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Amino acids modified nanoscale zero-valent iron:Density functional theory calculations,experimental synthesis and application in the Fenton-like degradation of organic solvents

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Journal of Environmental Sciences 2024年第1期135卷 296-309页

作者： Xingchen Yang Fucheng Ming jianlong wang Lejin Xu Department of Nuclear Engineering and Technology School of Energy and Power EngineeringHuazhong University of Science and TechnologyWuhan 430074China China-EU Institute for Clean and Renewable Energy Huazhong University of Science and TechnologyWuhan 430074China Institute of Nuclear and New Energy Technology Key Laboratory of Advanced Reactor Engineering and Safety of Ministry of EducationTsinghua UniversityBeijing 100084China Beijing Key Laboratory of Radioactive Wastes Treatment Tsinghua UniversityBeijing 100084China

To improve the adsorption and catalytic performance of heterogeneous Fenton-like catalysts for oil wastes,amino acids were used to modify nanoscale zero-valent iron(AA@Fe^(0)),which were applied in the Fenton-like degradation of organic solvents(tributyl phosphate and n-dodecane,named TBP and DD).Twelve amino acids,i.e.,glycine(Gly),alanine(Ala),leucine(Leu),proline(Pro),phenylalanine(Phe),methionine(Met),cysteine(Cys),asparagine(Asn),serine(Ser),glutamic acid(Glu),lysine(Lys)and arginine(Arg),were selected and calculated by density functional theory(DFT).The optimized structure,charge distribution,the highest occupied molecular orbital(HOMO),the lowest unoccupied molecular orbital(LUMO),interaction region indicator(IRI)isosurface map and adsorption energy of AA@Fe^(0),AA@Fe^(0)-TBP and AA@Fe^(0)-DD were studied,which indicated that Fe is more likely to approach and charge transfer with-COO and-NH_(3) on theα-carbon of amino acids.There is strong attraction between Fe and–COO,and Van der Waals force between Fe and-NH_(3),respectively.In the interaction of AA@Fe^(0)with TBP and DD,Van der Waal force plays an important role.AA@Fe^(0)was synthesized in laboratory and characterized to investigate physicochemical properties.In Fenton-like degradation of organic solvents,the change of COD in water phase during the degradation process as well as the volume of the organic phase after the reaction were investigated.The results of calculations combined with experiments showed that Ser-modified Fe^(0)performed the best in these amino acids,with 98%removal of organic solvents.A possible catalytic mechanism was proposed in which amino acids acted a linking role between Fe and organic solvents,activating H_(2)O_(2)to generate hydroxyl radicals for the degradation of organic solvents.

关键词： Amino acids Nanoscale zero-valent iron Density functional theory Organic solvents Fenton-like degradation

Solubility determination and comparison ofβ-HMX and RDX in two binary mixed solvents(acetonitrile+water,nitric acid+water)

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Chinese Journal of Chemical Engineering 2024年第5期69卷 238-249页

作者： Yuehua Yao Fan wang Yinguang Xu Zishuai Xu Lizhen Chen jianlong wang School of Chemistry and Chemical Engineering North University of ChinaTaiyuan 030051China Gansu Yinguang Chemical Industry Group Co.Ltd. Baiyin 730900China

In order to remove hexahydro-1,3,5-trinitro-1,3,5-triazine(RDX),the main impurity,in process of polymorphic transformation of octrahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine(HMX),the solubility ofβ-HMX and RDX in acetonitrile(ACN)+water in the temperature range of 288.15-333.15 K and in nitric acid(HNO_(3))+water in the temperature range of 298.15-333.15 K were measured by laser dynamic method.The results showed that the solubility of bothβ-HMX and RDX in binary mixed solvents increased monotonously as the temperature increase at a given solvent composition or with increasing of mole fraction of solvent(ACN and nitric acid).Solubility data were well correlated by the modified Apelblat equation,Jouyban-Acree model,Yaws equation and van't Hoff equation,and the Yaws equation achieved the best fitting results according to the relative error and the mean square error root.Furthermore,the solubility ofβ-HMX and RDX in binary mixed solvent was compared,based on the solubility difference and the solvent's own properties,the best separation degree ofβ-HMX and RDX was found when the mole fraction of nitric acid was 0.22 at room temperature,which provided data support for HMX crystallization in mixed solvent.The solubility differences between RDX andβ-HMX in mixed solvents were explained from the formation of intermolecular and intramolecular hydrogen bonds.

