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Chinese chemical Letters 2024年第8期35卷 15-24页

作者： Xianxu Chu Lu Wang Junru Li Hui Xu Henan Key laboratory of Biomolecular Recognition and Sensing College of Chemistry and Chemical EngineeringShangqiu Normal UniversityShangqiu 476000China Key laboratory of Advanced Catalytic Materials and Technology Advanced Catalysis and Green Manufacturing Collaborative Innovation CenterChangzhou UniversityChangzhou 213164China

Electrocatalysis is a surface-sensitive process,in which the catalytic activity of electrocatalyst highly re-lates to the surface adsorption/desorption behaviors of the reactants/intermediates/products on the cat-alytically active *** chemical microenvironment engineering via organic molecules functional-ization is a promising strategy to tune the electrocatalytic activity since it can well modify the elec-trode/electrolyte interface and alter the reaction *** this review,we summarize the recent progress of surface microenvironment engineering of electrocatalysts induced by organic molecules func-tionalization,with the special focus on the organic molecule-assisted growth mechanism and unique electronic *** importantly,the applications of organic molecule functionalized catalysts in var-ious electrocatalytic reactions are also systematically summarized,along with a deep discussion on the conclusion and *** work will open a new avenue for the construction and modification of advanced electrocatalysts based on organic molecule-mediated interface engineering.

关键词： chemical microenvironment engineering Organic molecules Electrocatalysis Functionalization Interface

Process intensification for the synthesis and purification of battery-grade Li_(2)CO_(3)with microfluidics

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Particuology 2024年第7期90卷 106-117页

作者： Haodu Li Jie Zhang Lin Dai Le Du Jiqin Zhu The State Key laboratory of chemical Resource engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Battery-grade lithium carbonate(Li_(2)CO_(3))with a purity of higher than 99.5 wt%is of great importance as a high value-added lithium ***,influences of different reaction systems and process control on product purity remain ***,a membrane dispersion microreactor was used to enhance the mass transfer of preparation and purification processes in homogeneous and heterogeneous *** systems of Na_(2)CO_(3)–LiCl,NH_(4)HCO_(3)–LiCl,and NH_(3)·H_(2)O−CO_(2)−LiCl,CO_(2)purification based on carbonation and decomposition were *** Li_(2)CO_(3)purity was increased by the improvement of mixing *** carbonation time was reduced by 62.5%and 58.3%for the NH_(3)·H_(2)O−CO_(2)and CO_(2)purification systems,*** the two ammonia-based systems,Li_(2)CO_(3)particles with a purity of 99.7–99.8 wt%were one-step prepared with a size of 3–5μm,which also met the requirement of the battery-grade *** purity was further increased to 99.9 wt%by CO_(2)purification and LiHCO_(3)*** investigation could provide a feasible alternative for the controllable preparation of battery-grade Li_(2)CO_(3)in one or multiple steps.

关键词： Microfluidics Battery grade Li_(2)CO_(3) Process intensification High purity

Microfluidic-oriented synthesis of enriched iridium nanodots/carbon architecture for robust electrocatalytic nitrogen fixation

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Green Energy & Environment 2024年第3期9卷 544-555页

作者： Hengyuan Liu Xingjiang Wu Yuhao Geng Xin Li Jianhong Xu The State Key laboratory of chemical engineering Department of Chemical EngineeringTsinghua UniversityBeijing100084China

Electrocatalytic nitrogen reduction reaction(NRR)is considered as a promising candidate to achieve ammonia synthesis because of clean electric energy,moderate reaction condition,safe operating process and harmless ***,the chemical inertness of nitrogen and poor activated capacity on catalyst surface usually produce low ammonia yield and faradic ***,the microfluidic technology is proposed to efficiently fabricate enriched iridium nanodots/carbon *** to in-situ co-precipitation reaction and microfluidic manipulation,the iridium nanodots/carbon nanomaterials possess small average size,uniform dispersion,high conductivity and abundant active sites,producing good proton activation and rapid electrons transmission and moderate adsorption/desorption *** a result,the as-prepared iridium nanodots/carbon nanomaterials realize large ammonia yield of 28.73 μg h^(-1) cm^(-2) and faradic efficiency of 9.14%in KOH ***,the high ammonia yield of 11.21 μg h^(-1) cm^(-2) and faradic efficiency of 24.30%are also achieved in H_(2)SO_(4) *** microfluidic method provides a reference for large-scale fabrication of nano-sized catalyst materials,which may accelerate the progress of electrocatalytic NRR in industrialization field.

