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MXenes/CNTs-based hybrids:Fabrications,mechanisms,and modification strategies for energy and environmental applications

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Nano Research 2024年第5期17卷 3429-3454页

作者： Jizhou Jiang Fangyi Li Lei Ding Chengxun Zhang Arramel Xin Li School of Environmental Ecology and Biological engineering School of Chemistry and Environmental EngineeringKey Laboratory of Green Chemical Engineering Process of Ministry of EducationEngineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationNovel Catalytic Materials of Hubei Engineering Research CenterWuhan Institute of TechnologyWuhan 430205China Nano Center Indonesia Jl.PUSPIPTEK Tangerang SelatanBanten 15314Indonesia Institute of Biomass engineering Key Laboratory of Energy Plants Resource and UtilizationMinistry of Agriculture and Rural AffairsSouth China Agricultural UniversityGuangzhou 510642China

Emerging two-dimensional(2D)layered metal carbide and nitride materials,commonly termed MXenes,are increasingly recognized for their applications across diverse fields such as energy,environment,and catalysis.In the past few years,MXenes/carbon nanotubes(CNTs)-based hybrids have attracted extensive attention as an important catalyst in energy and environmental fields,due to their superior multifunctions and mechanical stability.This review aims to address the fabrication strategies,the identification of the enhancement mechanisms,and recent progress regarding the design and modification of MXenes/CNTs-based hybrids.A myriad of fabrication techniques have been systematically summarized,including mechanical mixing,spray drying,three-dimensional(3D)printing,self-assembly/in-situ growth,freeze drying,templating,hydrothermal methods,chemical vapor deposition(CVD),and rolling.Importantly,the identification of the enhancement mechanisms was thoroughly discussed from the two dimensions of theoretical simulations and in-situ analysis.Moreover,the recent advancements in profound applications of MXenes/CNTs-based hybrids have also been carefully revealed,including energy storage devices,sensors,water purification systems,and microwave absorption.We also underscore anticipated challenges related to their fabrication,structure,underlying mechanisms,modification approaches,and emergent applications.Consequently,this review offers insights into prospective directions and the future trajectory for these promising hybrids.It is expected that this review can inspire new ideas or provide new research methods for future studies.

关键词： MXenes/carbon nanotubes(CNTs)-based hybrids fabrication applications modification strategies

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Rare earth element-modified MOF materials:synthesis and photocatalytic applications in environmental remediation

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Rare Metals 2024年第4期43卷 1390-1406页

作者： Shu-Kun Le Qi-Jie Jin Jia-Ao Han Hua-Cong Zhou Quan-Sheng Liu Fu Yang Jie Miao Pei-Pei Liu Cheng-Zhang Zhu Hai-Tao Xu Inner Mongolia key laboratory of high-Value Functional utilization of Low Rank Carbon Resources Chemical Engineering CollegeInner Mongolia University of Technology School of Environmental Science and engineering Nanjing Tech University School of Environmental and chemical engineering Jiangsu University of Science and Technology Institut National de la Recherche Scientifique-énergie Matériaux et Télécommunications

Metal-organic framework-like materials（MOFs）have been developed in the fields of photocatalysis for their excellent optical properties and physicochemical properties,including environmental remediation,CO2 photoreduction,water splitting,and so on.With their important roles in various fields,rare earth elements have received growing interests from scientists.Modifying MOFs with rare earth elements for modification allows broadening the absorption spectrum,while the active electrons on their empty 4f orbitals can act as traps to capture photoexcited carriers to inhibit the recombination of electron-hole pairs,thus promoting photocatalytic activity.Therefore,rare earth elements modified MOFs provide an attractive way to achieve their high value utilization.In this mini-review,the synthesis of rare earth element-modified MOFs photocatalysts and corresponding applications in the removal of antibiotics,CO2reduction,and hydrogen production are constructively summarized and discussed.Finally,the latest advancements and current difficulties of these materials as well as the application prospects are also provided.