关键词： Solubility Octrahydro-1 3 5 7-tetranitro-1 3 5 7-tetrazocine Hexahydro-1 3 5-trinitro-1 3 5-triazine Separation Model Hydrogen bond

Solubility and metastable zone width measurement of 2,4-diaminobenzenesulfonic acid in(H_(2)SO_(4)+H_(2)O)system

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Chinese Journal of Chemical Engineering 2022年第4期35卷 384-391页

作者： Fanfan Shen Lizhen Chen Pengbao Lian jianlong wang Duanlin Cao School of Chemical Engineering and Technology North University of ChinaTaiyuan 030051China

The equilibrium solubility of 2,4-diaminobenzenesulfonic acid and super solubility as well as metastable zone width were measured in(H_(2)SO_(4)+H_(2)O) system by the laser dynamic method at elevate temperature range from 298.15 K to 338.15 K.2,4-Diaminobenzenesulfonic acid solubility dependence on the temperature and solvent composition were correlated by the modified Apelblat equation,(CNIBS)/Redlich-Kister model and Jouyban-Acree model.The correlated results by three correlation models were in good accord with the experimental values according to relative average deviations(RD),root-mean-square deviations(RMSD),and correlation coefficients(R^(2)).The metastable zone width increased with temperature and sulfuric acid content.The dissolution enthalpy,dissolution entropy and the Gibbs energy were calculated from the experimental values,which indicated that dissolution process of the 2,4-diaminobenzenesulfonic acid was endothermic.The solubility and calculation models of 2,4-diaminobenzenesulfonic acid in(sulfuric acid+water)system could provide the basic data to the crystallization and purifying of the 2,4-diaminobenzenesulfonic acid.

关键词： 2 4-Diaminobenzenesulfonic acid Solubility Correlation Metastable zone width

18F-prostate specific membrane antigen positron emission tomography/computerized tomography for lymph node staging in medium/high risk prostate cancer: A systematic review and meta-analysis

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中华医学杂志(英文版) 2024年第8期137卷 2023 Sep 8页

作者： Lv Zhengtong Song Liuqi wang Miao Hou Huimin Li Haodong wang Xuan wang Jianye wang jianlong Liu Ming Beijing 100029 Department of Urology Beijing Hospital National Center of Gerontology Institute of Geriatric Medicine Chinese Academy of Medical Sciences Beijing 100730 China Peking University Fifth School of Clinical Medicine Peking University China-Japan Friendship School of Clinical Medicine

Background: Lymph node staging of prostate cancer (PCa) is important for planning and monitoring of treatment.18F-prostate specific membrane antigen positron emission tomography/computerized tomography (18F-PSMA PET/CT) has several advantages over68Ga-PSMA PET/CT, but its diagnostic value requires further investigation. This meta-analysis focused on establishing the diagnostic utility of18F-PSMA PET/CT for lymph node staging in medium/high-risk PCa.Methods: We searched the EMBASE, PubMed, Cochrane library, and Web of Science databases from inception to October 1, 2022. Prostate cancer,18F, lymph node, PSMA, and PET/CT were used as search terms and the language was limited to English. We additionally performed a manual search using the reference lists of key articles. Patients and study characteristics were extracted and the QUADAS-2 tool was employed to evaluate the quality of included studies. Sensitivity, specificity, the positive and negative likelihood ratio (PLR and NLR), diagnostic odds ratio (DOR), area under the curve (AUC), and 95% confidence interval (CI) were used to evaluate the diagnostic value of18F-PSMA PET/CT. Stata 17 software was employed for calculation and statistical analyses.Results: A total of eight diagnostic tests including 734 individual samples and 6346 lymph nodes were included in this meta-analysis. At the patient level, the results of each consolidated summary were as follows: sensitivity of 0.57 (95% CI 0.39-0.73), specificity of 0.95 (95% CI 0.92-0.97), PLR of 11.2 (95% CI 6.6-19.0), NLR of 0.46 (95% CI 0.31-0.68), DOR of 25 (95% CI 11-54), and AUC of 0.94 (95% CI 0.92-0.96). At the lesion level, the results of each consolidated summary were as follows: sensitivity of 0.40 (95% CI 0.21-0.62), specificity of 0.99 (95% CI 0.95-1.00), PLR of 40.0 (95% CI 9.1-176.3), NLR of 0.61 (95% CI 0.42-0.87), DOR of 66 (95% CI 14-311), and AUC of 0.86 (95% CI 0.83-0.89).Conclusions: 18F-PSMA PET/CT showed moderate sensitivity but high specificity in lymph node staging of medium/high-risk PCa. The

