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Enhanced interlayer interaction in sulfonated CONs membrane by amino-rich CONs enabling ultrafast proton transport

Green Energy & Environment 2025年第4期10卷 821-833页

作者： Ping Li Bo He Xuan Li Yunfei Lin Shaokun Tang Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjinChina School of Chemistry and Chemical Engineering Hainan UniversityHaikouChina

Covalent organic framework nanosheets(CONs)with porous crystalline features and ultrathin thickness are ideal candidates as membrane building blocks to form well-defined transfer *** formidable challenge behind self-supporting CONs membrane lies in weak noncovalent interlayer interactions and thus loose stacking,insufficient strength and structure ***,we propose the fabrication of interlayer force-strengthened freestanding CONs membrane through the electrostatic attraction bridge effect of positively-charged amino-rich CONs(CON-NH2)to negatively-charged sulfonated CONs(CON-SO_(3)H).Ultrathin and large lateral sized CON-SO_(3)H and CON-NH2 are synthesized,followed by restacking to prepare freestanding CONs membrane with CON-SO_(3)H as the membrane *** from effective interlayer interconnection due to strong electrostatic interaction,the obtained CON-SO_(3)H/CON-NH2 membrane displays features of ultrahigh integrity,dense stacking,eminent water/acid/base/organic solvents stabilities and mechanical strength(109 MPa).The shortened-SO_(3)H distance contributes to construct site-continuous transfer pathways,and the deprotonated-SO_(3)H and protonated-NH2 form acid-base pairs to decrease interfacial resistance,which impart membrane superior proton conductivity of 486 mS cm^(-1)(80℃,100%RH).This interlayer force enhancement strategy offers a promising perspective on achieving densely-stacked CONs membrane with ultrahigh mechanical property and conduction performance for fuel cell application.

关键词： Covalent organic framework nanosheet Self-supporting membrane Interlayer interaction Stability Proton conductivity

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Graphdiyne(C_(n)H_(2n-2))as an"electron transfer bridge"boosting photocatalytic hydrogen evolution over Zn_(0.5)Co_(0.5)S/MoS_(2)S-scheme heterojunction

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Rare Metals 2024年第5期43卷 1999-2014页

作者： Mei Li Jing-Zhi Wang Zhi-Liang Jin School of Chemistry and Chemical Engineering North Minzu UniversityYinchuan 750021China School of Chemistry and Chemical Engineering Ningxia Key Laboratory of Solar Chemical Conversion TechnologyKey Laboratory for Chemical Engineering and TechnologyState Ethnic Affairs CommissionNorth Minzu UniversityYinchuan 750021China

In the process of photocatalytic water cracking,the migration rate and utilization rate of photogenerated charges determine the hydrogen evolution performance of the *** this paper,a carbon isotope superconducting material graphdiyne(GDY)is prepared by mechanical ball milling and introduced into the S-scheme heterojunction Zn_(0.5)Co_(0.5)S/MoS_(2)inorganic *** terms of hydrogen evolution kinetics,GDY acts as an electron bridge,not only accelerating the migration of photogenerated carriers but also improving the utilization of photogenerated ***,the large twodimensional layer provides more loading and anchoring points for Zn_(0.5)Co_(0.5)S/MoS_(2),which increases the number of active *** ternary composite catalyst 20%GDY/Zn_(0.5)Co_(0.5)S/MoS_(2)(20-GCSM)generates 69.94μmol of hydrogen(5 h)in triethanolamine *** is 2.97 and1.80 times higher than Zn_(0.5)Co_(0.5)S and Zn_(0.5)Co_(0.5)S/MoS_(2),*** the cyclic experiment,it still has stable hydrogen evolution performance after standing for24 h(under dark conditions).In addition,the potential mechanism of photocatalytic hydrogen evolution is demonstrated through in-situ X-ray photoelectron *** work provides a reference for further research in the field of introducing carbon materials into photocatalytic systems and improving the utilization of photogenerated charges.

