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Identifying the dynamic behaviors in complete reconstruction of Co-based complex precatalysts during electrocatalytic oxygen evolution

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Journal of Energy Chemistry 2025年第1期100卷 226-233页

作者： Jingfang Zhang Danyang Wu Linke Cai Youluan Lu Fanpeng Cheng Lijuan Shi Qun Yi Yao Liu Yi Huang key laboratory of green chemical Engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education Hubei Key Laboratory of Novel Reactor and Green Chemical Technology School of Chemical Engineering & Pharmacy Wuhan Institute of Technology key laboratory of Pesticide & chemical Biology of Ministry of Education Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of Education College of Chemistry Central China Normal University College of Materials Science and Engineering Fuzhou University

Transition metal-based nanomaterials have emerged as promising electrocatalysts for oxygen evolution reaction（OER）. Considerable research efforts have shown that self-reconstruction occurs on these nanomaterials under operating conditions of OER process. However, most of them undergo incomplete reconstruction with limited thickness of reconstruction layer, leading to low component utilization and arduous exploration of real catalytic mechanism. Herein, we identify the dynamic behaviors in complete reconstruction of Co-based complexes during OER. The hollow phytic acid（PA） cross-linked CoFe-based complex nanoboxes with porous nanowalls are designed because of their good electrolyte penetration and mass transport ability, in favor of the fast and complete reconstruction. A series of experiment characterizations demonstrate that the reconstruction process includes the fast substitution of PA by OH-to form Co（Fe）(OH)xand subsequent potential-driven oxidation to Co（Fe）OOH. The obtained CoFeOOH delivers a low overpotential of 290 mV at a current density of 10 mA cm-2and a long-term *** experiment results together with theory calculations reveal that the Fe incorporation can result in the electron rearrangement of reconstructed CoFeOOH and optimization of their electronic structure,accounting for the enhanced OER activity. The work provides new insights into complete reconstruction of metal-based complexes during OER and offers guidelines for rational design of high-performance electrocatalysts.

关键词： Oxygen evolution reaction

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Optimal Conditions for Preparing Ultra-Fine CeO_2 Powders in A Submerged Circulative Impinging Stream reactor

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Journal of Rare Earths 2007年第4期25卷 422-427页

作者：池汝安徐志高吴元欣王存文 hubei key laboratory of novel chemical reactor & green chemical technology Wuhan Institute of Technology

Cerium carbonate powders were produced in a submerged circulation impinging stream reactor （SCISR） from Ce（NO3）3· 6H2O. NH4HCO3 was used as a precipitant in the reaction. Cerium carbonate powders were roasted to produce ultra-fine cerium dioxide （CeO2） powders. The optimal conditions of such production process were obtained by orthogonal and one-factor experiments. The results showed that ultra-fine and narrowly distributed cerium carbonate powders were produced under the optimal flowing conditions. The concentrations of Ce（NO3）3 and NH4HCO3 solutions were 02,5 and 0.3 mol · L^-1, respectively. The concentration of PEG4000 added in these two solutions was 4 g · L^-1. The stirring ratio, reaction temperature, feeding time, solution pH, reaction time and digestion time were 900 r · min^- 1,80 ℃, 20 min, 5 - 6, 5 min and 1 h, respectively. The final product, CeO2 powders, was obtained by roasting the produced cerium carbonate in air for 3 h at 500 ℃. The finally produced CeO2 powders were torispherical particles with a narrow size distribution of 0.8 -2.5 μm. The crystal structure of CeO2 powders belonged to cubic crystal system and its space point 5 group was OH^5-FM3M. Under optimal conditions, powders produced by SCISR were finer and more narrowly distributed than that by Stirred Tank reactor （STR）.

