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green Energy & Environment 2020年第1期5卷 69-75页

作者： Zhiwei Lu Xiaochao Xu Yujuan Chen Xiaohui Wang Li Sun Kelei Zhuo collaborative innovation Center of henan Province for green manufacturing of fine chemicals Key Laboratory of Green Chemical Media and ReactionsMinistry of Education School of Chemistry and Chemical Engineering Henan Normal University

Supercapacitors with unique performance have been widely utilized in many fields. Herein, we report a nitrogen and sulfur co-doped graphene aerogel(N/S-GA-2) prepared using a low toxic precursor for high-performance supercapacitors. The as-obtained material possesses a hierarchically porous structure and a large number of electrochemical active sites. At a current density of 1 Ag^-1, the specific capacitance of the N/S-GA-2 for supercapacitors with the ionic liquid as the electrolyte is 169.4 Fg^-1, and the corresponding energy density is 84.5 Wh kg^-*** a power density of 8.9 k W kg^-1, the energy density can reach up to 75.7 Wh kg^-1, showing that the N/S-GA-2 has an excellent electrochemical performance. Consequently, the N/S-GA-2 can be used as a promising candidate of electrode materials for supercapacitors with high power density and high energy density.

关键词： Graphene aerogel Hierarchically porous structure Supercapacitor Ionic liquid

Nitrogen-doped porous carbon nanosheets as both anode and cathode for advanced potassium-ion hybrid capacitors

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green Energy & Environment 2023年第2期8卷 579-588页

作者： Quanzhou Du Yuhua Zhao Yujuan Chen Jianming Liu Huanhuan Li Guangyue Bai Kelei Zhuo Jianji Wang collaborative innovation Center of henan Province for green manufacturing of fine chemicals Key Laboratory of Green Chemical Media and ReactionsMinistry of EducationSchool of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiangHenan453007China

Potassium-ion hybrid capacitors(PIHCs)as a burgeoning research hotspot are an ideal replacement for lithium-ion hybrid capacitors(LIHCs).Here,we report nitrogen-doped porous carbon nanosheets(NPCNs)with enlarged interlayer spacing,abundant defects,and favorable mesoporous *** structural changes of NPCNs in potassiation and depotassiation processes are analyzed by using Raman spectroscopy and transmission electron *** to the unique structure of NPCNs,the PIHC device assembled using NPCNs as both the anode and cathode material(double-functional self-matching material)exhibits a superior energy density of 128 Wh kg^(-1)with a capacity retention of 90.8%after 9000 *** research can promote the development of double-functional self-matching materials for hybrid energy storage devices with ultra-high performance.

关键词： Potassium-ion Porous carbon Hybrid capacitor Energy storage Nitrogen-doping

Anionic structural effect in liquid–liquid separation of phenol from model oil by choline carboxylate ionic liquids

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green Energy & Environment 2019年第2期4卷 131-138页

作者： Zhiyong Li Ruipeng Li Xiaoqing Yuan Yuanchao Pei Yuling Zhao Huiyong Wang Jianji Wang collaborative innovation Center of henan Province for green manufacturing of fine chemicals Key Laboratory of Green Chemical Media and ReactionsMinistry of Education School of Chemistry and Chemical Engineering Henan Normal University henan Key Laboratory of green Chemistry Henan Normal University

Phenolic compounds exist in crude oil as pollutants, and their removal is vital important for the refining and further application of oils. In traditional separation approaches, strong acid and strong base have to be used to remove these compounds, which may cause serious environmental problems. In this work, 19 kinds of cholinium ionic liquids have been developed to separate phenol from model oil by liquid–liquid extraction. Structural effect of anions of the ionic liquids in the separation is systematically investigated. It is found that depending on the chemical structure of ionic liquids, phenol can be removed from toluene with single-step removal efficiency from 86 to 99% under optimal conditions. The type of substituent groups and the-CH_2 number between two carboxylates have obvious effect on the removal efficiency, and more hydrophilic ionic liquids have a stronger extraction performance for phenol. Furthermore, thermodynamic,^(13) C NMR,~1 H NMR and density functional theory calculations have been performed to characterize the extraction process and to understand the extraction mechanism. It is shown that the extraction of phenol from oil to ionic liquid is a favorable process, and this process is mainly driven by enthalpy change. The formation of the hydrogen bond between anion of the ionic liquid and-OH of phenol is the main driving force for the extraction of phenol from oil to the ionic liquids.