关键词： Graphdiyne S-scheme heterojunction Electron transfer bridge Hydrogen production

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Wall-scaling prevention in cryogenic external cooler of ammonium chloride solution by liquid-solid fluidization

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Particuology 2024年第11期94卷 120-132页

作者： Yusu Zhu Yongli Ma Mingyan Liu School of Chemical Engineering and Technology Tianjin UniversityTianjin300350China State Key Laboratory of Chemical Engineering(Tianjin University) Tianjin300350China

A double-tube cooler with liquid-solid circulating fluidization operation and corresponding parameter measuring system are developed to avoid fouling of inner walls of heat exchange tubes in a cryogenic temperature external cooler of ammonium chloride solution in soda ash ***-scaling prevention performance of the cooling process is experimentally evaluated using convection and overall coefficients,enhancement factor,wall temperature and fouling *** of different volume fractions of added particles,particle size,superficial liquid velocity,and cooling medium temperature on heat transfer are *** present conditions,convection coefficient of liquid-solid flow inside the tube of external cooler is higher than that of the liquid phase flow,increased by 0.7–2.8 times,enhancing cooling performance *** coefficient initially increases and then decreases as the volume fraction of added particles increases,reaching its maximum value at a volume fraction of 2.0%.The wall-scaling prevention effect of glass beads mainly depends on the volume fraction of added particles;optimal anti-fouling effects are achieved when adding particles at a volume fraction of 2.0%,regardless of changes in superficial liquid velocity or cooling medium *** study lays a foundation for industrial applications of this new technique of fluidized bed external coolers.

关键词： Fouling Liquid-solid circulating fluidized bed External cooler Two-phase flow Ammonium chloride

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Mixing characteristics of three-cylinder valve-controlled energy recovery device based on liquid piston

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Chinese Journal of chemical engineering 2024年第10期74卷 83-91页

作者： Zheng Sun Zean Chen Weian Li Yue Wang Jing Yang School of Resources&Chemical Engineering Sanming UniversitySanming 365004China Chemical Engineering Research Center School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China State Key Laboratory of Chemical Engineering Tianjin 300072China

The isobaric energy recovery device can significantly reduce the energy consumption of the seawater reverse osmosis system by recycling the residual pressure energy of high-pressure concentrated ***-cylinder valve-controlled energy recovery device(TC-ERD)solves the fluid pulsation of traditional two-cylinder devices,but the use of a“liquid piston”exacerbates the mixing between brine and ***,the evolutionary law of“liquid piston”and the relationship between volumetric mixing degree and operating conditions are *** results show that the“liquid piston”first axially expands and then gradually stabilizes,isolating the brine and ***,as long as the volume utilization ratio(U_(R))of the pressure exchange cylinder remains constant,there will not be much difference in the volumetric mixing degree after stabilization of the“liquid piston”(Vm-max)regardless of changes in the processing capacity(Q)and cycle time(T_(0)).Therefore,the equation for Vm-max with respect to the operating parameters(Q,T_(0))is derived,which can not only predict the Vm-max of the TCERD,but also provide an empirical reference for the design of other valve-controlled devices with“liquid piston”.When the Vm-max is 6%,the efficiency of the TC-ERD at design conditions(30 m^(3)·h^(-1),5.0 MPa)is 97.53%.

关键词： Desalination Energy Recovery Mixing Liquid piston

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Transition metal sulfides in alkaline hydrogen evolution electrocatalysis:Re-exploring their structure and composition evolution and its correlation with activity

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Nano Research 2025年第3期18卷 153-168页

作者： Chengqi Wu Jiaqi Liu Yiwei Tan State Key Laboratory of Materials-Oriented Chemical Engineering School of Chemistry and Chemical EngineeringNanjing Tech UniversityNanjing 211816China

Herein,the activity and stability evolution of transition metal sulfides used as electrocatalysts for alkaline hydrogen evolution reaction(HER)are studied during a prolonged HER *** have thoroughly characterized and analyzed the composition and structure of NiV_(2)S_(4),NiS,Ni_(3)S_(2),and VS_(2)prior to HER and after the HER for 2-20 h at a constant current density of−100 mA·cm^(−2).It is found that all these metal sulfides in KOH electrolyte are gradually degraded to the corresponding amorphous metal hydroxy salts/oxysulfides(i.e.,a-KNi(OH)3/a-NiO_(x)S_(y)and a-KV(OH)_(6)/a-VO_(x)S_(y))and finally to amorphous metal hydroxy salts/oxides(i.e.,a-KNi(OH)_(3)and a-KV(OH)_(6)/a-V_(2)O_(3))from surface to bulk with elongating HER ***,the morphologies of the derived metal hydroxy salts/oxysulfides(oxides)are significantly different from the corresponding metal sulfide precursors,especially those containing metal ions(for example,V3+in NiV2S4 and Ni+in Ni_(3)S_(2))in intermediate valence states due to the modification of chemical bonds to an extensive extent invoked by their capability of facilely accepting and donating *** stability and structural evolution of these metal sulfides are substantiated by the calculated Pourbaix diagrams of Ni-S-H_(2)O and Ni-V-S-H_(2)O *** the HER at−100 mA·cm^(−2)for 20 h,compared to the corresponding pristine metal sulfides,the apparent HER activities of all the derived metal hydroxy salts/oxide decrease due to the diminution of their electrochemically active surface areas(ECSAs).On the contrary,their specific activities increase due to the enriched structural defects caused by the amorphous structures and changes in valence state of the metal ions.

