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Exploring nitrogen reduction reaction mechanisms in electrocatalytic ammonia synthesis:A comprehensive review

Journal of Energy Chemistry 2024年第5期92卷 681-697页

作者： Abhishek Umesh Shetty Ravi Sankannavar School of chemical and Materials Science Indian Institute of Technology GoaFarmagudiPonda 403401GoaIndia department of chemical Engineering M.S.Ramaiah Institute of TechnologyMSR NagarMSRIT PostBengaluru 560054KarnatakaIndia

The electrochemical nitrogen reduction reaction(eNRR)holds significant promise as a sustainable alternative to the conventional large-scale Haber Bosch process,offering a carbon footprint-free approach for ammonia *** the process is thermodynamically feasible at ambient temperature and pressure,challenges such as the competing hydrogen evolution reaction,low nitrogen solubility in electrolytes,and the activation of inert dinitrogen(N_(2))gas adversely affect the performance of ammonia *** hurdles result in low Faradaic efficiency and low ammonia production rate,which pose obstacles to the commercialisation of the *** have been actively designing and proposing various electrocatalysts to address these issues,but challenges still need to be resolved.A key strategy in electrocatalyst design lies in understanding the underlying mechanisms that govern the success or failure of the electrocatalyst in driving the electrochemical *** mechanistic studies,we gain valuable insights into the factors affecting the reaction,enabling us to propose optimised designs to overcome the *** review aims to provide a comprehensive understanding of the various mechanisms involved in eNRR on the electrocatalyst *** delves into the various mechanisms such as dissociative,associative,Mars-van Krevelen,lithium-mediated nitrogen reduction and surface hydrogenation mechanisms of nitrogen *** unravelling the intricacies of eNRR mechanisms and exploring promising avenues,we can pave the way for more efficient and commercially viable ammonia synthesis through this sustainable electrochemical process by designing an efficient electrocatalyst.

关键词： Green ammonia synthesis Electrolysis Electrocatalysis Nitrogen reductionreaction Electrochemical reaction pathways Reactionmechanism

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Effect of solvent on the initiation mechanism of living anionic polymerization of styrene:A computational study

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Chinese Journal of chemical Engineering 2024年第5期69卷 135-142页

作者： Shen Li Yin-Ning Zhou Zhong-Xin Liu Zheng-Hong Luo School of chemical Engineering and technology Hainan UniversityHaikou 570228China department of chemical Engineering School of Chemistry and Chemical EngineeringState Key Laboratory of Metal Matrix CompositesShanghai Jiao Tong UniversityShanghai 200240China

For living anionic polymerization(LAP),solvent has a great influence on both reaction mechanism and *** this work,by using the classical butyl lithium-styrene polymerization as a model system,the effect of solvent on the mechanism and kinetics of LAP was revealed through a strategy combining density functional theory(DFT)calculations and kinetic *** terms of mechanism,it is found that the stronger the solvent polarity,the more electrons transfer from initiator to solvent through detailed energy decomposition analysis of electrostatic interactions between initiator and solvent ***,we also found that the stronger the solvent polarity,the higher the monomer initiation energy barrier and the smaller the initiation rate ***,initiation is more favorable at lower temperatures based on the calculated results ofΔG_(TS).Finally,the kinetic characteristics in different solvents were further examined by kinetic *** is found that in benzene and n-pentane,the polymerization rate exhibits first-order ***,slow initiation and fast propagation were observed in tetrahydrofuran(THF)due to the slow free ion formation rate,leading to a deviation from first-order kinetics.

关键词： Living anionic polymerization Solvent effect Reaction kinetics Computational chemistry Mathematical modeling Kinetic modeling

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Studying the effect of surfactant assisted low-salinity water flooding on clay-rich sandstones

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Petroleum 2024年第2期10卷 306-318页

作者： Saeed Khezerloo-ye Aghdam Alireza Kazemi Mohammad Ahmadi department of Petroleum Engineering Amirkabir University of Technology (AUT) department of Petroleum and chemical Engineering College of Engineering Sultan Qaboos University

