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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 {1. 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 {1. 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 {1. laboratory of chemical resource engineering Beijing University of Chemical TechnologyBeijing 100029China

The engineering of microbial cell factories for the production of high-value {1.s 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 {1.s 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 {1. 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(3.7×1.^(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

Highly dispersed MgInCe-mixed metal oxides catalyzed direct carbonylation of glycerol and CO_(2)into glycerol carbonate

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Chinese Journal of chemical {1. 2024年第8期72卷 153-163页

作者： Xufang Chen Xin Shu Yanru Zhu Jian Zhang Zhigang Chai Hongyan Song Zhe An Jing He state {1. laboratory of chemical resource engineering Beijing University of Chemical TechnologyBeijing 100029China Quzhou Institute for Innovation in resource {1. engineering Quzhou 324000China

Glycerol carbonate,an important glycerol value-added product,has been widely used as an active intermediate and inert solvent in the synthesis of cosmetics,detergents,chemical intermediates,polymers,and so *** direct carbonylation from glycerol with CO_(2)is considered a promising route,but still tough work due to the thermodynamic stability and the kinetic inertness of CO_(2).In this work,highlyselective direct carbonylation of glycerol and CO_(2)into glycerol carbonate has been achieved over highly dispersed MgInCe-mixed metal oxides(MgInCe-MMO),which were prepared through the topological transformation derived from the MgInCe-layered double hydroxides(MgInCe-LDHs).By precisely modulating the surface basic-acidic properties and the oxygen vacancies,an efficient carbonylation of glycerol with CO_(2)has been achieved with a selectivity of up to>99%to glycerol *** investigation into the synergistic catalysis of base-acid sites and oxygen vacancies has been clarified.

关键词： Catalytic reaction engineering Glycerol carbonate Direct carbonylation from glycerol Carbon dioxide Mixed metal oxides Synergistic catalysis

Molecular-scale co-assembly membranes derived from keplerate cluster:carbonic anhydrase-mimicking nanocapsules for enhanced CO_(2)/N_(2)separation

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Science China Chemistry 2024年第10期67卷 3271-3282页

作者： Wan-Lei Zhao Hongqiang Li Ruoxuan Zheng Yixin Yang Wei Chen Yu-Fei Song state {1. laboratory of chemical resource engineering Beijing University of Chemical TechnologyBeijing 100029China Quzhou Institute for Innovation in resource {1. engineering Quzhou 324000China

The development of CO_(2)separation membranes with high permeability and high selectivity,as well as ultra-thin selective layers,has always been ***,a molecular-scaled co-assembly strategy is employed to fabricate the Pebax-Mo_(1.2)(Pebax=polyether-block-amide copolymer;Mo_(1.2)=(NH_(4))_(42)[Mo_(72)^(Ⅵ)Mo_(60)^(Ⅴ)O_(372)(CH_(3)COO)_(30)(H_(2)O)_(72)])*** optimal selfstanding membrane,Pebax-Mo_(1.2)-5%,shows a CO_(2)permeability of~384 Barrer and an ultra-high ideal CO_(2)/N_(2)selectivity of~244,outperforming most membranes reported in the *** CO_(2)permeability and ideal CO_(2)/N_(2)selectivity are increased by 70%and 367%,respectively,compared with the pristine Pebax membrane.A thin-film composite membrane prepared by spin-coating technique on a support membrane with gutter layers also exhibits a CO_(2)permeance of 838 GPU and a CO_(2)/N_(2)selectivity of *** excellent performance can be attributed to the following reasons:(1.strong hydrogen bonding interactions between{Mo_(1.2)}clusters and Pebax confer excellent interfacial compatibility to the mixed matrix membranes;(2)incorporation of hollow{Mo_(1.2)}clusters into the Pebax molecular chain decreases the crystallinity of Pebax,and thereby accelerates the chain dynamics and increases the free volume of the membrane;(3)in situ diffuse reflectance infrared Fouriertransform spectroscopy demonstrates that the{Mo_(1.2)}clusters can effectively catalyze the hydration reaction of CO_(2)and promote the transport of CO_(2);(4)furthermore,the 0.35 nm pores of the crown ether-type{Mo_(9)O_(9)}allow the accurate size sieving of CO_(2)(0.33 nm)and N_(2)(0.36 nm)molecules.

