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Strategies for improving extraction capacity through preorganization structure:A novel 5,6-bicyclicmalonamide extractant(THPPD)

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Journal of Rare Earths 2024年第4期42卷 768-774页

作者： Miaomiao Zhang Zhen Yang Yuhua Cui Jianhui Su Heng Zhao Chengjin Xu Xiaolei Liu Guoxin Sun Xiujing Peng Yu Cui School of Chemistry and Chemical Engineering University of JinanJinan250022China institute for Smart Materials&Engineering University of JinanJinan250022China Shandong institute for Food and Drug Control Jinan250101China

Rational design of extractant structure to improve the extraction and separation capacity of rare earth elements(REEs)is a long-standing ***,a new strategy was proposed to improve the stability of the chelating structure formed by malonamide and *** stability of the chelating structure is greatly improved by using a double-ring framework structure which makes the two carbonyl groups of malonamide unable to rotate freely and both of them point to the metal ion *** benzyl groups were used to construct the hydrophobicity of the extractant and the organic shell of the extracted ***-pyrrolo-pyridine-dione(THPPD)was designed and *** structure reduces the energy consumed by rotating carbonyl group in the coordination with metal ions and then improves the extraction ability of *** crystal structure was preorganized as expected,with the two carbonyls pointing in a favorable coordination direction to the structural complement of the metal *** extraction behaviors of REEs with THPPD in a nitric acid medium were *** with N,N’-dibenzyl-N,N’-dimethylmalonamide(DBDM-MA)with a chain structure,the extraction capacity of THPPD is 360 times higher than that of DBDM-MA at 5.0 mol/L sodium ***,the binding energy and Gibbs free energy were investigated by density functional theory(DFT)in conjunction with the *** theoretical results show that THPPD has more effective interaction with Pr(NO_(3))3 than *** construction of chelating groups conformation is a worthy direction to improve the coordination ability and even selectivity of extractant.

关键词： Rare earth elements Extraction separation 5,6-bicyclicdiamide extractant

Discovery of controllable high Chern number quantum anomalous Hall state in tetragonal lattice FeSIn

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Chinese Physics B 2024年第6期33卷 504-509页

作者：任小浪张昌文 School of Physics and Technology Institute of SpintronicsUniversity of JinanJinan 250022China

Quantum anomalous Hall(QAH) insulators have excellent properties driven by fancy topological physics, but their practical application is greatly hindered by the observed temperature of liquid nitrogen, and the QAH insulator with high Chern number is conducive to spintronic devices with lower energy consumption. Here, we find that monolayer Fe SIn is a good candidate for realizing the QAH phase;it exhibits a high magnetic transition temperature of 221 K and tunable C = ±2 with respect to magnetization orientation in the y–z plane. After the application of biaxial strain, the magnetic axis shifts from the x–y plane to the z direction, and the effect of the high C and ferromagnetic ground state on the stress is robust. Also, the effect of correlation U on C has been examined. These properties are rooted in the large size of the Fe atom that contributes to ferromagnetic kinetic exchange with neighboring Fe atoms. These findings demonstrate monolayer Fe SIn to be a major template for probing novel QAH devices at higher temperatures.

关键词： high Chern number Weyl semimetals quantum anomalous Hall insulator magnetic transition temperature

Electronic property and topological phase transition in a graphene/CoBr_(2) heterostructure

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Chinese Physics B 2024年第2期33卷 498-505页

作者：秦元秀李胜世纪维霄张昌文 School of Physics and Technology Institute of SpintronicsUniversity of JinanJinan 250022China

Recently,significant experimental advancements in achieving topological phases have been reported in van der Waals(vdW)heterostructures involving ***,using first-principles calculations,we investigate graphene/CoBr_(2)(Gr/CoBr_(2))heterostructures and find that an enhancement of in-plane magnetic anisotropy(IMA)energy in monolayer CoBr_(2) can be accomplished by reducing the interlayer distance of the vdW *** addition,we clarify that the enhancement of IMA energy primarily results from two factors:one is the weakness of the Co-d_(xy) and Co-d_(x^(2)-y^(2)) orbital hybridization and the other is the augmentation of the Co-d_(yz) and Co-d_(z)2 orbital ***,calculation results suggest that the Kosterlitz–Thouless phase transition temperature(TKT)of a 2D XY magnet Gr/CoBr_(2)(23.8 K)is higher than that of a 2D XY monolayer CoBr_(2)(1.35 K).By decreasing the interlayer distances,the proximity effect is more pronounced and band splitting ***,by taking into account spin–orbit coupling,a band gap of approximately 14.3 meV and the quantum anomalous Hall effect(QAHE)are attained by decreasing the interlayer distance by 1.0 *** by the above conclusions,we design a topological field transistor device *** results support that the vdW interlayer distance can be used to modulate the IMA energy and QAHE of materials,providing a pathway for the development of new low-power spintronic devices.