关键词： Iridium nanodots Carbon Microfluidic technology Efficient synthesis Electrocatalytic nitrogen fixation

Insights into the role of oxygen-containing functional groups on carbon surface in water–electricity generation

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Nano Research 2024年第7期17卷 6645-6653页

作者： Wan Xue Zongbin Zhao Honghui Bi Bolun Zhang Xuzhen Wang Jieshan Qiu State Key laboratory of Fine chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China State Key laboratory of Fine chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of ChemistryDalian University of TechnologyDalian 116024China State Key laboratory of chemical Resource engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

A deep understanding of the electricity generation mechanism from the interaction between water molecules and carbon material surfaces is attractive for next-generation water-based energy conversion and storage ***,an asymmetric generator was assembled based on functionalized carbon nanotubes films to investigate the relative contribution from various oxygen functional groups on carbon surface to the water-electrical *** and calculations demonstrate that the electricity mainly originates from the water molecule adsorption by carboxyl groups and dissociation of functional groups on carbon surface,which leads to the formation of electrical double layers at *** device allows the electricity generation with a variety of water sources,such as deionized water,tap water,as well as *** particular,the generator based on carboxyl carbon nanotubes can induce a voltage of over 200 mV spontaneously in natural seawater with the power density of about 0.11 mW·g^(−1).High voltages can be achieved easily through the series-connection strategy to power electronic products such as a liquid crystal *** work reveals the dominant role of carboxyl groups in carbon-based water–electricity conversion and is expected to offer inspiration for the preparation of carbon materials with high electrical performance.

关键词： electricity generation water adsorption dissociation carboxyl groups carbon nanotubes

Controllable Ring-opening Polymerization ofδ-Valerolactone Catalyzed by Quinolinyl-Urea/MTBD Systems

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Chinese Journal of Polymer Science 2024年第8期42卷 1103-1110页

作者： Xin-Yu Liu Liang Zhu Su-Yun Jie Bo-Geng Li State Key laboratory of chemical engineering College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310058China

Due to their excellent biocompatibility and biodegradability,aliphatic polyesters are widely used in the biomedical,packaging and agricultural fields,which are usually accessed by the ring-opening polymerization(ROP)of lactones and the catalysts particularly play an important *** a series of quinolinyl-urea catalysts have been synthesized via the reaction between isocyanate and aminoquinoline with an amino group at different substitution positions and *** combination with 7-methyl-1,5,7-triazabicyclo[4,4,0]dec-5-ene(MTBD)as a cocatalyst and benzyl alcohol(BnOH)as an initiator,1-(3,5-bis(trifluoromethyl)phenyl)-3-(quinolin-3-yl)urea(3-QU)was observed to be most active for the ROP ofδ-valerolactone(δ-VL).The polymerization conditions were optimized by varying the type of organic base,catalyst concentration and reaction *** changing the ratio of[M]_0/[I],linear polyvalerolactones(PVLs)with different molecular weights and narrow molecular weight distribution were *** kinetic and chain extension experiments were carried out to prove the"living"/controllable *** the NMR experiments were used to support the proposal of possible mechanism.

关键词： Quinolinyl-urea Ring-opening polymerization PVL

AI in chemical engineering: A New Chapter of Innovation

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engineering 2024年第8期39卷 1-2页

作者： Qilong Ren Key laboratory of Biomass chemical engineering of the Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Instiute of Zhejiang Universiy-Quzhou Quzhou 324000China

The integration of artificial intelli-gence(AI)into chemical engineering marks a transformative era,redefin-ing traditional methodologies with AI-driven *** has emerged as a powerful ally in tackling complex problems once considered *** chemical engineering grapples with increasingly complex systems and stringent sustainability targets,AI sets the stage for a new generation of solutions.

