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

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

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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

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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

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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

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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 key laboratory of chemical Resource engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China state key 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 182 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

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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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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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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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Kinetics and mechanism of propylene hydro-oxidation to acrolein on Au catalysts

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Nano Research 2024年第1期17卷 354-363页

作者： Wei Du Zhihua Zhang Nan Song Xuezhi Duan Xinggui Zhou state key laboratory of chemical engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China

Propylene epoxidation by H_(2)and O_(2)to propylene oxide(PO)over the Au-Ti bifunctional catalysts,as an ideal reaction for PO production,has attracted great *** the mechanism of acrolein formation is of great importance for understanding the mechanism of molecular oxygen activation and the formation of hydroperoxo species on the Au ***,we investigate the reaction mechanism of propylene oxidation to acrolein on the Au/uncalcined TS-1(Au/TS-1-B)catalyst through a combination of multiple characterization,H_(2)/D_(2)exchange,kinetics experiment,and *** Ti sites are found to be non-essential to acrolein ***,the acrolein formation on the Au/TS-1-B catalyst is confirmed to be promoted by H_(2)through hydroperoxo species formation,which includes two main steps:propylene dehydrogenation to*C_(3)H_(5)with the aid of*OOH species,and*C_(3)H_(5)oxidation by*OOH to *** latter step is determined to be the rate-determining step because the corresponding kinetics model gives the best description for experimental *** work not only provides kinetics insights for the propylene hydro-oxidation to acrolein on the Au-Ti bifunctional catalysts,but also facilitates the rational design of Au catalysts with high activity and selectivity in the direct propylene epoxidation with H_(2)and O_(2).

关键词： kinetics mechanism gold acrolein hydro-oxidation

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A thermodynamic view on the in-situ carbon dioxide reduction by biomass-derived hydrogen during calcium carbonate decomposition

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Chinese Journal of chemical engineering 2024年第4期68卷 231-240页

作者： Peng Jiang Hao Zhang Guanhan Zhao Lin Li Tuo Ji Liwen Mu Xiaohua Lu Jiahua Zhu state key laboratory of Materials-oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China

In the carbonate industry,deep decarbonization strategies are necessary to effectively remediate CO_(2).These strategies mainly include both sustainable energy supplies and the conversion of CO_(2)in downstream *** study developed a coupled process of biomass chemical looping H2 production and reductive calcination of CaCO_(3).Firstly,a mass and energy balance of the coupled process was established in Aspen *** this,process optimization and energy integration were implemented to provide optimized operation ***,a life cycle assessment was carried out to assess the carbon footprint of the coupled *** reveal that the decomposition temperature of CaCO_(3)in an H_(2)atmosphere can be reduced to 780℃(generally around 900℃),and the conversion of CO_(2)from CaCO_(3)decomposition reached 81.33%with an H2:CO ratio of 2.49 in gaseous *** optimizing systemic energy through heat integration,an energy efficiency of 86.30%was ***,the carbon footprint analysis revealed that the process with energy integration had a low global warming potential(GWP)of-2.624 kg·kg^(-1)(CO_(2)/CaO).Conclusively,this work performed a systematic analysis of introducing biomass-derived H_(2)into CaCO_(3)calcination and demonstrated the positive role of reductive calcination using green H_(2)in mitigating CO_(2)emissions within the carbonate industry.

关键词： Biomass CaCO_(3)reductive calcination chemical looping Hydrogen production Carbon footprint Thermodynamics process

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