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Furfural residues derived nitrogen-sulfur co-doped sheet-like carbon: An excellent electrode for dual carbon lithium-ion capacitors

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Green Energy & Environment 2024年第9期9卷 1427-1439页

作者： Xiaoying Guo Yan Qiao Zonglin Yi christian marcus pedersen Yingxiong Wang Xiaodong Tian Peide Han College of Materials Science and Engineering Taiyuan University of TechnologyTaiyuan030024China College of Chemistry Taiyuan University of TechnologyTaiyuan030024China State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan030001China CAS Key Laboratory of Carbon Materials Institute of Coal ChemistryChinese Academy of SciencesTaiyuan030001China University of Chinese Academy of Sciences Beijing100049China Department of Chemistry University of CopenhagenUniversitetsparken 5DK-2100 CopenhagenDenmark

The state-of-the-art lithium-ion capacitors (LICs),consisting of high-capacity battery-type anode and high-rate capacitor-type cathode,can deliver high energy density and large power density when comparing with traditional supercapacitors and lithium-ion batteries,***,the ion kinetics mismatch between cathode and anode leads to unsatisfied cycling lifetime and anode *** efforts have been devoted to solving the abovementioned *** promising strategy is altering high conductive hard carbon anode with excellent structural stability to match with activated carbon cathode,assembling dual-carbon *** this contribution,one-pot in-situ expansion and heteroatom doping strategy was adopted to prepare sheet-like hard carbon,while activated carbon was obtained involving *** persulfate was used as expanding and doping agent *** furfural residues (FR) were served as carbon *** resulting hard carbon (FRNS-HC) and activated carbon (FRNS-AC)show excellent electrochemical performance as negative and positive electrodes in a lithium-ion battery (LIB).To be specific,374.2 m Ah g^(-1)and 123.1 m Ah g^(-1)can be achieved at 0.1 A g^(-1)and 5 A g^(-1)when FRNS-HC was tested as *** combined with a highly porous carbon cathode (S_(BET)=2961 m^(2)g^(-1)) synthesized from the same precursor,the LIC showed high specific energy of147.67 Wh kg^(-1)at approximately 199.93 W kg^(-1),and outstanding cycling life with negligible capacitance fading over 1000 *** study could lead the way for the development of heteroatom-doped porous carbon nanomaterials applied to Li-based energy storage applications.

关键词： Furfural residue Ammonium persulfate Sheet-like carbon Lithium-ion capacitors Hard carbon

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Ternary deep eutectic solvents catalyzed D-glucosamine self-condensation to deoxyfructosazine: NMR study

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Green Energy & Environment 2021年第2期6卷 261-270页

作者： Pengfei Liu christian marcus pedersen Jiaojiao Zhang Rui Liu Zhenzhou Zhang Xianglin Hou Yingxiong Wang Shanxi Engineering Research Center of Biorefinery Instiute of Coal ChemistryChinese Academy of Sciences27 South Taoyucn Road Taiyun030001China Center of Materials Science and Optoeletronics Engineering University of Chinese Academy of SciencesBejing100049China Department of Chemistny University of CopenhagenUniversitetsparken 5DK-2100 CopenhagenDenmark School of Chemical Engineering Zhengzhou University Zhengzhou450001China

Ternary deep eutectic solvents(TDESs) comprising choline chloride(Ch Cl), glycerol and L-arginine were synthesized as catalysts and solvents for the conversion of D-glucosamine(GlcNH_(2)) into deoxyfructosazine(DOF). The interactions between these three components in the prepared TDESs were studied by ^(1)H-,^(35)Cl-NMR spectra and ^(1)H diffusion-ordered spectroscopy(DOSY) measurements. The chemical shift changes of active hydrogen in the ^(1)H-NMR spectra of TDES system and widening of signals in the^(35)Cl-NMR spectra confirmed the hydrogen bonding interaction between the components, which was further supported by the decrease of diffusion coefficients(D) of the TDES components according to ^(1)H DOSY measurements. The influences of reaction temperature and L-arginine content in the TDESs on the yield of DOF were also studied. The experimental results have shown that when the molar ratio of Ch Cl, glycerol, and L-arginine was 1:2:0.1, DOF was the major product with a yield of 22.6% at 90℃ for 120 min. The chemical shift titration indicated that the carboxyl group of L-arginine in the TDES is the catalytical active site, so the mechanism of the catalytic reaction between Glc NH_(2) and the TDES was proposed. Moreover, a reaction intermediate, dihydrofructosazine, was identified in the self-condensation reaction of Glc NH_(2) by an in situ ^(1)H NMR technique.

