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Self-separation ionic liquid catalyst for the highly effective conversion of H2S by α,β-unsaturated carboxylate esters under mild conditions

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Green Energy & Environment 2024年第9期9卷 1440-1448页

作者： Wenjie Xiong Xiaomin Zhang Xingbang Hu Youting Wu Key Laboratory of Mesoscopic chemistry of MOE School of Chemistry and Chemical Engineering Nanjing University The Institute of Green chemistry and engineering School of Chemistry and Chemical Engineering Nanjing University

The deep-processing utility of pure hydrogen sulfide （H2S） is a significant direction in natural gas chemical ***,a brand-new strategy of H2S conversion by a,β-unsaturated carboxylate esters into thiols or thioethers using task-specific carboxylate ionic liquids （ILs） as catalyst has been developed,firstly accomplishing the phase separation of product and catalyst without introducing the third *** can be considered as a cascade reaction in which the product selectivity can be controlled by adjusting the molar ratio of H2S to a,β-unsaturated carboxylate ***,the effects of ILs with different anions and cations,intermittent feeding operations,as well as pressure-time kinetic behaviors on cascade reaction were ***,the proposed interaction mechanism of H2S conversion using butyl acrylate catalyzed by[Emim][Ac]was revealed by DFT-based theoretical *** approach enables the self-phase separation promotion of catalyst and product and achieves 99%quantitative conversion under mild conditions in the absence of solvent,making the entire process ecologically ***-efficiency reaction activity can still be maintained after ten cycles of the ***,the good results,combined with its simplicity of operation and the high recyclability of the catalyst,make this green method environmentally friendly and *** is anticipated that this self-separation method mediated by task-specific ILs will provide a feasible strategy for H2S utilization,which will guide its application on an industrial scale.

关键词： Ionic liquid Cascade reaction Self-separation H 2 S conversion Catalysis

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Two-dimensional C2N-based single-atom catalyst with complex microenvironment for enhanced electrochemical nitrogen reduction:A descriptor-based design

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Journal of Energy chemistry 2024年第10期97卷 110-119页

作者： Enduo Dai Wei An Ruixian Guo Xugen Shi Yunyi Li Yibo Wang Mingming Liu College of chemistry and chemical engineering Shanghai University of Engineering Science

The catalytic descriptor with operational feasibility is highly desired towards rational design of high-performance catalyst especially the electrode/electrolyte solution interface working under mild ***,we demonstrate that the descriptor Ω parameterized by readily accessible intrinsic properties of metal center and coordination is highly operational and efficient in rational design of single-atom catalyst（SAC） for driving electrochemical nitrogen reduction（NRR）.Using twodimensional metal（M）-BxPySzNm@C2N as prototype SAC models,we reveal that*N2+（H++e-）→*N2H acts predominantly as the potential-limiting step（PLS） of NRR on M-B2P2S2@C2N and M-B1P1S1N3@C2N regardless of the distinction in coordination *** the 28 screened M active sites,with Ω values close to the optimal 4,M-B2P2S2@C2N(M=V（Ω=3.53）,Mo（Ω=5.12）,and W（Ω=3.92）) and M-B1P1S1N3@C2N(M=V（Ω=3.00）,Mo（Ω=4.34）,and W（Ω=3.32）) yield the lowered limiting potential（UL） as-0.45,-0.54.-0.36,-0.58,-0.25,and-0.24 V,respectively,thus making them the promising NRR *** importantly,these SACs are located around the top of volcano-shape plot of ULversus Ω,re-validating Ω as an effective descriptor for accurately predicting the high-activity NRR SACs even with complex *** study unravels the relationship between active-site structure and NRR performance via the descriptor Ω,which can be applied to other important sustainable electrocatalytic reactions involving activation of small molecules via σ-donation and π*-backdonation mechanism.

关键词： Descriptor DFT Electrocatalysis N2 reduction Single-atom catalyst

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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 chemistry 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 chemistry 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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NIR-IIb-triggered photodynamic therapy combined with chemotherapy platform based on rare-earth-doped nanoparticles

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Rare Metals 2024年第7期43卷 3220-3231页

作者： Zhuo Tu Yong Wan Juan Ge Chen-Chen Li Tao Liang Zhen Li chemistry and chemical engineering Hubei UniversityWuhan 430062China

Photodynamic therapy(PDT),with high spatiotemporal selectivity,minimal side effects and less drug resistance,has emerged as a promising approach for the treatment of ***,inadequate penetration depth and poor efficacy seriously restrict its practical *** address these challenges,we developed a combined therapy platform(RENP@C/D-FA)based on rare-earth-doped nanoparticles(RENPs)with a structure of NaErF_(4):Tm(0.5%)@NaYF_(4),on which photosensitizer Ce6(chlorin e6)and chemo-therapeutic drug(DOX)(doxorubicin)were loaded by encapsulating with an amphiphilic polymer distearoyl phosphatidylethanolamine-polyethylene glycol-folic acid(DSPE-PEG-FA).RENPs with NaErF_(4) as the matrix possess multiple excitation/emission peaks,enabling activation of PDT under near-infrared-Ⅱb(NIR-Ⅱb,1500-1700 nm)excitation and luminescence imaging in NIR-Ⅱb region by absorbing 808 nm near-infrared ***,DOX can be selectively released in the acidic microenvironment of *** from the tumor targeting capability of folic acid,this platform can successfully ablate tumor cells and inhibit tumor growth by combining PDT and *** innovative approach holds great promise as a powerful tool for cancer treatment,showing the potential to revolutionize PDT.