关键词： Rare earth metals MOFs Photocatalytic CO 2 reduction Environmental remediation Water splitting

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Recent advances of versatile reagents as controllable building blocks in organic synthesis

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Chinese chemical Letters 2024年第2期35卷 24-43页

作者： Shaomin Chen Luigi Vaccaro Yanlong Gu key laboratory of Material Chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China laboratory of green S.O.C. Dipartimento di ChimicaBiologia e BiotecnologieUniversità degli Studi di PerugiaVia Elce di Sotto 8Perugia 06123Italy School of Chemistry and chemical engineering The Key Laboratory for Green Processing of Chemical Engineering of Xinjiang BingtuanShihezi UniversityShihezi 832004China

Diversity-oriented synthesis is a powerful and interesting synthetic tool for the rapid construction of structurally complex and privileged scaffolds from readily accessible starting materials.To date,diversity-oriented synthesis mostly relies on the employment of versatile reagents.Versatile reagents can be regulated as controllable and flexible building blocks for multipurpose utilizations.Over the past decade,a variety of multifunctional reagents have been developed.However,most versatile reagents usually need multi-step synthesis,thus restricting their wide application to a large extent.In terms of the practicalities and universalities,we prefer to pay more attention to the utilization of simple and practical versatile reagents with multiple reactivities,mainly including atropaldehyde acetals,aryl methyl ketones,vinylene carbonate,vinyl azides,aryldiazonium salts,rongalite,halodifluoromethyl compounds.Most importantly,these versatile reagents can also play different roles simultaneously in the same reaction,in which their different reactivities are converged into the final target products.Such strategy can not only offer more possibilities for the synthesis of several active pharmaceutical ingredients,but also minimize the occurrence of some side reactions by lessening the varieties of materials.Also,a perspective is given at the end of this review.

关键词： Versatile reagents Divergent synthesis Dual synthons Bond cleavage Tandem reactions

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Enhanced population of excited single state strategy:Irradiation and ultrasound dual-response and host tumor-driven nanosensitizers construction in triple synergistic therapy

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Nano Research 2024年第6期17卷 5501-5511页

作者： Yaning Li Mengyan Tian Tianyue Yang Jiayu Cao Hongli Chen Jun Guo Pai Liu Yi Liu state key laboratory of Separation Membranes and Membrane Processes School of Materials Science and EngineeringTiangong UniversityTianjin 300387China state key laboratory of Separation Membranes and Membrane Processes School of ChemistryTiangong UniversityTianjin 300387China state key laboratory of Separation Membranes and Membrane Processes School of Life ScienceTiangong UniversityTianjin 300387China state key laboratory of Separation Membrane and Membrane Process&Tianjin key laboratory of green chemical Technology and Process engineering School of ChemistryTiangong UniversityTianjin 300387China School of chemical and Environmental engineering Wuhan Polytechnic UniversityWuhan 430023China Cangzhou Institute of Tiangong University Cangzhou 061000China

Phototheranostics is an emerging field in synergistic antitumor therapy in which irradiation and sensitizers are combined to produce reactive oxygen species(ROS),bio-images,and high temperatures.All of these are arrived from the energy of sensitizers,which located in excited single state(S_(1)).Undeniably,the decentralization of the S_(1)population indirectly decreases the effect of each individual treatment.In this study,a strategy was proposed for enhancing the S_(1)population,and a sensitizer with mitochondrial targeting property,1,4-indolyl iodinated pyrrolo[3,2-b]pyrrole derivative(2I-TPIS),was assembled into adenosine triphosphate(ATP)-responsive nanoparticles(DPA-2I NPs)to achieve dual responses to irradiation and ultrasonication(US)for application to photo-sonodynamic therapy(PSDT).Compared with monotherapies,2I-TPIS generated more ROS in PSDT,inducing mitochondrial autophagy and apoptosis,which in turn triggered immunogenic cell death(ICD).Subsequently,DPA-2I NPs were constructed and self-assembled with the chemotherapeutic agents DPA-Cd and 2I-TPIS to achieve a triple synergistic strategy involving chemotherapy(CT)and PSDT.DPA-2I NPs exhibited absolute sensitization,intra-tumoral overexpression of ATP,and disassembly.Importantly,the biosafety and potent antitumor efficiency of the DPA-2I NP-based“PSDT+CT”therapy were revealed using a 4T1 tumor model.The study results provide insights into the design of sensitizers possessing a sufficient S_(1)population and a highly efficient tumor ablation capacity derived from molecular structural modulation,further enabling triple synergistic antitumor therapies,and expanding the clinical application of sensitizers.