关键词： mount AI emerged

Antibonding orbital tailor and stress relief engineering for FeS2 complex toward superior sodium storage

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Rare Metals 2024年第10期43卷 5048-5059页

作者： You-Bin Zhang Zhen-Guo Qi Fu-Sheng Liu Guo-Hui Qin State Key laboratory Base for Eco-chemical engineering College of Chemical EngineeringQingdao University of Science and Technology Shandong Synergetic Innovation Center of Ecological and chemical engineering

The sluggish kinetics behaviors and vast volume variations of Na+hosts to FeS2anode involved intercalation,and conversion reactions plague its applicability of sodium-ion batteries （SIBs）.Here,a significantly expedited kinetics via cation intercalation and considerably relieved stress accumulation by constructing the concave scaffold protector are approached for *** Mn2+intercalation into FeS2,a new stable Mn–FeS2was generated with distorted coordination;elevated antibonding orbital occupancy and lowed d band center to the release of more free Na+were achieved,which was further encapsulated by hollow bowl-like carbon spheres （BC）This cation intercalation and concave morphology strategies confer Mn–FeS2@BC significantly enhanced electron ion transport kinetics via reversed electron transfer to FeS2fast desolvation kinetics,and evidently depressed structural deformation during Na+insertion and ***,Mn–FeS2@BC delivers the longevity and stable Na+storage capacity in both half and full cell ***,Mn–FeS2@BC also displays excellen adaptability in a wider temperature *** work proposes new views into the deep regulation of electrochemical performance of transition metal anodes via intercalation chemistry and concave engineering.

关键词： Concave engineering FeS2 Intercalation chemistry Sodium capture

Impact of Carbon Chain Structures in the Backbone on the Flexibility of Modified Polyarylene Sulfide Resins: Molecular Dynamics Simulations and Mesoscopic Analysis

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Chinese Journal of Polymer Science 2024年第4期42卷 544-557页

作者： Chi Zhang Rong Liu Jing-Yuan Liu Wen-Wei Jiang Key laboratory of Fine chemical engineering and Functional Materials School of Chemical EngineeringSichuan UniversityChengdu610065China

In the domain of high-performance engineering polymers, the enhancement of mechanical flexibility in poly(phenylene sulfide) (PPS) resins has long posed a significant challenge. A novel molecular structure, designated as PP-He-IS, wherein imide rings and an aliphatic hexylene chain are covalently incorporated into the PPS backbone to enhance its flexibility, is introduced in this study. Molecular dynamics (MD) simulations are employed to systematically explore the effects of diversifying the backbone chain structures by substituting phenyl units with alkyl chains of varying lengths, referred to as PP-A-IS where “A” signifies the distinct intermediary alkyl chain configurations. Computational analyses reveal a discernable decrement in the glass transition temperature (Tg) and elastic modulus, counterbalanced by an increment in yield strength as the alkyl chain length is extended. Notably, the PP-He-IS variant is shown to exhibit superior yield strength while simultaneously maintaining reduced elastic modulus and Tg values, positioning it as an advantageous candidate for flexible PPS applications. Mesoscopic analyses further indicate that structures such as PP-He-IS, PP-Pe-IS, and PP-Bu-IS manifest remarkable flexibility, attributable to the presence of freely rotatable carbon-carbon single bonds. Experimental validation confirms that a melting temperature of 504 K which is lower than that of conventional PPS, and lower crystallinity are exhibited by PP-He-IS, thereby affording enhanced processability without compromising inherent thermal stability. Novel insights into the strategic modification of PPS for mechanical flexibility are thus furnished by this study, which also accentuates the pivotal role played by molecular dynamics simulations in spearheading high-throughput investigations in polymer material modifications.