关键词： Photodynamic therapy Rare-earth-doped nanoparticles NIR-IIb Chemotherapy Combined therapy

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Programmed DNA walkers for biosensors

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Chinese chemical Letters 2024年第9期35卷 119-129页

作者： Chang Liu Tao Wu Lijiao Deng Xuzi Li Xin Fu Shuzhen Liao Wenjie Ma Guoqiang Zou Hai Yang School of chemistry and chemical engineering Hunan Institute of EngineeringXiangtan 411104China College of chemistry and chemical engineering Central South UniversityChangsha 410083China

Nowadays,due to excellent biological and polymeric characteristics,DNA has been widely noted as an emerging building block to construct diverse materials for biosensing,in vivo imaging,drug delivery,and disease ***,relying on programmability,predictability,and stability of DNA,DNA walkers have opened new and exciting opportunities in modern life sciences for target detection and biological analysis,which are constructed by self-assembly of DNA or combining DNA with other nanomaterials(e.g.,quantum dots,gold nanoparticles,magnetic nanoparticles,polymers).Compared with conventional nanomaterials(lanthanide-doped upconversion nanoparticles,magnetic nanomaterials,carbon dots,silicon dots,and so on),DNA walkers showed convenient modification,lower biotoxicity,excellent biocompatibility and high biostability,improving the biological ***,with high-speed operating efficiency and sustainable operation,DNA walkers powered by strand displacement reaction or protein enzyme/DNAzyme reaction,have highly sensitive detection and signal amplification abilities,which are applied in biosensing,material assembly and synthesis,and early cancer ***,DNA walkers could be regarded as signal amplifiers,which enhanced the signal transduction and amplified biosensor sensing ***,we systematically and comprehensively summarized the operating principles of various DNA walkers,categorized rational design of the DNA walker,and outlined the application of DNA walker in ***,the challenges and future trends of DNA walkers were discussed.

关键词： DNA walker Biosensors Signal amplification strategies Operating principles Design strategies

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An unexpected approach to enhance specific surface area and mesopore amount of polyaniline by Zn doping

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Rare Metals 2024年第9期43卷 4585-4594页

作者： Zhi-Da Zhu Yu-Zhe Han Xiao-Bi Jing School of Mechanical engineering Yangzhou University School of chemistry and chemical engineering Yangzhou University

Poly-p-anisidine could be easily fabricated via the oxidative polymerization reaction of p-anisidine using H2O2as the green oxidant. It was unexpectedly found that zinc doping could significantly improve the adsorption ability of the material versus heavy metals such as Pb, Cu,Pd, Ag and Hg. Results of nitrogen adsorption–desorption experiments demonstrated that Zn doping could enhance the specific surface area and mesopore amount of the prepared material, which might facilitate its absorption to metals. This work not only provides a novel material for the treatment of heavy metal-polluted water but also leads to a nice mesoporous catalyst support for environment protection and organic synthesis, i.e. the Zn-doped poly-panisidine can be employed as the catalyst support to prepare Cu@PANI-OMe/Zn or Pd@PANI-OMe/Zn for the oxidative degradation reaction of phenol or Suzuki–Miyaura coupling reactions, respectively. It discloses a new strategy for fabricating the mesoporous polyaniline materials with profound application potential.

关键词： Adsorption Catalysis Porous materials Rare metal concentration Surfaces

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Emerging perovskite materials for supercapacitors:Structure,synthesis,modification,advanced characterization,theoretical calculation and electrochemical performance

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Journal of Energy chemistry 2024年第2期89卷 41-70,I0003页

作者： Yuehua Qian Qingqing Ruan Mengda Xue Lingyun Chen Department of Applied chemistry School of Chemistry and Chemical EngineeringChongqing UniversityChongqing 401331China

As a new generation electrode materials for energy storage,perovskites have attracted wide attention because of their unique crystal structure,reversible active sites,rich oxygen vacancies,and good *** this review,the design and engineering progress of perovskite materials for supercapacitors(SCs)in recent years is ***,the review will focus on four types of perovskites,perovskite oxides,halide perovskites,fluoride perovskites,and multi-perovskites,within the context of their intrinsic structure and corresponding electrochemical performance.A series of experimental variables,such as synthesis,crystal structure,and electrochemical reaction mechanism,will be carefully analyzed by combining various advanced characterization techniques and theoretical *** applications of these materials as electrodes are then featured for various ***,we look forward to the prospects and challenges of perovskite-type SCs electrodes,as well as the future research direction.