关键词： impinging stream reactor cerium dioxide ultra-fine powder rare earths

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A novel Approach to Bioleach Soluble Phosphorus from Rock Phosphate

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过程工程学报 2007年第2期7卷 310-316页

作者：池汝安肖春桥黄晓慧王存文吴元欣 hubei key laboratory of novel chemical reactor and green chemical technology Wuhan Institute of technology

A novel approach to bioleach soluble phosphorus from rock phosphate,involving the bio-oxidation of pyrite by adaptated Acidithiobacillus ferrooxidans(At.f)and the product of sulfuric acid to dissolve rock phosphate,has been proposed in this *** soluble phosphorus could be leached more effectively in the presence of pyrite by At.f than that leached directly by sulfuric *** optimal technological parameters are *** highest phosphorus leaching rate is 9.00% when the culture substrate is the mixture of FeSO_47H_2O and pyrite,the phosphorus leaching rate is 8.00% when the initial pH and culture time are 2.5 and 5 d,*** optimal rock phosphate particle size is 0.05 mm for the leaching of *** bigger the grains of pyrite,the lower the phosphorus leaching *** bacterium At.f should be appropriately adaptated,which makes it easier to bioleach soluble phosphorus from rock phosphate.

关键词：微生物化学生物技术免疫力生物知识

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Correlation analysis on partition of rare earth in ion-exchangeable phase from weathered crust ores

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Transactions of Nonferrous Metals Society of China 2006年第6期7卷 1421-1425页

作者：池汝安戴祖旭徐志高吴元欣王存文 key laboratory of hubei Province for novel chemical reactor and green chemical technology Wuhan Institute of Technology

The rare earth(RE)in weathered crust ores mainly exists as ion-exchangeable phase,approximately 80%.The correlation analysis on partition of 376 samples in ion-exchangeable phase from weathered crust ores was *** results show that partition both among heavy RE elements and light RE elements with high partition appears positive correlation,but partition sums between the heavy RE elements and the light RE elements appear close negative correlation *** negative correlations exist between the light RE elements(except Ce)and yttrium(Y).Matrix of correlation analysis on this partition can be divided into three *** correlated coefficient variation from negative to positive in zones B and C occurs at Gd,so does that in zones B and A(except Ce,Eu,and Sm),suggesting that RE elements can be divided into two groups with Gd as *** phenomenon is called Gadolinium-broken effect.

关键词： weathered crust ore rare earth partition correlation analysis

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Bio-decomposition of rock phosphate containing pyrites by Acidithiobacillus ferrooxidans

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Journal of Central South University of technology 2007年第2期14卷 170-175页

作者：池汝安肖春桥黄晓慧王存文吴元欣 hubei key laboratory of novel chemical reactor and green chemical technology Wuhan Institute of Technology

Leaching soluble phosphorus from rock phosphate containing pyrites by Acidithiobacillus ferrooxidans (A.f.) is feasible, and the reaction mechanism is as follows. Pyrites are oxidized by A.f. to produce H_2SO_4 and FeSO_4; the rock phosphate is decomposed by H_2SO_4, forming soluble phosphorus compounds; and Fe2+ from FeSO_4 is oxidized to Fe^3+, providing energy for the growth of A. f.. In this process, as H_2SO_4 is produced in the reaction, an acidic condition in the culture medium is formed, which benefits the growth of A. f. and aids both continuous oxidation of pyrites and leaching of soluble phosphorus from rock phosphate. The fraction of phosphorous leached can reach the largest in the presence of 1.0 g/L Fe^3+, 200 mg/L Mg^2+ and 400 mg/L NH_4^+. The optimal technological parameters on the fraction of phosphorous leached are as follows: the volume fraction of inocula of A. f., the mass ratio of pyrites to rock phosphate and the pH value are in ranges of 5%-25%, 3:1-5:1 and 1.8-2.2, respectively.