关键词： 18F-PSMA PET/CT Diagnostic test Lymph node Meta-analysis Prostate cancer

Morphology prediction of dihydroxylammonium 5,5'-bistetrazole-1,1'-diolate (TKX-50) crystal in different solvent systems using modified attachment energy model

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Chinese Journal of Chemical Engineering 2023年第1期53卷 181-193页

作者： Fang Chen Tao Zhou Lijie Li Chongwei An Jun Li Duanlin Cao jianlong wang School of Chemical Engineering and Technology North University of ChinaTaiyuan 030051China School of Material Science and Engineering Beijing Institute of TechnologyBeijing 100081China School of Environmental and Safety Engineering North University of ChinaTaiyuan 030051China

In order to theoretically study the growth morphology of dihydroxylammonium 5,5’-bistetrazole-1,1’-dio late(TKX-50)crystal in different solvent systems,crystal–solvent models were established,and then molecular dynamics(MD)methods were adopted as a means to simulate particle motion.Modified attachment energy(MAE)model was employed to calculate the growth morphology of TKX-50.The simulation results demonstrate that COMPASS force field and RESP charge are suitable for molecular dynamics simulation of TKX-50.The morphologically dominant growth surfaces of TKX-50 in vacuum are(020),(011),(11–1),(100)and(120),respectively.In water(H_(2)O)and N,N-dimethylformamide(DMF)solvents,the(11–1)face is the largest in the habit face,the growth rate of(020)face becomes faster.With the increase of temperature,the aspect ratios of TKX-50 crystal in DMF solvent increase,and the areas of the(120)faces decrease.In ethylene glycol/H_(2)O mixed solvent system with volume ratio of 1/1,aspect ratio of TKX-50 is relatively small.In formic acid/H_(2)O mixed solvents with different volume ratios(1/4,1/3,1/2,1/1 and 2/1),aspect ratio of TKX-50 is relatively small when volume ratio is 1/2.

关键词： TKX-50 Crystal morphology Solvents Modified attachment energy model Molecular dynamics simulation

Zfp281 is essential for epiblast maturation through a cell autonomous effect

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Journal of Genetics and Genomics 2022年第1期49卷 85-88页

作者： Ruge Zang Xin Huang Dan Li Hongwei Zhou Shaorong Gao jianlong wang Clinical and Translational Research Center of Shanghai First Maternity and Infant Hospital School of Life Sciences and TechnologyTongji UniversityShanghai 200092China Department of Medicine Columbia Center for Human DevelopmentColumbia Stem Cell InitiativeHerbert Irving Comprehensive Cancer CenterColumbia University Irving Medical CenterNew YorkNY 10032USA

Pluripotency is recognized as a spectrum of cellular states spanning the na?ve pluripotency established in the preimplantation blastocyst and its transition into primed pluripotency in the postimplantation epiblast cells. The exit from pluripotency is followed by the initiation of gastrulation(Brennan et al., 2001;Nichols and Smith, 2009).

关键词： implantation autonomous effect

Crystallization thermodynamics of 2,4(5)-dinitroimidazole in binary solvents

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Chinese Journal of Chemical Engineering 2023年第5期57卷 173-182页

作者： Pengbao Lian Lizhen Chen Dan He Guangyuan Zhang Zishuai Xu jianlong wang School of Chemical Engineering and Technology North University of ChinaTaiyuan 030051China Shanxi North Xingan Chemical Industry Co.Ltd China North Industries Group Corporation LimitedTaiyuan 030008China Gansu Yinguang Chemical Industry Group Co. LtdBaiyin 730900China

2,4(5)-Dinitroimidazole(2,4(5)-DNI)is an important organic intermediate,and itself can also be used for energetic material.In this work,the solubility of 2,4(5)-DNI in(methanol+water,acetonitrile+water,acetone+water)binary solvents were measured by using a dynamic test method from 278.15 K to 323.15 K under 101.1 k Pa.The Jouyban–Acree model,van't Hoff–Jouyban–Acree model,Apelblat–Jouyb an–Acree model,Ma model,and Sun model were used to correlate the experimental data.The values of relative average deviation(RAD)and root-mean-square deviation(RMSD)were very small,indicating that the error between the experimental value and the correlated value was very small.The thermodynamic parameters such as dissolution enthalpy,dissolution entropy and Gibbs energy were calculated based on solubility data.High-purity of 2,4(5)-DNI was efficiently obtained by using cooling and dilution crystallization method.