关键词： van der Waals heterostructure in-plane magnetic anisotropy energy quantum anomalous Hall effect

Cascade electrolysis and thermocatalysis: a reliable system for upgrading C1 to C4 hydrocarbons

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Rare Metals 2024年第1期43卷 410-412页

作者： Chao-Yue Sun Wen Li Hai-Qing Wang institute for Advanced Interdisciplinary Research(iAIR) College of Chemistry and Chemical EngineeringUniversity of JinanJinan 250022China

The carbon cycle is important for maintaining a stable climate and carbon balance on Earth. Renewable-electricitydriven upcycling of carbon dioxide (CO_(2)) into value-added multi-carbon molecules is a potentially sus... 详细信息

关键词： cycling hydrocarbons enable

Highly efficient nitrogen fixation over S-scheme heterojunction photocatalysts with enhanced active hydrogen supply

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National Science Review 2024年第5期11卷 315-325页

作者： Tong Bao Yamin Xi Chaoqi Zhang Peiyang Du Yitong Xiang Jiaxin Li Ling Yuan Chengzhong Yu Chao Liu School of Chemistry and Molecular Engineering East China Normal University Australian institute for bioengineering and Nanotechnology The University of Queensland

Photocatalytic N2fixation is a promising strategy for ammonia（NH3） synthesis;however,it suffers from relatively low ammonia yield due to the difficulty in the design of photocatalysts with both high charge transfer efficiency and desirable N2adsorption/activation ***,an S-scheme CoSx/ZnS heterojunction with dual active sites is designed as an efficient N2fixation *** CoSx/ZnS heterojunction exhibits a unique pocket-like nanostructure with small ZnS nanocrystals adhered on a single-hole CoSxhollow *** the heterojunction,the ele ctronic interaction between ZnS and CoSxcreates electron-deficient Zn sites with enhanced N2chemisorption and electron-sufficient Co sites with active hydrogen supply for N2hydrogenation,cooperatively reducing the energy barrier for *** combination with the promoted photogenerated electron-hole separation of the S-scheme heterojunction and facilitated mass transfer by the pocket-like nanostructure,an excellent N2fixation performance with a high NH3yield of 1175.37 μmol g-1h-1is *** study provides new insights into the design of hetero junction photocatalysts for N2fixation.

关键词： photocatalysis nitrogen fixation S-scheme heterojunction active hydrogen ammonia

Unconventional Fluorescent and Multi-responsive Polyethyleneimine with LCST and UCST Behavior:Synthesis,Characterization and Biological Applications

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Chinese Journal of Polymer Science 2024年第6期42卷 826-837页

作者： Feng-Ming Yin Li-Li Wu Shu-Sheng Li Xiao-Na Pan Xiao-Li Zhu Xu-Bao Jiang Xiang Zheng Kong College of Chemistry and Chemical Engineering University of JinanJinan250022China Shandong institute for Product Quality Inspection Jinan250102China College of Chemical Engineering Tianjin UniversityTianjin300072China

Non-aromatic fluorescent and multi-responsive materials,exhibiting inherent fluorescence emission and controlled phase change,have garnered significant attention in recent ***,the underlying interaction between their fluorescent properties and phase transition remains *** this study,we synthesized a series of catalyst-free aza-Michael addition-based polyethyleneimine(RFPEI)materials by reacting polyethyleneimine(PEI)with N-isopropyl acrylamide(NIPAM).The resulting RFPEI was comprehensively characterized,and demonstrated dual-phase transition behavior(LCST and UCST)in water,which could be finely tuned by adjusting its composition or external factors such as ***,upon UV irradiation(365 nm),RFPEI exhibited strong fluorescence *** further investigated the effects of NIPAM grafting percentage to PEI,polymer concentration,and pH on the LCST/UCST and fluorescent properties of RFPEI aqueous ***,we showcased the great potential of RFPEI as a versatile tool for physiological cell imaging,trace detection,and controlled release of *** study presents a novel class of stimuli-responsive fluorescent materials with promising applications in the field of biomedicine.

关键词： Polyethyleneimine Multi-responsiveness Intrinsic fluorescence emission Cell imaging Controlled drug release

Intrinsic valley-polarized quantum anomalous Hall effect in a two-dimensional germanene/MnI_(2) van der Waals heterostructure

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Chinese Physics B 2024年第7期33卷 2-7页

作者：董晓晶张昌文 School of Physics and Technology Institute of SpintronicsUniversity of JinanJinan 250022China School of Physics and Physical Engineering Qufu Normal UniversityQufu 273100China

Valley-polarized quantum anomalous Hall effect(VQAHE), combined nontrivial band topology with valleytronics,is of importance for both fundamental sciences and emerging applications. However, the experimental realization of this property is challenging. Here, by using first-principles calculations and modal analysis, we predict a mechanism of producing VQAHE in two-dimensional ferromagnetic van der Waals germanene/MnI_(2) heterostructure. This heterostructure exhibits both valley anomalous Hall effect and VQAHE due to the joint effects of magnetic exchange effect and spin–orbital coupling with the aid of anomalous Hall conductance and chiral edge state. Moreover interestingly, through the electrical modulation of ferroelectric polarization state in In_(2)Se_(3), the germanene/Mn I_(2)/In_(2)Se_(3) heterostructure can undergo reversible switching from a semiconductor to a metallic behavior. This work offers a guiding advancement for searching for VQAHE in ferromagnetic van der Waals heterostructures and exploiting energy-efficient devices based on the VQAHE.