关键词： bio-deeomposition rock phosphate pyrites Acidithiobacillusferrooxidans

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Extend ethylene aromatization single-event kinetic modeling with physical and chemical descriptor based on ZSM-5 catalyst

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Petroleum Science 2023年第6期20卷 3841-3853页

作者： Jia-Rong Xie Fang Jin School of chemical Engineering and Pharmacy Wuhan Institute of TechnologyWuhan430205HubeiChina key laboratory for green chemical Process of Ministry of Education Wuhan Institute of TechnologyWuhan430205HubeiChina novel reactor&green chemical technology key laboratory Wuhan Institute of TechnologyWuhan430205HubeiChina

The ethylene aromatization is critical for the methanol to aromatics and light alkane dehydroaromatization *** single-event microkinetic(SEMK)model combining the linear free energy theory and solid acid distribution concept were established and extend for the ethylene aromatization process,which can reduce the kinetic parameters and simplify the reaction network by comparison with the SEMK model including subtype elementary steps based on the type of carbenium *** introducing deactivation parametersφinto the model and applying the linear free energy model to the deactivation experimental data,the obtained deactivation parametersφindicate that the carbon deposition precursors have the greatest impact on reducing the reaction rate of single-molecular reactions and the smallest impact on the hydrogen transfer ***,according to the change of reaction enthalpy,effect of carbenium ion structure on methylation,ethylation,cyclization and endo-βscission was investigated by introducing linear free energy concept into the SEMK *** effect of different acid strengths on elementary steps was investigated based on the acid strength distribution model,it was found that the methylation and oligomerization reactions,the ali-βscission reaction,endo-βscission reaction and the cyclization reaction were more sensitive to strong acidity *** physisorption and chemisorption heat are separated from the protonation heat in the linear free energy kinetic model and the acid strength distribution kinetic model,and the absolute values of the obtained physisorption and chemisorption heat increase with the carbon number of carbenium ***,the parameters of the acid strength distribution kinetic model were applied to propane dehydroaromatization on H-ZSM-5 and the ethane dehydroaromatization on Zn/ZSM-5 to confirm the independence of parameters in the SEMK model with the similar reaction network.

关键词： Kinetic model Ethylene aromatization Acid strength distribution Linear free energy theory

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Synthesis of Lanthanide Cryptates by Transmetalation Reaction

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Journal of Rare Earths 2005年第S1期23卷 543-546页

作者：胡学雷刘焕胡丹袁军陈中黄齐茂潘志权 hubei key laboratory of novel chemical reactor and green chemical technology Wuhan Institute of Chemical Technology Wuhan 430073 China

New lanthanide cryptates [LnL](ClO_4)_3 (Ln=Eu 3+, Ce 3+, Pr 3+, Sm 3+, Gd 3+, Tb 3+; L=1, 4, 12, 15, 18, 26, 31, 39, 42, 43, 44-undecaazapentacyclo-[13.***.13.1 6, 10.1 20, 24.1 33, 37]-tetratetraconta-4, 6, 8, 10(44), 11, 18, 20, 22, 24(43), 25, 31, 33, 35, 37(42), 38-penta decaene) were synthesized by transmetalation reaction of lanthanide perchlorates with its barium cryptate which was obtained by [2+3] template condensation of tren with 2,6-diformylpyridine in the presence of barium perchlorate, and characterized by elemental analysis, IR and electrospray mass spectrum.

关键词： lanthanide cryptate transmetalation reaction synthesis rare earths

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Effect of nickel oxide morphology on the nitrogen electrochemical reduction reaction

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Nano Materials Science 2020年第4期2卷 353-359页

作者： Ping Zhang Wei Xiong Min Zhou School of Chemistry and Environmental Engineering Key Laboratory for Green Chemical Process(Ministry of Education)Hubei Key Lab of Novel Reactor&Green Chemical TechnologyWuhan Institute of TechnologyLiufang Road 1Wuhan430205China