关键词： 2 4(5)-Dinitroimidazole Solid-liquid equilibrium Solubility model Three thermodynamic parameters Cooling and dilution crystallization

3D fully-enclosed triboelectric nanogenerator with bionic fish-like structure for harvesting hydrokinetic energy

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Nano Research 2022年第6期15卷 5098-5104页

作者： Zhaoxu Jing Jiacheng Zhang jianlong wang Mingkang Zhu Xinxian wang Tinghai Cheng Jianyang Zhu Zhong Lin wang Beijing Institute of Nanoenergy and Nanosystems Chinese Academy of SciencesBeijing 101400China School of Mechatronic Engineering Changchun University of TechnologyChangchunJilin 130012China Institute of Robotics and Intelligent Systems Wuhan University of Science and TechnologyWuhanHubei 430081China CUSTech Institute of Technology WenzhouZhejiang 325024China School of Materials Science and Engineering Georgia Institute of TechnologyAtlantaGA 30332-0245USA

The hydrokinetic energy of river current,as one of the essential and widespread renewable energies,is difficult to be harvested in low flow velocity and shallow water areas.In this work,a three-dimensional(3D)fully-enclosed triboelectric nanogenerator(FETENG)with bionic fish-like structure for harvesting hydrokinetic energy is reported,which is comprised of the triboelectric powergeneration unit,bionic fish-like structure and connection unit.Through the bionic structure,the FE-TENG realizes zero head power generation in shallow water with low flow velocity.What’s more,the effect of external excitations and bionic structures on the electrical performance are systematically studied in this work.The FE-TENG can generate peak power density of 7 and 0.36 W/m^(3)respectively under the simulated swing state with frequency of 1.25 Hz and simulated river current with flow velocity of 0.81 m/s.In practical applications,due to the 3D fully-enclosed design,the FE-TENG immersed in water for 35 days demonstrates excellent immersion durability with undiminished electrical performance.Therefore,the work proposes an efficient method realizing zero head power generation,and provides a good candidate for long-term service in the river current.

关键词： hydrokinetic energy three-dimensional(3D)fully-enclosed design triboelectric nanogenerator bionic fish-like structure zero head power generation water immersion durability

Impact of Lithium-Ion Coordination on Lithium Electrodeposition

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Energy & Environmental Materials 2023年第1期6卷 177-183页

作者： Li Sheng Yanzhou Wu Jiekang Tian Li wang jianlong wang Yaping Tang Hong Xu Xiangming He Institute of Nuclear and New Energy Technology Tsinghua UniversityBeijing 100084China School of Pharmaceutical Sciences Tsinghua UniversityBeijing 100084China Center of Pharmaceutical Technology Tsinghua UniversityBeijing 100084China

The lithium dendrite and parasitic reactions are two major challenges for lithium(Li)metal anode—the most promising anode materials for high-energy-density batteries.In this work,both the dendrite and parasitic reactions that occurred between the liquid electrolyte and Li-metal anode could be largely inhibited by regulating the Li+-solvation structure.The saturated Li+-solvation species exist in commonly used LiPF 6 liquid electrolyte that needs extra energy to desolvation during Li-electrodeposition.Partial solvation induced high-energy state Li-ions would be more energy favorable during the electron-reduction process,dominating the competition with solvent reduction reactions.The Li-symmetric cells that are cycling at higher temperatures show better performance;the cycled lithium metal anode with metallic lustre and the dendrite-free surface is observed.Theoretical calculation and experimental measurements reveal the existence of high-energy state Li+-solvates species,and their concentration increases with temperature.This study provides insight into the Li+-solvation structure and its electrodeposition characteristics.

关键词： Li^(+)-solvates lithium dendrite-free lithium metal anode molecular dynamics parasitic reactions