Sandstone reservoirs often contain clay particles that can cause damage and reduce permeability during low-salinity water flooding. In this study, the effect of surfactants on fine migration in clay-rich sandstones and its impact on oil recovery was ***, the impact of surfactants on interparticle forces in fine-matrix, fine-fine, and oil-matrix systems was modeled. The results showed that both CTAB(cetyltrimethyl ammonium bromide) and QS(quillaja saponin) cause EDL compaction, weakening the repulsive forces. However, SDS(sodium dodecyl sulfate)and TX(triton X-100) do not affect the EDL. Next, the effect of surfactants on IFT reduction and wettability alteration was experimentally investigated. All surfactants reduced IFT due to the surface excessive concentration mechanism. The wettability alteration experiment illustrated that although QS and CTAB compact EDL around oil and matrix particles leading to attraction force augmentation, they both alter wettability through adsorption on matrix and carboxylic groups present in crude oil, *** aqueous solutions were then injected into various clay-rich sandstone sanpacks, which resulted in increased oil recovery. However, the mechanisms leading to enhanced oil recovery variedby surfactant type. CTAB increased recovery by 10% through IFT reduction and wettability alteration, while SDS and TX increased recovery by 12% and 9%, respectively, through wettability alteration and extreme fine migration. In contrast, partial fine migration in the QS flooding experiment reached a recovery increase of 18%. Permeability trends through experiments were also recorded. During CTAB injection,permeability did not reduce, while QS aqueous solution reduced rock permeability to 5 m D. SDS and TX reduced the magnitude of permeability to 2 m *** conclusion, this study demonstrates that surfactants can effectively improve oil recovery in clay-rich sandstones by altering the interparticle forces, reducing IFT, a

关键词： Surfactant flooding Smart water Fine migration Recovery factor

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Recent Advances in Asymmetric Structural Composites for Excellent Electromagnetic Interference Shielding: A Review

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Chinese Journal of polymer Science 2024年第6期42卷 693-710页

作者： Ying Zhou Bai Xue Lan Xie Chang-Mei Wu Qiang Zheng department of polymer Materials and Engineering College of Materials and Metallurgy Guizhou University National Engineering Research Center for Compounding and Modification of polymer Materials National and Local Joint Engineering Research Center for Functional Polymer Membrane Materials and Membrane Processes State Key Laboratory of Public Big Data Guizhou University department of polymer Science and Engineering Zhejiang University

Since electromagnetic pollution is detrimental to human health and the environment, numerous efforts have been successively made to achieve excellent electromagnetic interference shielding effectiveness(EMI SE) via designing the hierarchical structures for electromagnetic interference(EMI) shielding polymer composites. Among the plentiful structures, the asymmetric structures are currently a hot spot, principally categorizing into multi-layered, porous, fibrous, and segregated asymmetric structures, which endows the high EMI shielding performance for polymer composites incorporated with magnetic, conductive, and/or dielectric micro/nano-fillers, due to the “absorption-reflection-reabsorption” shielding mechanism. Therefore, this review provides the retrospection and summary of the efforts with respect to abundant asymmetric structures and multifunctional micro/nano-fillers for enhancing EMI shielding properties, which is conducive to the booming development of polymeric EMI shielding materials for the promising prospect in modern electronics and 5-generation(5G) technology.

关键词： Asymmetric structure Microano functional filler polymer composite Electromagnetic interference shielding

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Toluene Processed All-polymer Solar Cells with 18% Efficiency and Enhanced Stability Enabled by Solid Additive:Comparison Between Sequential-Processing and Blend-Casting

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Energy & Environmental Materials 2024年第4期7卷 247-254页

作者： Guoping Zhang Chaoyue Zhao Liangxiang Zhu Lihong Wang Wenzhao Xiong Huawei Hu Qing Bai Yaping Wang Chen Xie Peng You He Yan Dan Wu Tao Yang Mingxia Qiu Shunpu Li Guangye Zhang College of New Materials and New Energies Shenzhen Technology University department of Chemistry and Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction The Hong Kong University of Science and Technology State Key Laboratory for Modification of chemical Fibers and polymer Materials Center for Advanced Low-dimension Materials College of Materials Science and Engineering Donghua University Julong College Shenzhen Technology University

The emergence of polymerized small molecule acceptors (PSMAs) has significantly improved the performance of all-polymer solar cells (all-PSCs).However,the pace of device engineering lacks behind that of materials deve... 详细信息

关键词： all-polymers solar cells sequential processing solid additive

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Advanced oxidation via the synergy of C-defective/C-O band modified ultrathin porous g-C3N4 and PMS for efficient photothermal degradation of bisphenol pollutants and lignin derivatives