关键词： triphosphate(ATP)-activated nano-sensitizers photo-sonodynamic therapy aggregation-induced emission enhanced excited state population

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Linear paired electrolysis of furfural to furoic acid at both anode and cathode in a multiple redox mediated system

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green Energy & Environment 2024年第1期9卷 104-113页

作者： Xinxin Li Linchuan Cong Haibo Lin Fangbing Liu Xiangxue Fu Hai-Chao Xu Nan Lin state key laboratory of Inorganic Synthesis and Preparative Chemistry Jilin UniversityChangchun 130012JilinChina state key laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005FujianChina

Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future.Here,we report a multiple redox-mediated linear paired electrolysis system,combining the hydrogen peroxide mediated cathode process with the I2 mediated anode process,and realize the conversion of furfural to furoic acid in both side of the dividedﬂow cell simultaneously.By reasonably controlling the cathode potential,the undesired water splitting reaction and furfural reduction side reactions are avoided.Under the galvanostatic electrolysis,the two-mediated electrode processes have good compatibility,which reduce the energy consumption by about 22%while improving the electronic efﬁciency by about 125%.This system provides a green electrochemical synthesis route with commercial prospects.

关键词： Multiple redox mediated system Linear paired electrolysis Furfural Furoic acid

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Preparation and properties of high-energy-density aluminum/boroncontaining gelled fuels

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Chinese Journal of chemical engineering 2024年第1期65卷 230-242页

作者： Yi Chen Kang Xue Yang Liu Lun Pan Xiangwen Zhang Ji-Jun Zou key laboratory for green chemical Technology of the Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Collaborative Innovative Center of chemical Science and engineering(Tianjin) Tianjin 300072China Haihe laboratory of Sustainable chemical Transformations Tianjin 300192China Zhejiang Institute of Tianjin University Ningbo 315201China

Energetic nanofluid fuel has caught the attention of the field of aerospace liquid propellant for its high energy density(HED), but it suffers from the inevitable solid-liquid phase separation problem. To resolve this problem, herein we synthesized the high-Al-/B-containing(up to 30%(mass)) HED gelled fuels, with low-molecular-mass organic gellant Z, which show high net heat of combustion(NHOC), density, storage stability, and thixotropic properties. The characterizations indicate that the application of energetic particles to the gelled fuels obviously destroys their fibrous network structures but can provide the new particle-gellant gelation microstructures, resulting in the comparable stability between 1.0%(mass) Z/JP-10 + 30%(mass) Al or B and pure JP-10 gelled fuel. Moreover, the gelled fuels with high-content Al or B exhibit high shear-thinning property, recovery capability, and mechanical strength, which are favorable for their storage and utilization. Importantly, the prepared 1.0%(mass) Z/JP-10 + 30%(mass) B(or 1.0%(mass) Z/JP-10 + 30%(mass) Al) shows the density and NHOC 1.27 times(1.30) and 1.43 times(1.21)higher than pure JP-10, respectively. This work provides a facile and valid approach to the manufacturing of HED gelled fuels with high content of energetic particles for gel propellants.