关键词： Molecular dynamics simulations Polyarylene Sulfide Main-chain modifications Flexibility Aliphatic hexylene chain

NaBH4-induced phase transition of CoSe_(2) with abundant Se deficiency for acidic oxygen reduction to hydrogen peroxide

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Rare Metals 2024年第2期43卷 500-510页

作者： Cai-Di Han Yong-Chao Zhang Qian Zhang Jin-Ting Wu Jian Gao Ji-Jun Zou Xiao-Dong Zhu State Key laboratory Base of Eco-chemical engineering College of chemical engineering Qingdao University of Science and TechnologyQingdao266042China Key laboratory for Green chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

Electrocatalytic oxygen reduction(ORR)via the 2e−pathway to form H_(2)O_(2) in acidic medium has attracted extensive ***,the low activity,insufficient selectivity and high cost of catalysts have been the ***,CoSe_(2) with abundant Se deficiency was synthesized by a simple hydrothermal method,and the addition of NaBH4-induced CoSe_(2) phase transition from orthorhombic to cubic phase with more Se *** cubic phase CoSe_(2) with abundant Se deficiency can effectively regulate the surface electronic structure with suitable binding energies of*OOH and*O,which shows high activity,selectivity and long-term stability for acidic ORR to H_(2)O_(2).The onset potential is as low as 0.73 V *** hydrogen electrode(RHE),the H_(2)O_(2) selectivity is 84%(0 V ***),and the average electron transfer number is about ***,the H_(2)O_(2) yield measured using a flow cell is as high as 115.92 mmol·gcat.^(−1)·h^(−1) and the Faradaic efficiency is 70%at 0 V ***,which presents high potential in electrocatalytic acidic ORR to H_(2)O_(2) and organic pollutant degradation using the electron-Fenton process.

关键词： Se defected CoSe_(2) Crystal phase transition Electrocatalysis Acidic oxygen reduction Hydrogen peroxide

Highly sensitive fluorescent sensing and photocatalytic degradation performance of two-dimensional Tb-organic network

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Journal of Rare Earths 2024年第2期42卷 303-313,I0003页

作者： Ting Gao Zhihu Ma Yixia Ren Zhixiang Wang Meili Zhang Xiaoli Chen Jijiang Wang laboratory of New Energy and New Function Materials Shaanxi Key Laboratory of Chemical Reaction EngineeringCollege of Chemistry and Chemical EngineeringYan'an UniversityYan'an716000China

A novel tetra-nuclear Tb-organic network,named as [Tb_(4)(2-pyia)_(6)(HAc)_(0.5)(2,2'-bipy)(H_(2)O)_(4.5)]·2,2'-bipy·H_(2)O(1),was synthesized hydrothermally based on 5-(pyridin-2-ylmethoxy) isophthalic acid(H_(2)pyia) and 2,2'-bipyridine(2,2'-bipy) ligands,and characterized by single crystal X-ray diffraction,thermogravimetric(TG) analyses,powder X-ray diffraction(PXRD) and infrared(IR) technology.1 possesses a two-dimensional network based on the tetra-nuclear inorganic building units,and the π-πstacking interactions between the pyia^(2-) ligands and the guest 2,2'-bipy molecules play an important role in the forming of 3D supramolecular structure.1 exhibits excellent fluorescent sensing performance for Fe^(3+)(1.26×10^(-8) mol/L),Cr_(2)O_(7)^(2-)(8.1×10^(-7) mol/L),2,4,6-trinitrophenol(TNP)(2.71×10^(-8) mol/L)and tetracycline(TCT)(2.76×10^(-7) mol/L) in aqueous solution with lower detection *** sensing mechanisms of 1 were investigated by density functional theory(DFT) calculations,ultraviolet-visible(UV-Vis) diffuse reflectance spectroscopy,PXRD and fluorescent lifetime *** activated product of 1 was prepared by heating at 255℃ under constant pressure and used to photo-catalytically degrade *** 1 and the activated one have good photocatalytic degradation performance for TCT with degradation rates of 84.29% and 96.07%,*** photocatalytic mechanisms were discovered by UV-Vis diffuse reflectance spectroscopy and radical trap *** Tb-organic framework might be an excellent multifunctional fluorescent sensor and a good photocatalytic agent for TCT degradation in the future.

关键词： Tb-organic network Fluorescent sensing Photocatalytic degradation Rare earths