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Green Energy & Environment 2024年第7期9卷 1159-1170页

作者： Liquan Jing Meng Xie Yuanguo Xu Chun Tong Xia Du Heng Zhao Na Zhong Huaming Li Jinguang Hu School of Chemistry and chemical Engineering Jiangsu University department of chemical and Petroleum Engineering University of Calgary School of Pharmacy Jiangsu University School of Material Science & chemical Engineering Harbin University of Science and Technology Institute for Energy Research Jiangsu University

This work uses thermal polymerization of urea nitrate, oxyacetic acid and urea as the raw material to prepare ultra-thin porous carbon nitride with carbon defects and C-O band（OA-UN-CN）. Density functional theory（DFT） calculations showed OA-UN-CN had narrower band gap,faster electron transport and a new internal construction electric field. Additionally, the prepared OA-UN-CN significantly enhanced photocatalytic activation of peroxymonosulfate（PMS） due to enhanced light absorption performance and faster electron overflow. As the result, the OA-UN-CN/PMS could entirely degrade bisphenol A（BPA） within 30 min, where the photodegradation rate was 81.8 and 7.9 times higher than that of g-C3N4and OA-UN-CN, respectively. Beyond, the OA-UN-CN/PMS could likewise degrade other bisphenol pollutants and sodium lignosulfonate efficiently. We suggested possible photocatalytic degradation pathways accordingly and explored the toxicity of its degradation products. This work provides a new idea on the development of advanced photocatalytic oxidation processes for the treatment of bisphenol pollutants and lignin derivatives, via a metal-free photothermal-catalyst.

关键词： Photothermal-catalytic G-C 3 N 4 Peroxymonosulfate Bisphenol Sodium lignosulfonate

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Preparing cyclic polymers at high concentrations via self-folding cyclization technique by adjusting the contents of hydrophilic units in linear precursors

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Chinese chemical Letters 2024年第2期35卷 283-288页

作者： Hao Zha Zuowei Wang Chao Liu Chunyan Hong department of polymer Science and Engineering University of Science and Technology of ChinaHefei 230026China Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China

Cyclic polymers are a class of polymers that feature endless topology,and the synthesis of cyclic polymers has attracted the attention of many ***,cyclic polymers were efficiently constructed by self-folding cyclization technique at high *** poly((oligo(ethylene glycol)acrylate)-co-(dodecyl acrylate))(P(OEGA-co-DDA))precursors with different ratios of hydrophilic and hydrophobic moieties were synthesized by reversible addition-fragmentation chain transfer(RAFT)polymerization using a bifunctional chain transfer agent with two anthryl end *** amphiphilic linear precursors underwent the self-folding process to generate polymeric nanoparticles in *** irradiating the aqueous solution of the nanoparticles with 365 nm UV light,cyclic polymers were synthesized successfully via coupling of anthryl *** effects of the ratios of hydrophilic and hydrophobic moieties in linear P(OEGA-co-DDA)copolymers and polymer concentration on the purity of the obtained cyclic polymers were explored in detail via ^(1)H nuclear magnetic resonance(^(1)H NMR),dynamic light scattering(DLS),UV‒visible(vis)analysis,three-detection size exclusion chromatography(TD-SEC)and transmission electron microscopy(TEM).It was found that by adjusting the content of the hydrophilic segments in linear precursors,single chain polymeric nanoparticles(SCPNs)can be generated at high polymer ***,cyclic polymers with high purity can be constructed *** method overcomes the limitation of traditional ring-closure method,which is typically conducted in highly dilute conditions,providing an efficient method for the scalable preparation of cyclic polymers.

关键词： Cyclic polymers Self-folding cyclization technique Single chain polymeric nanoparticles RAFT polymerization Direct visualization

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Multi-Objective Optimization Algorithm for Grouping Decision Variables Based on Extreme Point Pareto Frontier

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Computers, Materials & Continua 2024年第4期79卷 1281-1299页

作者： JunWang Linxi Zhang Hao Zhang Funan Peng Mohammed A.El-Meligy Mohamed Sharaf Qiang Fu College of Computer Science and technology Shenyang University of Chemical TechnologyShenyang110142China Key Laboratory of Intelligent technology for chemical Process Industry of Liaoning Province Shenyang University of Chemical TechnologyShenyang110142China Industrial Engineering department College of EngineeringKing Saud UniversityP.O.Box 800Riyadh11421Saudi Arabia