关键词： polyoxometalates molecular-scale assembly CO_(2)capture mixed matrix membranes

Highly selective extraction of aromatics from aliphatics by using metal chloride-based ionic liquids

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Chinese Journal of chemical {1. 2024年第1期65卷 222-229页

作者： Hui Yu Xiaojia Wu Chuanqi Geng Xinyu Li Chencan Du Zhiyong Zhou Zhongqi Ren state {1. laboratory of chemical resource engineering Beijing University of Chemical TechnologyBeijing 100029China

The separation of aromatics from aliphatics is essential for achieving maximum exploitation of oil resources in the petro{1. *** this study,a series of metal chloride-based ionic liquids were prepared and their performances in the separation of 1.2,3,4-tetrahydronaphthalene(tetralin)/dodecane and tetralin/decalin systems were *** these ionic liquids,1.ethyl-3-methylimidazolium tetrachloroferrate([EMIM][FeCl_(4)])with the highest selectivity was used as the *** functional theory calculations showed that[EMIM][FeCl_(4)]interacted more strongly with tetralin than with dodecane and *** decomposition analysis of[EMIM][FeCl_(4)]-tetralin indicated that electrostatics and dispersion played essential roles,and induction cannot be *** van der Waals forces was a main effect in[EMIM][FeCl_(4)]-tetralin by independent gradient model *** tetralin distribution coefficient and selectivity were 0.8 and 1.0,respectively,with 1.%(mol)tetralin in the initial tetralin/dodecane system,and 0.67 and 1..5,respectively,with 1.%(mol)tetralin in the initial tetralin/decalin *** selectivity increased with decreasing alkyl chain length of the *** influence of the extraction temperature,extractant dosage,and initial concentrations of the system components on the separation performance were *** experiments showed that the regenerated[EMIM][FeCl_(4)]could be used repeatedly.

关键词： Ionic liquid Aromatic hydrocarbon Aliphatic hydrocarbon Extraction

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 {1. laboratory of Fine chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China state {1. laboratory of Fine chemicals Liaoning Key Laboratory for Energy Materials and Chemical EngineeringSchool of ChemistryDalian University of TechnologyDalian 116024China state {1. 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 0.1. 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

Breakthrough in Li-mediated continuous electrosynthesis of ammonia

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Science China Chemistry 2024年第10期67卷 3191-3192页

作者： Fei Zhan Chang Yu state {1. laboratory of chemical resource engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China state {1. laboratory of Fine chemicals Liaoning Key Lab for Energy Materials and Chemical EngineeringSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China

Ammonia(NH3)ranks among the manufactured chemicals,with an annual production surpassing 1.2 million tons[1.,which is an indispensable raw material for fertilizer industry and has been recognized as a promising carbon-... 详细信息

关键词： ammonia Ammonia suppl

Layered double hydroxides functionalization toward rechargeable batteries Author links open overlay panel

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Particuology 2024年第8期91卷 138-154页

作者： Jianxiong Gao Bowen Jin Mingfei Shao state {1. laboratory of chemical resource engineering Beijing University of Chemical TechnologyBeijing100029China Renewable Energy Research Institute Quzhou Institute for Innovation in Resource Chemical EngineeringQuzhou324000China

Layered double hydroxides(LDHs),known as typical two-dimensional materials with unique physicochemical properties,are regarded as promising candidates in energy storage ***,some inherent defects,such as poor conductivity and limited active sites,hinder the further development of ***,various functionalization strategies(e.g.,intercalation of guest molecules;metal ions doping and defect introduction of host layer;exfoliation to monolayer;hybridization with functional materials;construction of hierarchical structure;interface {1. and phase transformation)have been used to modify the characteristics of LDHs,which provides guidance for designing novel *** this review,we discuss how these strategies improve the properties of LDH-based materials,which are expected to possess high electronic and ionic conductivity,high specific surface area and high mechanical and chemical stability ***,the application of LDH-based materials in advanced energy conversion and storage techniques,including metal-ions batteries,lithium-sulfur batteries and metal-air batteries,have been comprehensively summarized.

关键词： Layered double hydroxide Functionalization strategy Rechargeable battery