关键词： Ternary deep eutectic solvents Hydrogen bonding NMR D-glucosamine Deoxyfructosazine

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Characterization of the acidity and basicity of green solvents by NMR techniques

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Magnetic Resonance Letters 2021年第1期1卷 81-88页

作者： Kemeng Shi christian marcus pedersen Hui Chang Jing Shi Yingxiong Wang Yan Qiao Institute of Coal Chemistry Chinese Academy of SciencesTaiyuan030001China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing100049China Department of Chemistry University of CopenhagenDK-2100 CopenhagenDenmark Sinopec Shanghai Petrochemical Co. Ltd.Shanghai200540China

The acidity and basicity of the solvents can influence the reaction outcome notably,and hence the precise measurement of pH is important for ***,not all the pH values of organic solvents can be determined with a classic pH meter *** this research,the acidity and basicity of environmentally friendly green solvents,such as ZnCl_(2) molten salt hydrate,ionic liquids(ILs)and deep eutectic solvents(DESs),were characterized by 31P and 1 H NMR spectroscopy using trimethylphosphine oxide(TMPO)and pyrrole as probe molecules at 298 *** the ZnCl_(2) molten salt hydrate,the acidic strength of the ZnCl_(2) molten salt hydrate increased with the concentration of ZnCl_(2).By using the ^(1)H-pyrrole NMR approach,it was found that the base strength of amino acid-based ILs follows the order:[Ch][Lys]>[Ch][His].

关键词： Green solvents Acidity Basicity ^(31)P-TMPO NMR ^(1)H-pyrrole NMR

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NMR diffusion analysis of catalytic conversion mixtures from lignocellulose biomass using PSYCHE-iDOSY

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Green Energy & Environment 2023年第5期8卷 1409-1416页

作者： Qi Zhao christian marcus pedersen Jiamin Wang Rui Liu Yuanli Zhang Xiuyin Yan Zhenzhou Zhang Xianglin Hou Yingxiong Wang Shanxi Engineering Research Center of Biorefinery Institute of Coal ChemistryChinese Academy of Sciences27 South Taoyuan RoadTaiyuan030001China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing100049China Department of Chemistry University of CopenhagenUniversitetsparken 5DK-2100CopenhagenDenmark School of Chemical Engineering Zhengzhou University Zhengzhou450001China Shanxi Inspection and Testing Center 106 Changzhi RoadTaiyuan030012China

The component analysis and structure characterization of complex mixtures of biomass conversion remain a challenging ***,developing effective and easy to use techniques is ***-ordered NMR spectroscopy(DOSY)is a non-selective and non-invasive method capable of achieving pseudo-separation and structure assignments of individual compounds from biomass mixtures by providing diffusion coefficients(D)of the ***,the conventional 1H DOSY NMR is limited by crowded resonances when analyzing complex mixtures containing similar chemical structure resulting in similar *** we describe the application of an advanced diffusion NMR method,Pure Shift Yielded by CHirp Excitation DOSY(PSYCHE-iDOSY),which can record high-resolution signal diffusion spectra efficiently separating compounds in model and genuine mixture samples from cellulose,hemicellulose and *** sets of isomers(D-glucose/D-fructose/D-mannose and 1,2-/1,5-pentadiol),homologous compounds(ethylene glycol and 1,2-propylene glycol),model compounds of lignin,and a genuine reaction system(furfuryl alcohol hydrogenolysis with ring opening)were successfully separated in the diffusion *** results show that the ultrahigh-resolution DOSY technique is capable of detecting and pseudo-separating the mixture components of C_(5)/C_(6) sugar conversion products and its derivative hydrogenation/hydrogenolysis from lignocellulose biomass.

