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Catalytically generated noncovalent ammonium dienolate:a versatile platform for the development of organocatalytic asymmetric cascade reactions

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Science China chem.stry 2024年第8期67卷 2524-2546页

作者： Jun-Bing Lin Dong-Sheng Ji Peng-Fei Xu State Key Laboratory of Applied Organic chem.stry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China Shaanxi Key Laboratory of chemical Reaction Engineering College of Chemistry and Chemical EngineeringYan’an UniversityYan’an 716000China

Organocatalytic cascade reactions represent a powerful strategy for the rapid construction of complex chiral molecules with multiple stereocenters from simple substrates under mild conditions. The intriguing structural feature and diverse reactivity of catalytically generated dienolate species render them competent and versatile intermediates for the development of practical and valuable cascade reactions. Over the past years, a plethora of innovative and pioneering noncovalent ammonium dienolatemediated cascade reactions have been designed and implemented under the catalysis of chiral organocatalysts, making dienolate activation a general, robust, and complementary method for the functionalization of unsaturated carbonyl compounds and related substances. This review illustrates the recent advances in organocatalytic noncovalent ammonium dienolate-mediated cascade reactions(mainly from 2010 to 2023), including the cascade transformations of ammonium dienolates directly generated from unsaturated ketone/aldehyde, ester/lactone/azlactone, amide/lactam/pyrazolone/oxindole, and alkylidene nitrile compounds. The contents are arranged based on the reaction types of the ammonium dienolates, with an emphasis on cascade 2,5-, 3,5-, and 4,5-difunctionalizations of these intermediates. Furthermore, other cascade reactions involving the 1,3-, 2,3-, and even more complex 3,4,5-reactivities of ammonium dienolates were also discussed. The reaction pathway, reaction stereoinduction, and synthetic applications of the ammonium dienolate-mediated cascade reactions were highlighted throughout the article. As a stimulating and ever-growing research area, the organocatalytic noncovalent ammonium dienolate-mediated cascade reactions are expected to continue demonstrating their magic power for constructing chiral targets in the future and further expanding the boundaries of asymmetric catalysis.

关键词： organocatalysis asymmetric catalysis ammonium dienolate cascade reaction difunctionalization

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Towards carbon neutrality of calcium carbide-based acetylene production with sustainable biomass resources

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Green Energy & Environment 2024年第6期9卷 1068-1078页

作者： Peng Jiang Guanhan Zhao Hao Zhang Tuo Ji Liwen Mu Xiaohua Lu Jiahua Zhu State Key Laboratory of Materials-oriented chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing211816China

Acetylene is produced from the reaction between calcium carbide(CaC_(2))and water,while the production of CaC_(2) generates significant amount of carbon dioxide not only because it is an energy-intensive process but also the raw material for CaC_(2) synthesis is from ***,a comprehensive biomass-to-acetylene process was constructed that integrated several units including biomass pyrolysis,oxygen-thermal CaC_(2) fabrication and calcium *** comparison,a coal-to-acetylene process was also established by using coal as *** carbon efficiency,energy efficiency and environmental impacts of the bio-based calcium carbide acetylene(BCCA)and coal-based calcium carbide acetylene(CCCA)processes were systematically ***,the environmental impacts were further evaluated by applying thermal integration at system level and energy substitution in CaC_(2) *** though the BCCA process showed lower carbon efficiency and energy efficiency than that of the CCCA process,life cycle assessment demonstrated the BCCA(1.873 kgCO_(2eq) kg-prod^(-1))a lower carbon footprint process which is 0.366 kgCO_(2eq) kg-prod^(-1) lower compared to the CCCA *** sustainable energy(biomass power)substitution in CaC_(2) furnace,an even lower GWP value of 1.377 kgCO_(2eq) kg-prod^(-1) can be achieved in BCCA *** work performed a systematic analysis on integrating biomass into industrial acetylene production,and revealed the positive role of biomass as raw material(carbon)and energy supplier.

关键词： Biomass pyrolysis CO_(2)mitigation Calcium carbide Acetylene Calcium loop

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Regulating the oxidation state of Pd to enhance the selective hydrogenation for 5-hydroxymethylfurfural

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Chinese Journal of chemical Engineering 2024年第8期72卷 60-68页

作者： Xin Li Yue Ma Xuning Wang Jianguo Wu Dong Cao Daojian Cheng State Key Laboratory of Organic-Inorganic Composites and college of chemical Engineering Beijing University of Chemical TechnologyBeijing 100029China