关键词： valley-polarized quantum anomalous Hall effect ferromagnetic

Effects of operating conditions on iron(hydr)oxides evolution and ciprofloxacin degradation in potassium ferrate-ozone stepwise oxidation system

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Journal of Environmental Sciences 2024年第1期135卷 367-378页

作者： Xiaochen Li Yifan Wang Ning Wang Mei Li Maomao Bai Jingtao Xu Hongbo Wang School of Municipal and Environmental Engineering Shandong Jianzhu UniversityJinan 250101China Resources and Environment Innovation institute Shandong Jianzhu UniversityJinan 250101China

In this study,a stepwise oxidation system of potassium ferrate(K_(2)FeO_(4))combined with ozone(O+3)was used to degrade ciprofloxacin(CIP).The effects of pH and pre-oxidation time of K_(2)FeO_(4) on the evolution of K_(2)FeO_(4) reduction products(iron(hydr)oxides)and CIP degradation were *** was found that in addition to its own oxidation capacity,K_(2)FeO_(4) can also influence the treatment effect of CIP by changing the catalyst *** presence of iron(hydr)oxides effectively enhanced the mineralization rate of CIP by catalyzing *** pH value can influence the content and types of the components with catalytic ozonation effect in iron(hydr)*** K_(2)FeO_(4) pre-oxidation stage can produce more iron(hydr)oxides with catalytic components for subsequent ozonation,but the evolution of iron(hydr)oxides components was influenced by O_(3) *** can also avoid the waste of oxidation capacity owing to the oxidation of iron(hydr)oxides by O_(3) and free *** intermediate degradation products were identified by Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR-MS).Besides,the degradation pathways were *** the degradation products of CIP,the product with broken quinolone ring structure only appeared in the stepwise oxidation system.

关键词： Potassium ferrate reduction products Catalytic ozonation Ciprofloxacin Potassium ferrate pre-oxidation time

Hypomethylation of glycine dehydrogenase promoter in peripheral blood mononuclear cells is a new diagnostic marker of hepatitis B virus-associated hepatocellular carcinoma

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Hepatobiliary & Pancreatic Diseases International 2024年第1期23卷 35-42页

作者： Li-Li Miao Jing-Wen Wang Hui-Hui Liu Shuai Gao Yu-Chen Fan Kai Wang Department of Hepatology Qilu Hospital of Shandong UniversityJinan 250012China Experimental Center Shandong University of Traditional Chinese MedicineJinan 250355China institute of Hepatology Shandong UniversityJinan 250012China

Background: Glycine dehydrogenase(GLDC) plays an important role in the initiation and proliferation of several human cancers. In this study, we aimed to detect the methylation status of GLDC promoter and its diagnostic value for hepatitis B virus-associated hepatocellular carcinoma(HBV-HCC). Methods: We enrolled 197 patients, 111 with HBV-HCC, 51 with chronic hepatitis B(CHB), and 35 healthy controls(HCs). The methylation status of GLDC promoter in peripheral mononuclear cells(PBMCs) was identified by methylation specific polymerase chain reaction(MSP). The mRNA expression was examined using real-time quantitative polymerase chain reaction(q PCR). Results: The methylation frequency of the GLDC promoter was significantly lower in HBV-HCC patients(27.0%) compared to that in CHB patients(68.6%) and HCs(74.3%)( P < 0.001). The methylated group had lower alanine aminotransferase level( P = 0.035) and lower rates of tumor node metastasis(TNM) Ⅲ/Ⅳ( P = 0.043) and T3/T4( P = 0.026). TNM stage was identified to be an independent factor for GLDC promoter methylation. GLDC mRNA levels in CHB patients and HCs were significantly lower than those in HBV-HCC patients( P = 0.022 and P < 0.001, respectively). GLDC mRNA levels were significantly higher in HBV-HCC patients with unmethylated GLDC promoters than those with methylated GLDC promoters( P = 0.003). The diagnostic accuracy of alpha-fetoprotein(AFP) combined with GLDC promoter methylation for HBV-HCC was improved compared with that of AFP alone(AUC: 0.782 vs. 0.630, P < 0.001). In addition, GLDC promoter methylation was an independent predictor for overall survival of HBV-HCC patients( P = 0.038). Conclusions: The methylation frequency of GLDC promoter was lower in PBMCs from HBV-HCC patients than that from patients with CHB and HCs. The combination of AFP and GLDC promoter hypomethylation significantly improved the diagnostic accuracy of HBV-HCC.

关键词： Hepatocellular carcinoma Glycine dehydrogenase DNA methylation Peripheral blood mononuclear cells