关键词： Diffusion NMR Pure shift spectroscopy PSYCHE-iDOSY Mixture analysis Biomass

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NMR studies of stock process water and reaction pathways in hydrothermal carbonization of furfural residue

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Green Energy & Environment 2018年第2期3卷 163-171页

作者： Fen Yue christian marcus pedersen Xiuyin Yan Yequn Liu Danlei Xiang Caifang Ning Yingxiong Wang Yan Qiao Institute of Coal Chemistry Chinese Academy of Sciences Institute of Process Engineering Chinese Academy of Sciences Department of Chemistry University of Copenhagen Taiyuan Supervision and Testing Station for Quality of Grain Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University

Hydrothermal carbonization(HTC) is a valuable approach to convert furfural residue(FR) into carbon material. The prepared biochars are usually characterized comprehensively, while the stock process water still remains to be studied in detail. Herein, a NMR study of the main components in stock process water generated at different HTC reaction conditions was reported. Various qualitative and quantitative NMR techniques(~1H and ^(13)C NMR,~1H-~1H COSY and ~1H-^(13)C HSQC etc.) especially 1D selective gradient total correlation spectroscopy(TOCSY NMR) were strategically applied in the analysis of HTC stock process water. Without separation and purification, it was demonstrated that the main detectable compounds are 5-hydroxymethylfurfural, formic acid, methanol, acetic acid, levulinic acid, glycerol, hydroxyacetone and acetaldehyde in this complicate mixture. Furthermore, the relationship between the concentration of major products and the reaction conditions(180-240 ℃ at 8 h, and 1-24 h at 240 ℃) was established. Finally, reasonable reaction pathways for hydrothermal conversion of FR were proposed based on this result and our previously obtained characteristics of biochars. The routine and challenging NMR methods utilized here would be an alternative other than HPLC or GC for biomass conversion research and can be extended to more studies.

关键词： NMR Hydrothermal carbonization Furfural residue Stock process water

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以氧化石墨烯为酸催化剂制备2,5-二甲基-N-苯基吡咯（英文）

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新型炭材料 2017年第2期32卷 160-167页

作者：陈春燕郭晓亚吕广强 christian marcus pedersen 乔岩侯相林王英雄上海大学环境与化学工程学院上海200444 中国科学院山西煤炭化学研究所山西省生物炼制工程技术研究中心山西太原030001 Department of Chemistry University of Copenhagen 中国科学院山西煤炭化学研究所煤转化重点实验室山西太原030001

介绍了氧化石墨烯作为一种高效且可回收的催化剂应用于2,5-己二酮与苯胺通过Paal-Knorr缩合反应合成N-取代吡咯。研究了反应时间、反应温度、溶剂、催化剂用量以及苯胺与2,5-己二酮的摩尔比对2,5-二甲基-N-苯基吡咯收率的影响。通过原... 详细信息

介绍了氧化石墨烯作为一种高效且可回收的催化剂应用于2,5-己二酮与苯胺通过Paal-Knorr缩合反应合成N-取代吡咯。研究了反应时间、反应温度、溶剂、催化剂用量以及苯胺与2,5-己二酮的摩尔比对2,5-二甲基-N-苯基吡咯收率的影响。通过原位核磁技术在分子水平上跟踪了Paal-Knorr缩合的反应过程。结果表明在25℃下通过氧化石墨烯的催化作用反应6 h后吡咯的最大收率可达到90%。氧化石墨烯易回收,且经5次回收使用后还能表现出很好的循环使用性和高催化性能。

关键词：氧化石墨烯 Paal-Knorr 吡咯非均相酸催化原位核磁

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Understanding the interaction mechanism of carbazole/anthracene with N,Ndimethylformamide:NMR study substantiated carbazole separation