In order to study the effect of catalysts’morphology on the electrochemical reduction of nitrogen gas,sample catalysts of NiO with four different morphologies(hollow spherical,sea urchin-shape,cubic block,and rod-like)were *** of the NiO catalysts was carried out using SEM,BET,XRD and electrochemical investigation *** results indicated that the nitrogen reduction reaction(NRR)is strictly dependent on the morphology of the NiO catalysts,as the hollow spherical NiO showed the best electrochemical NRR performance of NH3 yield rate(3.21μg h^-1 mg^-1 cat.,4.1910^-11 mol cm^-2 s^-1)and Faradaic efficiency(1.37%),which was higher than the yields and efficiencies of the rod-NiO(1.8μg h^-1 mg^-1 cat.,3.2410^-11 mol cm^-2 s^-1,1.17%),sea urchin-NiO(1.66μg h^-1 mg^-1 cat.,2.4410^-11 mol cm^-2 s^-1,1.08%)and cubic block-NiO(1.32μg h^-1 mg^-1 cat.,2.1410^-11 mol cm^-2 s^-1,0.81%),*** results match the order of the specific surface area of the NiO samples,with hollow spherical(113.91 m^2 g^-1)>rod-NiO(55.12 m^2 g^-1)sea urchin-NiO(55.29 m^2 g^-1)>cubic block-NiO(38.57 m^2 g^-1).This correlation can be attributed to the fact that large specific surface areas can provide more active sites for *** work demonstrates the effect of the morphology of the NiO catalysts on its electrochemical NRR properties,which could offer some opportunity for the preparation of new electrode materials with improved electrocatalytic properties.

关键词： Nickel oxide Morphology structure Electrocatalytic N2 reduction

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Characterization and Luminescence Properties of a New Europium(Ⅲ) Complex with a Macrocyclic Ligand

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Journal of Wuhan University of technology(Materials Science) 2010年第6期25卷 987-990页

作者：吴起峰胡学雷 key laboratory of green chemical Process of Ministry of Education-hubei key laboratory of novel chemical reactor and green chemical technology Wuhan Institute of Technology

The title compound（13,27-dichloro-3,6,9,17,20,23-hexaazatricyclo-[23.***.1.111,15]-triaconta-l（29）,2,9,11,13,15（30）,16,23,25,27-decaene-29,30-diol-N3,N6,N9,O29,O30）-bis（nitrato-O,O）-Europium（Ⅲ） nitrate was prepared and characterized by elemental analysis,infrared spectra,electrospray mass spectrum and X-ray diffraction,*** crystal of the complex crystallizes in the monoclinic system,space group C2/c with a=2.3737（2） nm,b=14.333（1） nm,c=19.388（2） nm,β = 91.804（1）°,Mr= 850.4,V= 6.5929（8） nm3,R= 0.0333,wR= *** room temperature,excitation of the title complex gives rise to the characteristic luminescent emissions of the Eu3＋ ion.

关键词： lanthanide macrocycle crystal structure luminescence

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PARTIAL CARBAMOYLATION OF CELLULOSE MICROSPHERES: A NEW METHOD TO PREPARE ADSORBENTS FOR LIQUID CHROMATOGRAPHY

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Chinese Journal of Polymer Science 2013年第12期31卷 1725-1732页

作者： Wei Chen Qin Bin 柏正武周兴平 Xiao-lin Xie key lab for Large-Format Battery Materials and Systems Ministry of EducationSchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology key lab of green chemical Process Ministry of EducationHubei Key Laboratory of Novel Chemical Reactor and Green Chemical TechnologyWuhan Institute of Technology

Micron-sized cellulose microspheres were prepared through sol-gel method using NaOH/urea solution to dissolve cellulose, then cross-linked by 1,6-hexanylene diisocyanate （HDI）, toluene 2,4-diisocyanate （TDI） and 1,4-phenylene diisocyanate （PDI）, respectively. The reaction conditions for partial modification of the microspheres were studied. The degree of substitution （DS） in cellulose was controlled by adjusting the reaction conditions. HDI-crosslinked microspheres were partially modified with phenyl isocyanate to obtain chiral stationary phases （CSPs）. The CSPs of a lower degree of crosslinking （DC） showed better chiral recognition ability than those of a higher DC. Meanwhile the CSPs prepared by pre- modification exhibited better chiral recognition ability than those prepared by pre-crosslinking.

关键词： Cellulose Microspheres Functionalization Chiral stationary phase Chiral recognition.

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