关键词： Perovskite Modification engineering Oxygen vacancy Theoretical calculation methodology Supercapacitor

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Micro/nanoelectrode-based electrochemical methodology for single cell and organelle analysis

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Nano Research 2024年第1期17卷 196-206页

作者： Chuchu Xu De Yang Yuchan Wang Ruolin Liu Fan Wang Zhongqun Tian Keke Hu Department of chemistry College of Chemistry&Chemical EngineeringXiamen UniversityXiamen 361005China

Cells are the basic unit of *** analysis of single cells/organelles is essential for uncovering the molecular mechanisms of physiological and pathological processes that are difficult to elucidate on a larger *** paper provides an overview of the commonly used fabrication methods for micro/nanoelectrodes applied in the investigations of single cells/organelles as well as the corresponding electrochemical measurements over the last four years including extracellular measurement,combination of extra and intracellular measurement,intracellular reactive oxygen species and reactive nitrogen species(ROS/RNS)measurement,and isolated organelles measurement.

关键词： single cell/organelle micro/nanoelectrode electrochemical measurement chemical transmitters

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Phase and chemical state tuning of FeNi oxides for oxygen evolution reaction

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Science China chemistry 2024年第8期67卷 2755-2766页

作者： Jiawei Wu Zhouyang Ma Lice Yu Shuli Wang Fulin Yang Ligang Feng School of chemistry and chemical engineering Yangzhou UniversityYangzhou 225002China

Advancing and deploying the Fe Ni-based catalyst,the state-of-the-art pre-electrocatalysts,for oxygen evolution reactions(OER)still suffer from unclear chemical state correlation to the catalytic ability,as evidenced by the variedly reported performance for the different Fe Ni ***,we contributed the phase and redox chemical states tuning of Fe Ni oxides by the surface microenvironment regulation for the OER catalysis that was realized by the urea-assisted pyrolysis and molybdenum-doping technique by integrating molybdenum into the iron–nickel metal-organic *** by the complicated and compromised atmosphere,namely,the oxidation state driven by the Mo doping and reduction ability induced by the urea-assisted pyrolysis,could transfer confined Fe Ni oxides to hybrid phases of Fe_(2)O_(3)and FeNi_(3)alloy,and the resultant compromised chemical states by the charge redistribution imparted very high electrocatalytic performance for OER compared with the control *** insitu Raman spectroscopy and post-XPS analysis confirmed the facile Fe/Ni oxyhydroxide active phase formation resulting from the proper phase and chemical states,and theoretical analysis disclosed the microenvironment regulation resulting in the charge redistribution forming the electron accumulation and depletion sites to accelerate the oxygen-species to oxyhydroxide-species transformation and enhance the electronic state density near the Fermi level by significantly reducing the energy *** work not only showed the importance of surface chemical state tunning that can basically answer the varied performance of Fe Ni catalysts but also revealed an effective approach for fine-tuning their catalytic properties.

关键词： oxygen evolution reaction FeNi-based catalysts urea pyrolysis chemical states charge redistribution

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Iron-nickel alloy particles with N-doped carbon “armor” as a highly selective and long-lasting catalyst for the synthesis of Nbenzylaniline molecules

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Nano Research 2024年第4期17卷 2308-2319页

作者： Gang Wang Longchao Sun Wanyi Liu Haijuan Zhan Shuxian Bi College of chemistry and chemical engineering Ningxia UniversityYinchuan 750021China

A scalable strategy for the convenient and rapid preparation of nitrogen-doped carbon-coated iron-based alloy catalysts was *** controlling the type and amount of metal salts in the precursor,various types of nitrogen-doped carbon-coated alloy catalysts can be prepared in a targeted ***_(2)Ni2@CN materials with small particle sizes and relatively homogeneous basic sites showed promising results in the N-alkylation reaction of benzyl alcohol with aniline(optimum yield:99%).It is worth noting that the catalyst can also be magnetically separated and recovered after the reaction,and its performance can be regenerated through simple ***,it was confirmed by kinetic experiments that the activation of C–H at the benzyl alcohol benzylic position is the rate-determining step(RDS).According to density flooding theory calculations,Fe_(2)Ni2@CN catalysts require less energy than other materials(Fe@CN and Ni@CN)for the RDS(dehydrogenation reaction)*** N-alkylation reactions are more easily carried out on Fe_(2)Ni2@CN catalysts,which may be the reason for the best catalytic activity of Fe-Ni alloy *** carbon-coated alloy materials will show great potential in more types of heterogeneous catalysis.

关键词： iron-nickel alloy catalyst N-alkylation reaction magnetic separation reaction path dehydrogenation reaction

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