-LCF) matrix with strengthened robustness of metal/oxide support interface. We further co-achieved the enhanced performance, anti-overoxidation as well as resistance of vapor-poisoning in durability measurement. The operando X-ray photoelectron spectroscopy(O-XPS) combined with various morphology characterizations confirms that the accumulation of surface deep-oxidation species of Pd^(4+) is the culprit for fast activity loss in exsolved Pd system, especially at high temperature of 400 ℃. Conversely, it could be completely suppressed by in-situ alloying Pd with equal amount of Pt, which helps maintain the metastable Pd^(2+)/Pd shell and metallic solid-solution core structure. The density function theory(DFT) calculations further buttress that the dissociation of C–H was facilitated on alloy/perovskite interface which is, on the contrary, resistant toward O–H bond cleavage, as compared to Pd/perovskite. Our work suggests that the modification of exsolved metal/oxide catalytic interface could further enrich the toolkit of heterogeneous catalyst design.

关键词： Exsolution PdPt alloy Operando characterization Methane conversion Deep-oxidation