The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an important reaction in the field of biomass hydrogenation,because it is a bridge between biomass resources and chemical ***,we precisely constructed carbon nitride supported Pd-based catalysts by a simple impregnation-reduction *** changing the reduction temperature,catalysts with different oxidation state could be precisely ***,the important correlation between the ratio of Pd^(0)/Pd^(2+)and catalytic activity is revealed during the selective hydrogenation of *** Pd/g—C_(3)N_(4)—300 catalyst with a Pd^(0)/Pd^(2+)ratio of 3/2 showed the highest catalytic activity,which could get 96.9%5-hydroxymethylfurfural conversion and 90.3%2,5-dihydroxymethylfuran *** density functional theory calculation revealed that the synergistic effect between Pd0and Pd2+in Pd/g—C_(3)N_(4)—300 system could boost the adsorption of the substrate and the dissociation of *** this work,we highlight the important correlation between metal oxidation state and catalytic activity,which provides valuable insights for the rational design of precious metal catalysts for hydrogenation reactions.

关键词： Pd/g-C_(3)N_(4) Selective hydrogenation 5-hydroxymethylfurfural 2,5-dihydroxymethylfuran Oxidation state

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Enabling heterogeneous catalysis to achieve carbon neutrality: Directional catalytic conversion of CO_(2) into carboxylic acids

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Carbon Energy 2024年第3期6卷 1-35页

作者： Xiaofei Zhang Wenhuan Huang Le Yu Max García-Melchor Dingsheng Wang Linjie Zhi Huabin Zhang KAUST Catalysis Center(KCC) King Abdullah University of Science and Technology(KAUST)ThuwalSaudi Arabia Key Laboratory of chemical Additives for China National Light industry College of Chemistry and Chemical EngineeringShaanxi University of Science and TechnologyXi'anChina State Key Lab of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijingChina School of chem.stry CRANN and AMBERResearch CentresTrinity College DublinCollege GreenDublinIreland Department of chem.stry Tsinghua UniversityBeijingChina Advanced chemical Engineering and Energy Materials Research Center China University of Petroleum(East China)QingdaoChina

The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon *** to the core goal of achieving carbon neutrality is the utilization of CO_(2) under economic and sustainable ***,the strong need for carbon neutrality has led to a proliferation of studies on the direct conversion of CO_(2) into carboxylic acids,which can effectively alleviate CO_(2) emissions and create high-value *** purpose of this review is to present the application prospects of carboxylic acids and the basic principles of CO_(2) conversion into carboxylic acids through photo-,electric-,and thermal *** attention is focused on the regulation strategy of the activity of abundant catalysts at the molecular level,inspiring the preparation of high-performance *** addition,theoretical calculations,advanced technologies,and numerous typical examples are introduced to elaborate on the corresponding process and influencing factors of catalytic ***,challenges and prospects are provided for the future development of this *** is hoped that this review will contribute to a deeper understanding of the conversion of CO_(2) into carboxylic acids and inspire more innovative breakthroughs.

关键词： carbon neutrality carboxylic acids CO_(2)conversion heterogeneous catalyst in situ technology

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Process design and intensification of multicomponent azeotropes special distillation separation via molecular simulation and system optimization

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Chinese Journal of chemical Engineering 2024年第7期71卷 24-44页

作者： Chunliang Liu Jianhui Zhong Ranran Wei Jiuxu Ruan Kaicong Wang Zhaoyou Zhu Yinglong Wang Limei Zhong college of chemical Engineering Qingdao University of Science and TechnologyQingdao 266042China

This work provides an overview of distillation processes,including process design for different distillation processes,selection of entrainers for special distillation processes,system integration and intensification of distillation processes,optimization of process parameters for distillation processes and recent research progress in dynamic control ***,the feasibility of using thermodynamic topological theories such as residual curve,phase equilibrium line and distillation boundary line to analyze different separation regions is discussed,and the rationality of distillation process design is discussed by using its ***,the application of molecular simulation methods such as molecular dynamics simulation and quantum chemical calculation in the screening of entrainer is discussed for the extractive distillation *** thermal coupling mechanism of different distillation processes is used to explore the process of different process ***,a mixed integer nonlinear optimization strategy for the distillation process based on different algorithms is ***,the improvement of dynamic control strategies for different distillation processes in recent years is *** work focuses on the application of process intensification and system optimization in the design of distillation process,and analyzes the challenges,prospects,and development trends of distillation technology in the separation of multicomponent azeotropes.