关键词： Ionic liquid Extraction Phenol Choline Hydrogen bonding

Core-shell Prussian blue analogues derived from metal-organic frameworks as efficient electrocatalysts for oxygen evolution reaction

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Nano Research 2023年第3期16卷 3695-3702页

作者： Qing Zhang Hongyan Wang Wenjie Han Lin Yang Yan Zhang Zhengyu Bai collaborative innovation Center of henan Province for green manufacturing of fine chemicals Key Laboratory of Green Chemical Media and ReactionsMinistry of EducationSchool of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiang 453007China

Developing high-performance and low-cost electrocatalysts for oxygen evolution reaction(OER)is still a great challenge for water-splitting ***,an innovative metal-organic frameworks(MOFs)hybrid-assisted strategy is reported to synthesize core-shell Co/Mn-ZIF@Fe-Co-Mn Prussian blue analogues(PBAs)toward highly efficient OER electrocatalysts in alkaline *** characterization indicates that the amorphous hydroxide transformed from Co/Mn-ZIF@Fe-Co-Mn PBA(ZIF:zeolitic imidazolate frameworks)during the electrochemical process acted as the electroactive *** from these structural and compositional features,the developed composite delivers a remarkably low overpotential of 270 mV with a current density of 10 mA·cm^(−2)in 1.0 M KOH ***,water splitting is catalyzed to reach a current density of 10 mA·cm^(−2)at 1.62 V.

关键词： core-shell structure metal-organic framework Prussian blue analogues amorphous hydroxide oxygen evolution reaction

Tunable LCST-type phase behavior of [FeCl4]--based ionic liquids in water

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Science China Chemistry 2016年第5期59卷 587-593页

作者： Yuanchao Pei Yuan Cao Yanjie Huang Xinxin Song Huiyong Wang Yuling Zhao Jianji Wang collaborative innovation Center of henan Province for green manufacturing of fine chemicals Key Laboratory of Green Chemical Media and ReactionsMinistry of EducationSchool of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiang 453007China

In this work, 16 kinds of [FeCl4]--based magnetic ionic liquids （ILs） with different cation structures have been designed and synthesized, and their structures are characterized by IR and Raman spectroscopy. Then the lower critical solution temperature （LCST）-type phase behavior of these magnetic ILs in water is investigated as a function of concentration. It is shown that cat- ion structure, alkyl chain length and molar ratio of FeCl3/chloride IL have a significant influence on the LCST of the mixtures. The phase separation temperature can be tuned efficiently by these factors. Meanwhile, the LCST-type phase separation pro- cess is also investigated by dynamic light scattering. The results support the mechanism that the hydrogen bonds of the [Fefl4]- anion with water have been gradually disrupted to form ILs aggregates with increasing temperature. In addition, the stability of the ILs in water is also examined in some details. These LCST-type phase separation systems may have potential applications in extraction and separation techniques at room temperature.

关键词： magnetic ionic liquids IR and Raman spectroscopy lower critical solution temperature tunable phase separation

Photocatalytic Transition-Metal-Free Direct 3-Acetalation of Quinoxaline-2(1H)-ones

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Chinese Journal of Chemistry 2022年第22期40卷 2655-2662页

作者： Chunhua Ma Hui Meng Jing Li Xianguang Yang Yuqin Jiang Bing Yu collaborative innovation centre of henan provincefor green manufacturing of fine chemicals Key Laboratory of Green Chemical Media and ReactionsMinistry of EducationHenan Engineering Research Centre of Chiral Hydroxyl PharmaceuticalHenan Engineering Laboratoryof Chemical Pharmaceutical and Biomedical MaterialsSchool of Chemistry and Chemical EngineeringHenanNormal UniversityXinxiangHenan453007China green Catalysis centre College of ChemistryZhengzhou UniversityZhengzhouHenan 45001China

A general transition-metal-free visible-light-promoted 3-acetalation reaction of quinoxaline-2(1H)-ones was developed under mild *** employing 1,2,3,5-tetrakis(carbazol-9-yl)-4,6-dicyanobenzene(4CzIPN)as an inexpensive photocatalyst,and glyoxylic acid acetal as a radical source,various acetalated quinoxaline-2(1H)-ones were constructed in moderate to good ***,the versatility of this protocol is highlighted by the successful application in the late-stage modification of drug molecules and the various functionality *** excellent antitumor activity of the acetalated product demonstrated that this streamlined and sustainable approach could have emerged as a powerful strategy for structural modification in medicinal chemistry.

关键词： Photocatalysis Transition-metal-free Synthetic methods Radical reactions Antitumor activity

Hydrogen bonding mediated ion pairs of some aprotic ionic liquids and their structural transition in aqueous solution

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Science China Chemistry 2017年第7期60卷 970-978页

作者： Huiyong Wang Miao Liu Yuling Zhao Xiaopeng Xuan Yang Zhao Jianji Wang collaborative innovation Center of henan Province for green manufacturing of fine chemicals School of Chemistry and Chemical EngineeringKey Laboratory of Green Chemical Media and ReactionsMinistry qf EdueationHenan Normal UniversityXinxiang 453007China

