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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

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

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

Tailoring NH4+ storage by regulating oxygen defect in ammonium vanadate

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Green Energy & Environment 2024年第7期9卷 1171-1182页

作者： Yanyan Liu Ziyi Feng Hanmei Jiang Xueying Dong Changgong Meng Yifu Zhang State Key laboratory of Fine chemicals School of Chemical Engineering Dalian University of Technology College of Environmental and chemical engineering Dalian University

Defect engineering is an effective strategy for modifying the energy storage materials to improve their electrochemical ***, the impact of oxygen defect and its content on the electrochemical performances in the burgeoning aqueous NH+4storage field remains explored. Therefore, for the first time in this work, an oxygen-defective ammonium vanadate [（NH4）2V10O25·8H2O, denoted as Od-NHVO] with a novel 3D porous flower-like architecture was achieved via the reduction of thiourea in a mild reaction condition, which is a facile method that can realize the intention to regulate the oxygen defect content, with the capability of mass-production. The as-prepared OdM-NHVO with moderate oxygen defect content can deliver a stable specific capacitance output(505 F g-1, 252 mAh g-1at 0.5 A g-1with ～80% capacitance retention after 10,000 cycles), which benefits from extra active sites, unimpeded NH+4-migration path and relatively high structure integrity. In contrast, low oxygen defect content will lead to the torpid electrochemical reaction kinetics while too high content of it will reduce the chargestorage capability and induce structural disintegration. The superior NH+4-storage behavior is achieved with the reversible intercalation/deintercalation process of NH+4accompanied by forming/breaking of hydrogen bond. As expected, the assembled flexible OdM-NHVO//PTCDI quasi-solid-state hybrid supercapacitor（FQSS HSC） also exhibits high areal capacitance, energy density and reliable flexibility. This work provides a new avenue for developing materials with oxygen-deficient structure for application in various aqueous non-metal cation storage systems.

关键词： Ammonium vanadate Oxygen defect Ammonium-ion storage Hybrid supercapacitors Electrochemical performance

Amorphous hybrid tungsten oxide–nickel hydroxide nanosheets used as a highly efficient electrocatalyst for hydrogen evolution reaction

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Nano Research 2024年第4期17卷 2499-2508页

作者： Chao Lyu Chenghai Dai Yiwei Tan State Key laboratory of Materials-Oriented chemical engineering School of Chemistry and Chemical EngineeringNanjing Tech UniversityNanjing 211816China

There are more challenges for alkaline hydrogen evolution reaction(HER)via simultaneously expediting the electron-coupled water dissociation process(Volmer step)and the following electrochemical H_(2) desorption(Heyrovsky step).Hybrid amorphous electrocatalysts are highly desirable for efficient hydrogen evolution from water-alkali electrolyzers due to the bifunctionality for the different elementary steps of HER and optimal interactions with water molecules and the reactive hydrogen intermediates(Had).Herein,the synthesis of amorphous hybrid ultrathin(tungsten oxide/nickel hydroxide)hydrate(a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O)nanosheets on nickel foam(NF)for efficient alkaline HER is *** structural and composition features of a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O are characterized in *** resulting a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O/NF electrocatalyst with the synergistic effect of both hybrid components for the HER elementary steps shows greatly improved the activity and durability for the HER with a low overpotential of-41 and-163 mV at-10 and-500 mA·cm^(-2),respectively,a Tafel slope as low as-72.9 mV·dec^(-1),and long-term stability of continuous electrolysis for at least 150 h accompanying by inappreciable overpotential change in 1 M *** the hybrid a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O,Ni(OH)_(2) and WO_(3) moieties are separately responsible for accelerating dissociative adsorption of water and weakening Had adsorption strength,which is beneficial to the improvement of the alkaline HER activity.

关键词： amorphous nanomaterial bimetallic electrocatalyst tungsten oxide ultrathin nanosheet hydrogen evolution reaction

The flow behavior of droplet adsorption on a liquid-liquid interface accompanied by cross-linking reaction and phase separation in a microchannel

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Chinese Journal of chemical engineering 2024年第2期66卷 60-70页

作者： Haozhe Yi Taotao Fu Chunying Zhu Youguang Ma State Key laboratory of chemical engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

The adsorption process of droplets on the liquid-liquid interface and phase separation process can regulate the spatial distribution of the fluid system,which are crucial for chemical ***,the cross-linking reaction,which is widely used in the field of polymers,can change the physical properties of the fluids and affect the flow behavior accordingly.A configuration of microchannels is designed to conveniently generate uniform droplets in one phase of the parallel *** flow behavior of the adsorption process of sodium alginate droplets on the liquid-liquid interface is investigated,and the subsequent process of phase separation is *** the process of droplet adsorption,the crosslinking reaction occurs synchronously,which makes the droplet viscosity and the elasticity modules of the droplet surface increase,thus affecting the dynamics of the adsorption process and the equilibrium shape of the *** variation of the adsorption length with time is divided into three stages,which all conform to power law *** exponents of the second and third stages deviate from the results of the Tanner's *** flow pattern maps of droplet adsorption and phase separation are drawn,and the operating ranges of complete adsorption and complete separation are *** study provides a theoretical basis for further studying the flow behavior of droplets with cross-linking reaction in a microchannel.