关键词： Gelled fuels Energetic aluminum/boron Low-molecular-mass organic gellant Fuel property

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Mechanism study of Cu(Ⅱ) adsorption from acidic wastewater by ultrasonic-modified municipal solid waste incineration fly ash

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Chinese Journal of chemical engineering 2024年第3期67卷 157-165页

作者： Shunda lin Yang Lu Lin Zheng Ling Long Xuguang Jiang Jianhua Yan state key laboratory of Clean Energy utilization Institute for Thermal Power EngineeringZhejiang UniversityHangzhou 310027China Zhejiang University Qingshanhu Energy Research Center Hangzhou 310027China Hangzhou Xiaoshan Jinjiang green Energy Co. Ltd.XiaoshanHangzhou 310000China

high concentrations of copper ions(Cu(Ⅱ)) in water will pose health risks to humans and the ecological environment. Therefore, this study aims to utilize ultrasonic-cured modified municipal solid waste incineration(MSWI) fly ash for Cu(Ⅱ) adsorption to achieve the purpose of “treating waste by waste.” The effects of p H, adsorption time, initial concentration, and temperature on the modified MSWI fly ash’s adsorption efficiency were systematically studied in this article. The adsorption performance of the modified MSWI fly ash can be enhanced by the ultrasonic modification. At pH = 2, 3 and 4, the adsorption capacity of the modified MSWI fly ash for Cu(Ⅱ) increased by 2.7, 1.9 and 1.2 times, respectively. Furthermore, it was suggested that the adsorption process of the modified MSWI fly ash can be better simulated by the pseudo-second-order kinetic model, with a maximum adsorption capacity calculated by the Langmuir model of 24.196 mg.g-1. Additionally, the adsorption process is spontaneous,endothermic, and chemisorption-dominated from the thermodynamic studies(ΔH and ΔS > 0, ΔG < 0).Finally, the enhanced adsorption performance of the modified MSWI fly ash for Cu(Ⅱ) may be attributed to electrostatic interaction and chelation effects.

关键词： Ultrasound MSWI fly ash Cu(Ⅱ) Wastewater Adsorption

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Efficient continuous synthesis of 2-hydroxycarbazole and 4-hydroxycarbazole in a millimeter scale photoreactor

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Chinese chemical Letters 2024年第4期35卷 399-403页

作者： Zhixiang Li Zhirong Yang Chang Yao Bin Wu Gang Qian Xuezhi Duan Xinggui Zhou Jing Zhang state key laboratory of chemical engineering East China University of Science and TechnologyShanghai 200237China School of chemical engineering Zhengzhou UniversityZhengzhou 450001China

2-Hydroxycarbazole and 4-hydroxycarbazole are important chemicals with extensive applications in optoelectronic materials and pharmaceutical field.state of the art yield of 2-hydroxycarbazole is~30%and the reaction time is typically in hours or days.Herein,we developed a green route for the continuous and high-throughput synthesis of 2-hydroxycarbazole and 4-hydroxycarbazole via photochemical intramolecular cyclization of 3–hydroxy-2–chloro-diphenylamine using a self-designed millimeter scale photoreactor,which was designed based on sizing-up and numbering-up strategies for a decent liquid holdup(6.8 m L)and fabricated via femtosecond laser engraving technique.The photochemical synthesis was carried out continuously under the illumination of 365 nm UV-LED with dimethyl sulfoxide as solvent and potassium t-butoxide as catalyst.It was found that under optimized conditions a 2-hydroxycarbazole yield of 31.6%and a 4-hydroxycarbazole yield of 11.1%were obtained with a residence time of 1 min.Compared to semibatch operations,the reaction time was shortened by 1–2 orders of magnitude.As a result,a throughput of 11.3 g/day 2-hydroxycarbazole and 4.0 g/day 4-hydroxycarbazole can be achieved from the photoreactor.It was proposed that the short reaction time and high product yield are resulted from higher photon transfer rates and more uniform photon distribution provided by the millimeter scale photoreactor,which enhances the reaction rates and mitigates overreaction.

