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Suppression of current-induced membrane discharge of bipolar membranes by regulating ion crossover transport

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Journal of Energy Chemistry 2024年第9期96卷 387-395页

作者： Tingting Yu Haolan Tao Jingkun Li Cheng Lian Honglai Liu State Key laboratory of chemical engineering Shanghai Engineering Research Center of Hierarchical NanomaterialsSchool of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China School of Chemistry and Molecular engineering East China University of Science and TechnologyShanghai 200237China

Bipolar membranes(BPMs)exhibit the unique capability to regulate the operating environment of electrochemical system through the water dissociation-combination ***,the industrial utilization of BPMs is limited by instability and serious energy *** current-induced membrane discharge(CIMD)at high-current conditions has a negative influence on the performance of anion-exchange membranes,but the underlying ion transport mechanisms in the BPMs remain ***,the CIMD-coupled Poisson-Nernst-Planck(PNP)equations are used to explore the ion transport mechanisms in the BPMs for both reverse bias and forward bias at neutral and acid-base *** is demonstrated that the CIMD effect in the reverse-bias mode can be suppressed by enhancing the diffusive transport of salt counter-ions(Na^(+)and Cl^(−))into the BPMs,and that in the forward-bias mode with acid-base electrolytes can be suppressed by matching the transport rate of water counter-ions(H_(3)O^(+)and OH^(−)).Suppressing the CIMD can promote the water dissociation in the reverse-bias mode,as well as overcome the plateau of limiting current density and reduce the interfacial blockage of salt co-ions(Cl^(−))in the anion-exchange layer in the forward-bias mode with acid-base *** work highlights the importance of regulating ion crossover transport on improving the performance of BPMs.

关键词： Bipolar membranes Current-induced membrane discharge Salt ion crossover Diffusion-migration-reaction process

Surface chemical microenvironment engineering of catalysts by organic molecules for boosting electrocatalytic reaction

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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

A multifunctional electrolyte additive for zinc-ion capacitors with low temperature resistant and long lifespan

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Journal of Energy Chemistry 2024年第7期94卷 477-485页

作者： Ming Sun Zekai Zhang Shuqing Fu Yifan Zhang Ruoyu Wang Hongchun Mu Cheng Lian Wenqiang Wang Gengchao Wang Shanghai engineering Research Center of Hierarchical nanomaterials Shanghai Key Laboratory of Advanced Polymeric MaterialsSchool of Materials Science and EngineeringEast China University of Science and TechnologyShanghai 200237China State Key laboratory of chemical engineering Shanghai Engineering Research Center of Hierarchical NanomaterialsFrontiers Science Center for Materiobiology and Dynamic Chemistryand School of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China State Key laboratory of Molecular engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200438China

Aqueous zinc-ion capacitors (ZICs) are considered as potential candidates for next generation electrochemical energy storage devices due to their high safety and low ***,the existing aqueous ZICs usually have the problems of zinc dendrite growth and unsatisfactory performance at low ***,an erythritol (Eryt) additive with inhibition of zinc dendrites and anti-freezing capability was introduced into the *** experimental characterization and theoretical calculation confirm that the Eryt adsorbed on the surface of zinc anodes regulates the deposition orientation of Zn^(2+) and inhibits the formation of *** also reconstructs the solvation structure in the electrolyte to reduce water activity,enabling the electrolyte to have a lower freezing point for operation at low *** the assistance of Eryt,the Zn||Zn symmetric cell exhibits a long cycle life of 2000 h,while the ZIC assembled with activated carbon (AC) cathode and zinc anode (Zn||AC) maintains a capacity retention of 98.2% after 30,000 cycles at a current density of 10 A g^(-1)(even after 10,000 cycles at-20°C,the capacity retention rate reached 94.8%.).This work provides a highly scalable,low-cost and effective strategy for the protection of the anodes of low-temperature aqueous ZICs.

关键词： Zinc-ioncapacitors Electrolyte additive Dendrite-free Freeze-resistant electrolyte

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