Industrial Chemistry & Materials

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Industrial Chemistry & Materials 2023年第2期1卷 240-246页

作者： Hui Cao Mengyu Dou Zexiang Lyu Yingxiong Wang christian marcus pedersen Yan Qiao State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of Sciences27 South Taoyuan RoadTaiyuan 030001China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China Department of Chemistry University of CopenhagenUniversitetsparken 5DK-2100 CopenhagenDenmark

Carbazole and anthracene,two aromatic hydrocarbon components contained in coal tar,are used as essential organic intermediates to synthesize various carbazole derivatives and anthraquinones.N,NDimethylformamide(DMF)is a commonly used solvent to extract carbazole from crude mixtures of carbazole and ***,the interaction between carbazole/anthracene and DMF in the extraction process is still to be fully understood at the molecular *** this work,the intermolecular interaction of carbazole/anthracene with DMF was investigated using various NMR techniques,including 1 H NMR titration,variable temperature NMR spectroscopy(VT-NMR),Nuclear Overhauser Effect Spectroscopy(NOESY),and diffusion-ordered spectroscopy(DOSY).The observed 1 H chemical shift changes of carbazole indicated strong intermolecular hydrogen bonds between carbazole and DMF,which was further supported by the decrease in the molecular self-diffusion coefficients(D)of both carbazole and DMF according to DOSY ***,NOESY experiments revealed that the distance between the aldehydic hydrogen of DMF and the N–H of carbazole was smaller than 5Å.Accordingly,an intermolecular hydrogen bond between carbazole and DMF in the form of CO⋯H–N was *** research increases our knowledge about the separation process of carbazole and anthracene and hence helps improve the methods.

关键词： NMR Carbazole Separation Intermolecular hydrogen bonds.

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Early dynamics in plant community trait responses to a novel, more extreme hydrological gradient

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Journal of Plant Ecology 2019年第2期12卷 327-335页

作者： Andrea Oddershede Cyrille Violle Annette Baattrup-pedersen Jens-christian Svenning christian Damgaard Section for Plant and Insect Ecology Department of BioscienceAarhus UniversityVejlsøvej 25DK-8600 SilkeborgDenmark Section for Ecoinformatics&Biodiversity Department of BioscienceAarhus UniversityNy Munkegade 114DK-8000 Aarhus CDenmark CEFE UMR 5175 CNRS-Universitéde Montpellier-UniversitéPaul-Valéry MontpellierEPHE-1919 route de MendeF-34293 MontpellierCEDEX 5France Section for Stream and Wetland Ecology Department of BioscienceAarhus UniversityVejlsøvej 25DK-8600 SilkeborgDenmark

Aims For temperate regions such as Northern Europe,predicted climate change patterns include an increase in winter precipitation causing increased risk of flooding,whereas periods of droughts will become more frequent in *** aim of this study is to explore vari-ations in plant functional trait distributions along a hydrological gradient spanning from recurrent drought events to recurrent flood-ing-mimicking future precipitation *** The experiment was conducted in a controlled grassland experi-ment over a period of 3 years.A novel and more extreme hydro-logical regime was achieved by manipulating the flow of a nearby stream thereby creating a continuous hydrological gradient from flooding during winter to drought during *** commu-nity responses were recorded along this hydrological ***-weighted trait distribution changes along the gradient were described using null *** functional traits were con-sidered:seed mass,leaf dry matter content(LDMC),leaf area,leaf thickness,specific leaf area(SLA)and *** findings Over time,responses in plant functional traits changed at the community *** the study period consistent changes occurred in the mean trait value of several *** in relatively dry plots became dominated by species with water-conserving life strategies,represented by high seed mass and thick *** contrast,disturbance-resistant species(high leaf dry matter content)became dominant in flooded plots,indicating that persistence to flooding was the most important factor control-ling the functional structure in those ***,a high abundance of small-seeded species in flooded plots likely indicates higher frequency of species with higher dispersal ability through *** conclusion,plant traits are useful for predicting responses to climate change,but abrupt and extreme climate event may cause unexpected responses because they have no analog to previously more sta