关键词： Millimeter scale reactor 2-Hydroxycarbazole Photochemistry UV-LED Process intensification

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Few-layered hexagonal boron nitride nanosheets stabilized Pt NPs for oxidation promoted adsorptive desulfurization of fuel oil

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green Energy & Environment 2024年第3期9卷 495-506页

作者： Peiwen Wu Xin Song Linlin Chen Lianwen He Yingcheng Wu Duanjian Tao Jing He Chang Deng Linjie Lu Yanhong Chao Mingqing Hua Wenshuai Zhu School of Chemistry and chemical engineering Jiangsu UniversityZhenjiang212013China College of chemical engineering and Environment State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum-BeijingBeijing102249China College of Chemistry and chemical engineering Jiangxi Normal UniversityNanchang330022China College of Science State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum-BeijingBeijing102249China

A few-layered hexagonal boron nitride nanosheets stabilized platinum nanoparticles(Pt/h-BNNS)is engineered for oxidation-promoted adsorptive desulfurization(OPADS)of fuel oil.It was found that the few-layered structure and the defective sites of h-BNNS not only are beneficial to the stabilization of Pt NPs but also favor the adsorption of aromatic sulfides.By employing Pt/h-BNNS with a Pt loading amount of 1.19 wt%as the active adsorbent and air as an oxidant,a 98.0%sulfur removal over dibenzothiophene(DBT)is achieved along with a total conversion of the DBT to the corresponding sulfones(DBTO_(2)).Detailed experiments show that the excellent desulfurization activity originates from the few-layered structure of h-BNNS and the high catalytic activity of Pt NPs.In addition,the OPADS system with Pt/h-BNNS as the active adsorbent shows remarkable stability in desulfurization performance with the existence of different interferents such as olefin,and aromatic hydrocarbons.Besides,the Pt/h-BNNS can be recycled 12 times without a significant decrease in desulfurization performance.Also,a process flow diagram is proposed for deep desulfurization of fuel oil and recovery of high value-added products,which would promote the industrial application of such OPADS strategy.

关键词： Desulfurization Adsorption Catalytic oxidation Active adsorbent Dibenzothiophene

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Optimized the vanadium electrolyte with sulfate-phosphoric mixed acids to enhance the stable operation at high-temperature

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Frontiers of chemical Science and engineering 2024年第2期18卷 13-26页

作者： Ling Ge Tao Liu Yimin Zhang Hong Liu School of Resource and Environmental engineering Wuhan University of Science and TechnologyWuhan 430081China state Environmental Protection key laboratory of Mineral Metallurgical Resources utilization and Pollution Control Wuhan University of Science and TechnologyWuhan 430081China Hubei Collaborative Innovation Center for high Efficient utilization of Vanadium Resources Wuhan University of Science and TechnologyWuhan 430081China Hubei Provincial engineering Technology Research Center of high Efficient Cleaning utilization for Shale Vanadium Resource Wuhan University of Science and TechnologyWuhan 430081China School of Resource and Environmental engineering Wuhan University of TechnologyWuhan 430070China

Herein, the influence of the concentration design and comprehensive performance of the sulfate-phosphoric mixed acid system electrolyte is investigated to realize an electrolyte that maintains high energy density and stable operation at high temperatures. Static stability tests have shown that VOPO4 precipitation occurs only with vanadium(V) electrolyte. The concentration of vanadium ion of 2.0–2.2 mol·L^(–1), phosphoric acid of 0.10–0.15 mol·L^(–1), and sulfuric acid of 2.5–3.0 mol·L^(–1) are suitable for a vanadium redox flow battery in the temperature range from –20 to 50 ℃. The equations for predicting the viscosity and conductivity of electrolytes are obtained by the response surface method. The optimized electrolyte overcomes precipitation generation. It has 2.8 times higher energy density than the non-phosphate electrolyte, and a coulomb efficiency of 94.0% at 50 ℃. The sulfate-phosphoric mixed acid system electrolyte promotes the electrode reaction process, increases the current density, and reduces the resistance. This work systematically optimizes the concentrations of composition of positive and negative vanadium electrolytes with mixed sulfate-phosphoric acid. It provides a basis for the different valence states and comprehensive properties of sulfate-phosphoric mixed acid system vanadium electrolytes under extreme environments, guiding engineering applications.

关键词： all vanadium redox flow battery mixed-acid vanadium electrolyte concentration optimization response surface methodology high-temperature stability

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