关键词： hydrogen evolution reaction transition metal sulfides alkaline water electrolysis amorphous structures metal hydroxy salts Pourbaix diagrams

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Synthetic auxotrophs accelerate cell factory development through growth-coupled models

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Frontiers of chemical Science and engineering 2024年第9期18卷 73-87页

作者： Liangpo Li Linwei Yu Xinxiao Sun Qipeng Yuan Xiaolin Shen Jia Wang State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China

The engineering of microbial cell factories for the production of high-value chemicals from renewable resources presents several challenges,including the optimization of key enzymes,pathway fluxes and metabolic *** these challenges involves the development of synthetic auxotrophs,a strategy that links cell growth with enzyme properties or biosynthetic *** linkage allows for the improvement of enzyme properties by in vivo directed enzyme evolution,the enhancement of metabolic pathway fluxes under growth pressure,and remodeling of metabolic networks through directed strain *** advantage of employing synthetic auxotrophs lies in the power of growth-coupled selection,which is not only high-throughput but also labor-saving,greatly simplifying the development of both strains and *** auxotrophs play a pivotal role in advancing microbial cell factories,offering benefits from enzyme optimization to the manipulation of metabolic networks within single ***,this strategy extends to coculture systems,enabling collaboration within microbial *** review highlights the recently developed applications of synthetic auxotrophs as microbial cell factories,and discusses future perspectives,aiming to provide a practical guide for growth-coupled models to produce value-added chemicals as part of a sustainable biorefinery.

关键词： synthetic auxotrophs growth-coupled directed enzyme evolution pathway flux directed strain evolution coculture

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Vanadium(V) Complexes Containing Unsymmetrical N-Heterocyclic Carbene Ligands: Highly Efficient Synthesis and Catalytic Behavior towards Ethylene/Propylene Copolymerization

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Chinese Journal of Polymer Science 2024年第1期42卷 32-41,I0006页

作者： Yi-Cong Wang Hui Zhat Pei-Yi Cheng Shu Zhang Xiang-Wei Liu Yi-Xian Wu State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBejing 100029China

The highly efficient method has been developed for the synthesis of NHC·VOCl_(3) containing symmetrical or unsymmetrical Nheterocyclic carbene(NHC) ligands by the transmetallation reaction of NHC·AgCl with VOCl_(3).The total isolated yield of VOCl_(3)[1,3-(2,4,6-Me_(3)C_(6)H_(2))_(2)(NCH=)_(2)C:](V4') reached 86% by transmetallation reaction,which is much higher than that(48%) by direct coordination *** methodology has also been used to synthesize the novel vanadium complexes containing unsymmetrical NHC ligands of VOCl_(3)[PhCH_(2)NCH=CHNR)C:](V5',R=2,4,6-Me_(3)C_(6)H_(2);V6',R=2,4-Me_(2)-6-Ph-C_(6)H_(2);V7',R=2,6-^(i)Pr_(2)-C_(6)H_(3)) with high yield,which could not be obtained by direct coordination *** catalytic activity and copolymerization ability would be improved by introducing unsymmetrical NHC ligands due to their less steric bulky *** vanadium complex V5' containing unsymmetrical NHC ligand exhibits higher catalytic activity(3.7×10^(5)g_(copolymer)·mol^(-1) of V·h^(-1)) than that of V4' containing symmetrical NHC ***,the higher propylene incorporation ratio(45.6 mol%) in the copolymers of ethylene with propylene could be obtained by using V5' than that(39.9%) by using V4'.The results would provide a highly efficient strategy for the synthesis of early transition metal complexes containing versitile NHC ligands,affording the catalyst with both high catalytic activity and copolymerization ability for the synthesis of high performance polyolefin elastomers.