关键词： Azeotrope separation Process design Optimization algorithm Process integration Dynamic control Entrainer selection

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Tough lanthanide luminescent hydrogel for nitroaromatics detection

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Journal of Rare Earths 2024年第2期42卷 293-302,I0003页

作者： Shu Xie Fei Li Fengyi Liu Quanqing Xu Xufeng Zhang college of chem.stry and chemical Engineering Yunnan Normal UniversityKunming650092China

Luminescent hydrogels have received considerable attention in the application of *** matics are harmful to human health and can be *** skin allergies and central nervous system injuries may also be attributed to the over exposure to ***,nitroaromatics sensor with fast detection and low detection limit is highly ***,novel tough hydrogels were prepared by introducing hydrogen bonds and covalent bonds into the interpenetrating networks of modified chitosan and poly(vinyl alcohol)(PVA) via frozen-thawing induced chemical *** synthesized hydrogels exhibit high mechanical strength(0.23 MPa tensile strength at 140% tensile strain,1.0 MPa compressive strength at 80% compressive strain).Strong green emission was realized by energy transfer from the modified chitosan to Tb^(3+)via the so-called "antenna effect." The prepared luminescent hydrogels show an excellent detection effect on nitroaromatic compounds and its detection limit can reach *** hydrogels also exhibit good reversibility and a fast "off-on" fluorescence switching *** work may open up a new way for the development of stable,rapid,and reusable sensors for the detection of harmful nitroaromatics.

关键词： Hydrogels Lanthanide Luminescence Nitroaromatics Sensors Rare earths

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High-performance Ti_(3)C_(2)T_(x)achieved by polyaniline intercalation and gelatinization as a high-energy cathode for zinc-ion capacitor

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Nano Research 2024年第6期17卷 5305-5316页

作者： Peng Liao ZiYu Geng Xin Zhang Wenjie Yan Zenghui Qiu Haijun Xu college of Mathematics and Physics Beijing University of Chemical TechnologyBeijing 100029China

The actual manufacture of supercapacitors(SCs)is restricted by the inadequate energy density,and the energy density of devices can be properly promoted by assembling zinc-ion capacitors(ZICs)which used capacitive cathode and battery-type ***-dimensional(2D)MXene has brought great focuses in the electrode research on the foundation of large redox-active surface,but the specific capacitance is still affected by the tight stacking of ***_(3)C_(2)T_(x)@polyaniline(PANI)heterostructures are prepared by uniformly depositing the conductive polymer PANI nanorods as the intercalation agent into the external of Ti_(3)C_(2)T_(x)nanosheets to inhibit ***,by using graphene oxide(GO)-assisted low-temperature hydrothermal self-assembly manufacture,2D heterostructures are assembled into the three-dimensional(3D)porous crosslinked Ti_(3)C_(2)T_(x)@PANI-reduced graphene oxide(RGO)*** to the synergistic work of PANI nanorods,Ti_(3)C_(2)T_(X)nanosheets,and 3D crosslinking frameworks of RGO to match capacitive and battery effects,3D porous hierarchical Ti_(3)C_(2)T_(x)@PANI-RGO heterostructure hydrogels have rich ion transport channels,a large number of active sites,and excellent reaction *** is assembled by using Ti_(3)C_(2)T_(x)@PANI-RGO heterostructure hydrogels as cathodes and zinc foil as *** this work,Ti_(3)C_(2)T_(x)@PANI-RGO//Zn ZIC exhibits a wide working window(2.0 V),marked specific capacitance(589.89 F·g^(−1)at 0.5 A·g−1),salient energy density(327.71 Wh·kg^(−1)at 513.61 W·kg^(−1)and 192.20 Wh·kg^(−1)at 13,005.87 W·kg^(−1)),and durable cycling stability(97.87%capacitance retention after 10,000 cycles at 10 A·g^(−1)).This study emphasizes the device design of ZICs and the broad prospect of Ti_(3)C_(2)T_(x)-based hydrogels as viable cathodes for ZICs.

关键词： polyaniline(PANI) Ti_(3)C_(2)T_(x)@PANI heterostructure intercalation process three-dimensional(3D)porous hydrogel high energy density zinc-ion capacitor

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Transition metal clusters with precise numbers of atoms anchored on graphdiyne as multifunctional electrocatalysts for OER/ORR/HER:a computational study

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Rare Metals 2024年第7期43卷 3107-3117页

作者： Xin-Yang Liu Jing-Wei Liu Gang Li Jing-Xiang Zhao college of chem.stry and chemical Engineering Harbin Normal UniversityHarbin 150025China