关键词： Microfluidics Droplet Dynamics Crosslink Adsorption Separation

Study on trifluoromethanesulfonic acid-promoted synthesis of daidzein: Process optimization and reaction mechanism

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Chinese Journal of chemical engineering 2024年第7期71卷 132-139页

作者： Hai Cao Haibin Yang Yanxiong Fang Yuandi Zeng Xiaolan Cai Jingjing Ma School of chemical engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006China Jieyang Branch of Chemistry and chemical engineering Guangdong laboratory(Rongjiang laboratory) Jieyang 515200China

Daidzein has been widely used in pharmaceuticals,nutraceuticals,cosmetics,feed additives,*** preparation process and related reaction mechanism need to be further investigated.A cost-effective process for synthesizing daidzein was developed in this *** this article,a two-step synthesis of daidzein(Friedel–Crafts acylation and[5+1]cyclization)was developed via the employment of trifluoromethanesulfonic acid(TfOH)as an effective promoting *** effect of reaction conditions such as solvent,the amount of TfOH,reaction temperature,and reactant ratio on the conversion rate and the yield of the reaction,respectively,was systematically investigated,and daidzein was obtained in 74.0%isolated yield under optimal *** to the facilitating effect of TfOH,the Friedel–Crafts acylation was completed within 10 min at 90℃ and the[5+1]cyclization was completed within 180 min at 25℃.In addition,a possible reaction mechanism for this process was *** results of the study may provide useful guidance for industrial production of daidzein on a large scale.

关键词： Synthesis Optimal design chemical processes Reaction mechanism

Relationship between hydrogenation degree and pyrolysis performance of jet fuel

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Chinese Journal of chemical engineering 2024年第4期68卷 35-42页

作者： Qing Liu Tinghao Jia Lun Pan Jijun Zou Xiangwen Zhang Key laboratory for Green chemical and Technology School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Haihe laboratory of Sustainable chemical Transformations Tianjin 300192China Zhejiang Institute of Tianjin University Ningbo 315201China Zhejiang Provincial Key laboratory of Advanced chemical engineering Manufacture Technology College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China

Understanding the relationship between the chemical composition and pyrolysis performance of endothermic hydrocarbon fuel(EHF) is of great significance for the design and optimization of advanced EHFs. In this work, the effect of deep hydrogenation on the pyrolysis of commercial RP-3 is *** with different hydrogenation degrees were obtained by the partially and completely catalytic hydrogenation and their pyrolysis performances were investigated using an apparatus equipped with an electrically heated tubular reactor. The results show that with the increase of hydrogenation degree, fuel conversion almost remains constant during the pyrolysis process(500-650°C, 4 MPa);however, the heat sink increases slightly, and the anti-coking performance significantly improves, which are highly related to their H/C ratios. Detailed characterisations reveal that the difference of the pyrolysis performance can be ascribed to the content of aromatics and cycloalkanes: the former are prone to initiate secondary reactions to form coking precursors, while the latter could act as the hydrogen donor and release hydrogen, which will terminate the radical propagation reactions and suppress the coke deposition. This work should provide the guidance for upgrading EHFs by modulating the composition of EHFs.

关键词： RP-3 Fuel Pyrolysis Hydrogenation Deposition

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

A robust & weak-nucleophilicity electrocatalyst with an inert response for chlorine ion oxidation in large-current seawater electrolysis

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Journal of Energy Chemistry 2024年第3期90卷 486-495,I0011页

作者： Junting Dong Chang Yu Hui Wang Lin Chen Hongling Huang Yingnan Han Qianbing Wei Jieshan Qiu State Key laboratory of Fine chemicals Frontier Science Center for Smart MaterialsSchool of Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina College of chemical engineering State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Seawater splitting into hydrogen,a promising technology,is seriously limited by the durability and tolerance of electrocatalysts for chlorine ions in seawater at large current densities due to chloride oxidation and ***,we present a robust and weak-nucleophilicity nickel-iron hydroxide electrocatalyst with excellent selectivity for oxygen evolution and an inert response for chlorine ion oxidation which are key and highly desired for efficient seawater *** a weak-nucleophilicity electrocatalyst can well match with strong-nucleophilicity OH-compared with the weak-nucleophilicity Cl^(-),resultantly,the oxidation of OH-in electrolyte can be more easily achieved relative to chlorine ion oxidation,confirmed by ethylenediaminetetraacetic acid disodium probing ***,no strongly corrosive hypochlorite is produced when the operating voltage reaches about 2.1 V ***,a potential that is far beyond the thermodynamic potential of chlorine ion oxidatio *** concept and approach to reasonably designing weaknucleophilicity electrocatalysts that can greatly avoid chlorine ion oxidation under alkaline seawater environments can push forward the seawater electrolysis technology and also accelerate the development of green hydrogen technique.

关键词： Nickel-iron hydroxide electrocatalysts Highly selective seawater electrolysis Weak nucleophilicity Oxygen evolution reaction Hydrogen