关键词： Vanadium complex N-heterocyclic carbene ligand Transmetallation reaction Copolymerization of ethylene with propylene

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Sourcing the merits of 3D integrated air cathodes for highperformance Zn-air batteries by bubble pump consumption chronoamperometry

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Nano Research 2024年第8期17卷 6951-6959页

作者： Mengxuan Li Linfeng Yu Hai Liu Chuanyi Zhang Jiazhan Li Liang Luo Xiaoming Sun State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China

Zn-air batteries(ZABs)as a potential energy conversion system suffer from low power density(typically≤200 mW·cm^(−2)).Recently,three-dimensional(3D)integrated air cathodes have demonstrated promising performance over traditional twodimensional(2D)plane ones,which is ascribed to enriched active sites and enhanced diffusion,but without experimental ***,we applied a bubble pump consumption chronoamperometry(BPCC)method to quantitatively identify the gas diffusion coefficient(D)and effective catalytic sites density(ρEC)of the integrated air cathodes for ***,the D andρEC values can instruct consequent optimization on the growth of Co embedded N-doped carbon nanotubes(CoNCNTs)on carbon fiber paper(CFP)and aerophilicity tuning,giving 4 times D and 1.3 timesρEC over the conventional 2D Pt/C-CFP *** a result,using the CoNCNTs with half-wave potential of merely 0.78 V ***(Pt/C:0.89 V ***),the superaerophilic CoNCNTs-CFP cathode-based ZABs exhibited a superior peak power density of 245 mW·cm^(−2) over traditional 2D Pt/C-CFP counterparts,breaking the threshold of 200 mW·cm^(−2).This work reveals the intrinsic feature of the 3D integrated air cathodes by yielding exact D andρEC values,and demonstrates the feasibility of BPCC method for the optimization of integrated electrodes,bypassing trial-and-error strategy.

关键词： Zn-air batteries three-dimensional(3D)integrated air cathodes superaerophilic gas diffusion coefficient effective catalytic sites density

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Bubble breakup in viscous liquids at a microfluidic T-junction

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Chinese Journal of chemical engineering 2025年第2期78卷 44-57页

作者： Hongwei Zhu Junjie Feng Ziyi Xu Chunying Zhu Youguang Ma Wei Xu Bing Sun Taotao Fu SINOPEC Research Institute of Safety Engineering Co. Ltd. State Key Laboratory of Chemical Engineering School of Chemical Engineering and Technology Tianjin University

Bubble breakup at T-junction microchannels is the basis for the numbering-up of gas—liquid two-phase flow in parallelized microchannels. This article presents the bubble breakup in viscous liquids at a microfluidic T-junction. Nitrogen is used as the gas phase, and glycerol-water mixtures with different mass concentration of glycerol as the liquid phase. The evolution of the gas—liquid interface during bubble breakup at the microfluidic T-junction is explored. The thinning of the bubble neck includes the squeezing stage and the rapid pinch-off stage. In the squeezing stage, the power law relation is found between the minimum width of the bubble neck and the time, and the values of exponents a1and a2are influenced by the viscous force. The values of pre-factors m1and m2are negatively correlated with the capillary number. In the rapid pinch-off stage, the thinning of the bubble neck is predominated by the surface tension, and the minimum width of the bubble neck can be scaled with the remaining time as power-law. The propagation of the bubble tip can be characterized by the power law between the movement distance and the time, with decreasing exponent as increased liquid viscosity.

关键词： Breakup Bubble Microchannel Microfluidics Viscous fluid

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Effect of binder addition on combustion characteristics of cotton straw pellets and kinetic analysis

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Frontiers of chemical Science and engineering 2024年第10期18卷 133-143页

作者： Yiwen Dai Bin Guan Xingxiang Wang Jinli Zhang Bin Dai Jiangbing Li Jichang Liu School of Chemistry and Chemical Engineering/State Key Laboratory Incubation Base for Green Processing of Chemical Engineering Shihezi UniversityShihezi 832003China School of Chemical Engineering and Technology Tianjin UniversityTianjin 300350China

In this study,the combustion characteristics and kinetics of cotton straw(CS)particles mixed with polyethylene(PE)film and coal gangue(CG)were *** co-combustion characteristics of CS mixed with PE and CG at different heating rates were revealed by the thermogravimetric method and differential thermogravimetric *** ignition temperature,burnout temperature,and maximum weight loss rate were measured,and the comprehensive combustion and flammability indexes were *** results showed that the composite combustion characteristic index and flammability index increased with the increase in heating *** addition of PE and CG additives could effectively extend the combustion *** Coats-Redfern(C-R)reaction model and N-order reaction model were used to evaluate the kinetic parameters of the *** results showed that 12.5%PE+12.5%CG particles had the lowest activation energy(Ea=103.73 kJ·mol^(-1))at the volatile combustion *** dynamics conform to the third-order dynamics *** addition,the applicability of C-R model,Flynn-Wall-Ozawa(FWO)model,and Starink model in the calculation of activation energy was explored,and it was found that the FWO model is not suitable for the calculation of activation energy of biomass pellet combustion *** study provides a new method for the development and utilization of mixed fuel particles of cotton stalk and solid waste and expands the application prospect of biomass.

关键词： biomass straw pellet comprehensive combustion index flammability index combustion kinetics

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