关键词： functional diversity trait-environment relationship hydrology extreme events flooding

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Lattice distortion releasing local surface strain on high-entropy alloys

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Nano Research 2022年第6期15卷 4775-4779页

作者： christian M.Clausen Jack K.pedersen Thomas A.A.Batchelor Jan Rossmeisl Department of Chemistry University of Copenhagen2100 KøbenhavnØDenmark

High-entropy alloys(HEAs)have the potential to be a paradigm-shift for rational catalyst discovery but this new type of alloy requires a completely new approach to predict the surface *** addition to the ligand effect perturbing the surface–adsorbate bond,the random configuration of elements in the surface will also induce local strain effects due to the varying radii of neighboring *** modelling of HEA surface reactivity requires an estimate of this effect:To what degree is the adsorption of intermediates on these lattice distorted atomic environments affected by local strain?In this study,more than 3,500 density functional theory(DFT)calculated adsorption energies of*OH and*O adsorbed on the HEAs IrPdPtRhRu and AgAuCuPdPt are statistically analyzed with respect to the lattice constants of the alloys and the surfaces of each individual binding *** is found that the inherent distortion of the lattice structure in HEAs releases the local strain effect on the adsorption energy as the atomic environment surrounding the binding atom(s)settles into a relaxed *** is even observed to be true for clusters of atoms of which the sizes deviate significantly from the atomic environment in which they are *** elucidates an important aspect of binding site interaction with the neighboring atoms and thus constitutes a step towards a more accurate theoretical model of estimating the reactivity of HEA surfaces.

关键词： high-entropy alloys surface reactivity strain effect surface strain electrocatalysis oxygen reduction reaction

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Experimental treatment of pancreatic cancer with two novel histone deacetylase inhibitors

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World Journal of Gastroenterology 2008年第23期14卷 3681-3692页

作者： Martin Haefner Thilo Bluethner Manuel Niederhagen christian Moebius christian Wittekind Joachim Mossner Karel Caca marcus Wiedmann Department of Internal Medicine II University of LeipzigPhilipp-Rosenthal-Str. 27Leipzig 04103Germany Institute of Pathology University of LeipzigLiebigstr. 26Leipzig 04103Germany Department of Surgery II University of LeipzigLiebigstrasse 20aLeipzig 04103Germany Department of Internal Medicine I Klinikum LudwigsburgPosilipostr. 4Ludwigsburg 71640Germany

AIM:To investigate in vitro and in vivo treatment with histone deacetylase inhibitors NVP-LAQ824 and NVP-LBH589 in pancreatic cancer. METHODS:Cell-growth inhibition by NVP-LAQ824 and NVP-LBH589 was studied in vitro in 8 human pancreatic cancer cell lines using the 3-(4,5-dimethylthiazol-2-yl) -2,5-diphenyltetrazolium bromide(MTT) assay. In addition,the anti-tumoral effect of NVP-LBH589 was studied in a chimeric mouse model. Anti-tumoral activity of the drugs was assessed by immunoblotting for p21WAF-1,acH4,cell cycle analysis,TUNEL assay,and immunohistochemistry for MIB-1. RESULTS:In vitro treatment with both compounds significantly suppressed the growth of all cancer cell lines and was associated with hyperacetylation of nucleosomal histone H4,increased expression of p21WAF-1,cell cycle arrest at G2/M-checkpoint,and increased apoptosis. In vivo,NVP-LBH589 alone significantly reduced tumor mass and potentiated the efficacy of gemcitabine. Further analysis of the tumor specimens revealed slightly increased apoptosis and no significant reduction of cell ***:Our findings suggest that NVP-LBH589 and NVP-LAQ824 are active against human pancreatic cancer,although the precise mechanism of in vivo drug action is not yet completely understood. Therefore,further preclinical and clinical studies for the treatment of pancreatic cancer are recommended.

关键词： Histone deacetylase inhibitor Pancreatic cancer NVP-LAQ824 NVP-LBH589

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