Ion pair speciation of ionic liquids(ILs) has an important effect on the physical and chemical properties of ILs and recognition of the structure of ion pairs in solution is essential. It has been reported that ion pairs of some ILs can be formed by hydrogen bonding interactions between cations and anions of them. Considering the fact that far-IR(FIR) spectroscopy is a powerful tool in indicating the intermolecular and intramolecular hydrogen bonding, in this work, this spectroscopic technique has been combined with molecular dynamic(MD) simulation and nuclear magnetic resonance hydrogen spectroscopy(~1H NMR) to investigate ion pairs of aprotic ILs [Bmim][NO_3], [BuPy][NO_3], [Pyr_(14)][NO_3], [PP_(14)][NO_3] and [Bu-choline][NO_3] in aqueous IL mixtures. The FIR spectra have been assigned with the aid of density functional theory(DFT) calculations, and the results are used to understand the effect of cationic nature on the structure of ion pairs. It is found that contact ion pairs formed in the neat aprotic ILs by hydrogen bonding interactions between cation and anion, were still maintained in aqueous solutions up to high water mole fraction(say 0.80 for [BuPy][NO3]). When water content was increased to a critical mole fraction of water(say 0.83 for [BuPy][NO3]), the contact ion pairs could be transformed into solvent-separated ion pairs due to the formation of the hydrogen bonding between ions and water. With the further dilution of the aqueous ILs solution, the solvent-separated ion pairs was finally turned into free cations and free anions(fully hydrated cations or anions). The concentrations of the ILs at which the contact ion pairs were transformed into solvent-separated ion pairs and solvent-separated ion pairs were transformed into free ions(fully hydrated ion) were dependent on the cationic structures. These information provides direct spectral evidence for ion pair structures of the aprotic ILs in aqueous solution. MD simulation and ~1H NMR results support

关键词： ionic liquids ion pair hydrogen bonding far infrared spectroscopy solution

Synthesis of 5-functionalized-1,2,3-triazoles via a one-pot aerobic oxidative coupling reaction of alkynes and azides

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Chinese Chemical Letters 2014年第8期25卷 1161-1164页

作者： Ling-Jun Li Yu-Qin Zhang Yang Zhang An-Lian Zhu Gui-Sheng Zhang School of Chemistry and Chemical Engineering Key Laboratory of Green Chemical Media and Reactions Ministry of EducationCollaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals Henan Normal University

In this paper, an efficient synthesis of 5-alkynyl-1,2,3-triazoles through a one-pot aerobic oxidative coupling reaction of various alkynes and azides has been developed. Further derivatization of 5-alkynyl-1,2,3-triazoles readily yielded 5-carbonyl-1,2,3-triazoles, 5-carboxylic-1,2,3-triazole, 5-hydroxyalkyl-1,2,3-triazoles and 5-quinoxaline-1,2,3-triazole, which provided an entry into structurally diverse 5-functionalized-1,2,3-triazoles.

关键词： Alkyne Azide 1,2,3-Triazole Copper catalysis

Synthesis of[60]Fullerene-Fused Allylbenzofurans via Palladium-Catalyzed Migration Reaction

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Chinese Journal of Chemistry 2023年第14期41卷 1733-1739页

作者： Tong-Xin Liu Panting Yang Nana Ma Xiaojun Li Xin Wang Jinliang Ma Guisheng Zhang collaborative innovation Center of henan Province for green manufacturing of fine chemicals Key Laboratory of Green Chemical Media and ReactionsMinistry of EducationSchool of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiangHenan453007 China

Chemical functionalization of fullerenes has been an important topic in fullerene chemistry. Herein, an unprecedented Pd-catalyzed migration reaction of [60]fullerene with allyloxy-tethered aryl iodides is present for the preparation of novel [60]fullerene-fused allylbenzofurans. The use of 1,2-bis(diphenylphosphino)benzene (DPPBz) as a ligand is crucial for the success of the transformation. The reaction shows high chemo- and regioselectivity, and is flexible with regard to allyl-migration site, providing a new and efficient approach to rare [60]fullerene-fused benzofurans. Control experiments disclose that the reaction most probably undergoes a sequential C—O bond cleavage/allyl-migration/intermolecular cycloaddition cascade process.

关键词： Fullerenes Transition-metal catalysis Cross-coupling Cycloaddition Oxygen heterocycles

Rh(Ⅲ)-Catalyzed Diverse C-H Functionalization of Iminopyridinium Ylides

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Chinese Journal of Chemistry 2021年第9期39卷 2489-2494页

作者： Zhenzhen Dong Pengfei Li Xingwei Li Bingxian Liu NMPA Key Laboratory for Research and Evaluation of Innovative Drug Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine ChemicalsSchool of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiangHenan 453007China

Divergent synthesis of useful skeletons has been realized via rhodium(Ⅲ)-catalyzed C-H activation of iminopyridinium ylides and coupling with various unsaturated coupling *** and isoquinolones were obtained via cleavage of the C-N or N-N bond in the ylidic di recti ng group,while fluorinated alkenes were delivered with the di recti ng group in *** reactions occurred with wide substrate scopes and good efficiency under redox-neutral and air-tolerant *** products exhibit solid-state fluoresce nt property and bioactivity of in hibiti on toward huma n cancer cells.

关键词： C-H functionalization Iminopyridinium ylide Diverse transformation Redox-neutral Ylidic directing group