Subnanometer metal clusters play an increasingly important role in heterogeneous catalysis due to their high catalytic activity and *** this work,by means of the density functional theory(DFT) calculations,the catalytic activities of transition metal clusters with precise numbers of atoms supported on graphdiyne(TM_(1-4)@GDY,TM=V,Cr,Mn,Fe,Co,Ni,Cu,Ru,Rh,Pd,Ir,Pt) were investigated for oxygen evolution reactions(OER),oxygen reduction reactions(ORR) and hydrogen evolution reactions(HER).The computed results reveal that the Pd_(2),Pd_(4) and Pt_(1) anchored graphdiyne can serve as trifunctional catalysts for OER/ORR/HER with the overpotentials of 0.49/0.37/0.06,0.45/0.33/0.12 and 0.37/0.43/0.01 V,respectively,while Pd_(1) and Pt_(2)@graphdiyne can exhibit excellent catalytic performance for water splitting(OER/HER) with the overpotentials of 0.55/0.17 and 0.43/0.03 *** addition,Ni_(1) and Pd_(3) anchored GDY can perform as bifunctional catalysts for metal-air cells(OER/ORR) and fuels cells(ORR/HER) with the overpotentials of 0.34/0.32 and 0.42/0.04 V,***,by precisely controlling the numbers of atoms in clusters,the TM_(1-4) anchored graphdiyne can serve as promising multifunctional electrocatalysts for OER/ORR/HER,which may provide an instructive strategy to design catalysts for the energy conversation and storage devices.

关键词： Density functional theory Graphdiyne Single-cluster catalysts Multifunctional electrocatalysts Overpotential

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A healable, mechanically robust and ultrastretchable ionic conductive elastomer for durably wearable sensor

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Nano Research 2024年第4期17卷 3369-3378页

作者： Guoxian Zhang Chunmei Li JiaoJun Tan Mingqi Wang Yafeng Ren Feijie Ge Qiuyu Zhang Key Laboratory of Special Functional and Smart Polymer Materials of Ministry of industry and Information Technology School of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi'an 710072China college of Bioresources chemical and Materials Engineering National Demonstration Center for Experimental Light Chemistry Engineering EducationShaanxi University of Science&TechnologyXi’an 710021China

The ionic conductive elastomers show great promise in multifunctional wearable electronics,but they currently suffer from liquid leakage/evaporation or mechanical *** ionic conductive elastomers integrating non-volatility,mechanical robustness,superior ionic conductivity,and ultra-stretchability remains urgent and ***,we developed a healable,robust,and conductive elastomer via impregnating free ionic liquids(ILs)into the ILs-multigrafted poly(urethane-urea)(PUU)elastomer networks.A crucial strategy in the molecular design is that imidazolium cations are largely introduced by double-modification of PUU and centipede-like structures are obtained,which can lock the impregnated ILs through strong ionic *** this system,the PUU matrix contributes outstanding mechanical properties,while the hydrogen bonds and ionic interactions endow the elastomer with self-healing ability,conductivity,as well as non-volatility and *** fabricated ionic conductive elastomers show good conductivity(3.8×10^(-6) S·cm^(-1)),high mechanical properties,including tensile stress(4.64 MPa),elongation(1470%),and excellent healing ability(repairing efficiency of 90%after healing at room temperature for 12 h).Significantly,the conductive elastomers have excellent antifatigue properties,and demonstrate a highly reproducible response after 1000 uninterrupted extension-release *** work provides a promising strategy to prepare ionic conductive elastomers with excellent mechanical properties and stable sensing capacity,and further promote the development of mechanically adaptable intelligent sensors.

关键词： ionic conductive elastomers poly(urethane-urea)(PUU) ionic interactions centipede-like self-healing

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Preparation and properties of poly(ethylene glycol)-bpoly( 3-acrylamidophenylboronic acid) glucose responsive particles and their hyaluronic acid-based microneedle patches

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Journal of Zhejiang University-Science A(Applied Physics & Engineering) 2024年第5期25卷 395-410页

作者： Yichuan HONG Haojie YU Li WANG Xiang CHEN Di SHEN Yu WANG Shuning REN Yudi HUANG Jian YANG State Key Laboratory of chemical Engineering College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310058China Zhejiang-Russia Joint Laboratory of Photo-Electro-Magnetic Functional Materials College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310058China

To overcome the pain and risk of hypoglycemia in insulin administration,glucose-responsive microneedles have been developed by researchers,which could release insulin according to the blood glucose *** designed a kind of particles by a reversible addition-fragmentation chain transfer(RAFT)method containing a phenylboronic acid group as the sensor of glucose and carrier of ***(ethylene glycol)(PEG)-2-(dodecylthio(thiocarbonyl)thio)-2-methylpropionic acid(DDMAT)was synthesized as a macromolecular RAFT agent,which was then reacted with 3-acrylamidophenylboronic acid(AAPBA)to synthesize the block copolymer ***-responsive particles loaded with insulin were prepared by self-assembly based on hydrophilic-hydrophobic *** patches loaded with glucose-responsive particles were prepared using hyaluronic acid as the *** insulin release behavior of the particles in glucose solutions of 0,100,and 400 mg/dL showed significant glucose responsiveness and good *** results of blood glucose control experiments in rats indicate that a single microneedle patch can effectively maintain normal blood glucose for over 7 h.

关键词： Diabetes Hyaluronic acid Phenylboronic acid(PBA) Glucose responsive hydrogel Microneedles

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