The existing algorithms for solving multi-objective optimization problems fall into three main categories:Decomposition-based,dominance-based,and *** multi-objective optimization problemsmainly focus on objectives,treating decision variables as a total variable to solve the problem without consideringthe critical role of decision variables in objective *** seen,a variety of decision variable groupingalgorithms have been ***,these algorithms are relatively broad for the changes of most decisionvariables in the evolution process and are time-consuming in the process of finding the Pareto *** solvethese problems,a multi-objective optimization algorithm for grouping decision variables based on extreme pointPareto frontier(MOEA-DV/EPF)is *** algorithm adopts a preprocessing rule to solve the Paretooptimal solution set of extreme points generated by simultaneous evolution in various target directions,obtainsthe basic Pareto front surface to determine the convergence effect,and analyzes the convergence and distributioneffects of decision *** the later stages of algorithm optimization,different mutation strategies are adoptedaccording to the nature of the decision variables to speed up the rate of evolution to obtain excellent individuals,thusenhancing the performance of the *** validation of the test functions shows that this algorithmcan solve the multi-objective optimization problem more efficiently.

关键词： Multi-objective evolutionary optimization algorithm decision variables grouping extreme point pareto frontier

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An approach of the internal friction-dependent temperature changes for conventional and pure biogenic lubricating greases

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Friction 2024年第4期12卷 780-795页

作者： Leif AHME Erik KUHN MiguelÁngel DELGADO department of Mechanical Engineering and Production Management Hamburg University of Applied SciencesHamburg 20099Germany department of chemical Engineering Research in Product Technology and Chemical Processes(Pro2TecS)University of HuelvaHuelva 21071Spain

This work investigated the temperature changes inside the bulk of lubricating greases under controlled high-shear stress conditions(250-500 s-1).For this purpose,a newly developed temperature-measuring cell called Calidus was successfully *** temperature changes(ΔT)have been related to the greases'components(thickener,base oil-type,and composition)and the structural degradation of the lubricating ***,a theoretical approach was proposed for calculating the internal temperature change of lubricating greases during shear *** greases showed an internal temperature profile characterised by a sudden rise inΔT within the first 4 h from starting the test and subsequentΔT decay until it reaches the steady state ***,it was found that greases C1 and C5,formulated with lithium and calcium soap,respectively,with different soap content(16.1 wt%and 9.7 wt%,respectively),but the same base castor oil,showed the highest value of the maximumΔT,c.a.3.2 K,and the most drastic drop ofΔ*** greases showed both the highest specific densities and heat *** addition,they showed the lowest ratio of expended energies(Rtee),which means more structural degradation in the stressed *** the contrary,the grease C3,with 13 wt%of Li-soap but the lowest base oil's viscosity,showed the lowest maximumΔT and the temperature profile was characterised by a moderate variation ofΔT along the *** biogenic grease B3 developed a low-temperature change in the group of pure bio-genic greases close to grease C3.

关键词： shear-induced structural degradation rheology temperature measurements lubricating greases density lubricating greases specific heat capacities

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Segregation of binary particles in gas-solid fluidized bed

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Frontiers of chemical Science and Engineering 2024年第6期18卷 113-121页

作者： Yaxiong Yu Feng Lu Xuan He Fei Wei Chenxi Zhang Beijing Key Laboratory of Green chemical Reaction Engineering and technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China School of chemical Engineering and technology Xi’an Jiaotong UniversityXi’an 710049China Ordos Laboratory Ordos 017010China Institute for Carbon Neutrality Tsinghua UniversityBeijing 100084China

Particle segregation and mixing behavior play a crucial role in industrial *** study investigates the saturated jetsam fraction,which indicates the maximum capacity of flotsam to entrain jetsam,in an initially separated binary fluidized bed with particle size *** to the value of saturated jetsam fraction,three distinct regimes-segregation,mixing,and an intermediate regime-are ***,intriguing relationships between the saturated jetsam fraction and superficial gas velocity are observed,exhibiting monotonic trends in both the segregation and mixing regimes,while a unique volcano-shaped curve in the intermediate ***,a comprehensive entrainment model based on two-fluid model elucidates the observed phenomena,emphasizing the significance of mixing behavior in fluidized layer on the saturated jetsam *** work offers potential insights for evaluating segregation in industrial applications.

关键词： fluidized bed segregation binary bubbles entrainment

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