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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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Formation of mesophase microbeads from bulk mesophase pitch induced by fullerene

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新型炭材料（中英文） 2024年第4期39卷 645-654页

作者： CHEN Wen-sheng LIU Lan-tao WANG Zheng DUAN Chun-feng ZHANG Xing-wei MA Zhao-kun CHEN Xiao-hong SONG Huai-he State key laboratory of chemical Resource Engineering Beijing Key Laboratory of Electrochemical Process and Technology for MaterialsBeijing Uni-versity of Chemical TechnologyBeijing 100029China

A transformation of naphthalene-based coalescenced mesophase pitch(NMP)to mesophase microbeads was achieved by heating a mixture of NMP and fullerene(C_(60)).This is different from the conventional process of the liquid-phase carbonization of isotropic pitch to the emergence of carbon microbeads in the matrix and finally their growth to form a 100%anisotropic bulk meso-phase,but rather a reverse *** effects of C_(60) loading and reaction temperature on the morphological transformation of mesophase were investigated by polarizing optical and scanning electron *** physical changes in the NMP induced by C_(60) were characterized by thermogravimetric analysis,Fourier transform infrared spectroscopy,X-ray diffractometry and Raman *** results show that the coalesced NMP can be converted to a spherical type at 300-320℃ with the addition of 5%C_(60),and the size of the mesophase microbeads increases with increasing ***,a model is established to ex-plain the unique induction effect of C_(60) in the transformation *** work makes the morphological transformation of MP con-trollable,and provides a new idea for the understanding and research of mesophase pitch.

关键词： Reversible transformation Fullerene induction mechanism Mesophase texture π-electron-induced effect Mesophase microbeads

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Ionic liquid-assisted preparation of hydroxyapatite and its catalytic performance for decarboxylation of itaconic acid

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Chinese Journal of chemical Engineering 2024年第3期67卷 9-15页

作者： Shutong Pang Hualiang An Xinqiang Zhao Yanji Wang Hebei Provincial key laboratory of Green chemical Technology and Efficient Energy Saving Tianjin Key Laboratory of Chemical Process SafetySchool of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300130China

The synthesis of methacrylic acid from biomass-derived itaconic acid is a green route,for it can get rid of the dependence on fossil *** order to solve the problems on this route such as use of a preciousmetal catalyst and a corrosive homogeneous alkali,we prepared a series of hydroxyapatite catalysts by an ionic liquid-assisted hydrothermal method and evaluated their catalytic *** results showed that the ionic liquid[Bmim]BF_(4) can affect the crystal growth of hydroxyapatite,provide fluoride ion for fluorination of hydroxyapatite,and adjust the surface acidity and basicity,morphology,textural properties,crystallinity,and composition of ***[Bmim]BF4 dosage and hydrothermal temperature can affect the fluoride ion concentration in the hydrothermal system,thus changing the degree of fluoridation of *** fluoride-ion concentration can lead to the formation of CaF_(2) and thus significantly decrease the catalytic performance of *** hydrothermal time mainly affects the growth of hydroxyapatite crystals on the c axis,leading to different catalytic *** suitable conditions for the preparation of this fluoridized hydroxyapatite are as follows:a mass ratio of[Bmim]BF4 to calcium salt=0.2:1,a hydrothermal time of 12 h,and a hydrothermal temperature of 130℃.A maximal methacrylic acid yield of 54.7%was obtained using the fluoridized hydroxyapatite under relatively mild reaction conditions(250℃ and 2 MPa of N_(2))in the absence of a precious-metal catalyst and a corrosive homogeneous alkali.

关键词： Ionic liquid Hydroxyapatite Itaconic acid Methacrylic Decarboxylation reaction

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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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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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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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Energy-saving design and optimization of pressure-swing-assisted ternary heterogenous azeotropic distillations

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Chinese Journal of chemical Engineering 2024年第4期68卷 1-7页

作者： Lianjie Wu Kun Lu Qirui Li Lianghua Xu Yiqing Luo Xigang Yuan Tianjin key laboratory of Organic Solar Cells and Photochemical Conversion College of Chemical and Chemical EngineeringTianjin University of TechnologyTianjin 300384China State key laboratory of chemical Engineering Tianjin UniversityTianjin 300072China

A huge amount of energy is always consumed to separate the ternary azeotropic mixtures by *** heterogeneous azeotropic distillation and the pressure-swing distillation are two kinds of effective technologies to separate heterogeneous azeotropes without entrainer *** give better play to the synergistic energy-saving effect of these two processes,a novel pressure-swing-assisted ternary heterogeneous azeotropic distillation(THAD)process is proposed *** this process,the ternary heterogeneous azeotrope is decanted into two liquid phases before being refluxed into the azeotropic distillation column to avoid the aqueous phase remixing,and three columns'pressures are modified to decrease the flowrates of the recycle *** the dividing wall column and heat integration technologies are introduced to further reduce its energy consumption,and the pressureswing-assisted ternary heterogeneous azeotropic dividing-wall column and its heat integration structure are achieved.A genetic algorithm procedure is used to optimize the proposed *** design results show that the proposed processes have higher energy efficiencies and lower CO_(2)emissions than the published THAD process.

关键词： Distillation Separation Process control Process systems

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Engineering oxygen vacancies on Tb-doped ceria supported Pt catalyst for hydrogen production through steam reforming of long-chain hydrocarbon fuels

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Chinese Journal of chemical Engineering 2024年第4期68卷 181-192页

作者： Zhourong Xiao Changxuan Zhang Peng Li Desong Wang Xiangwen Zhang Li Wang Jijun Zou Guozhu Li State key laboratory of Metastable Materials Science and Technology(MMST) Hebei Key Laboratory of Applied ChemistryCollege of Environmental and Chemical EngineeringYanshan UniversityQinhuangdao 066004China key laboratory for Green chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Steam reforming of long-chain hydrocarbon fuels for hydrogen production has received great attention for thermal management of the hypersonic vehicle and fuel-cell *** this work,Pt catalysts supported on CeO_(2)and Tb-doped CeO_(2)were prepared by a precipitation *** physical structure and chemical properties of the as-prepared catalysts were characterized by powder X-ray diffraction,scanning electron microscopy,transmission electron microscopy,Raman spectroscopy,H_(2)temperature programmed reduction,and X-ray photoelectron *** results show that Tb-doped CeO_(2)supported Pt possesses abundant surface oxygen vacancies,good inhibition of ceria sintering,and strong metal-support interaction compared with CeO_(2)supported *** catalytic performance of hydrogen production via steam reforming of long-chain hydrocarbon fuels(n-dodecane)was *** with 2Pt/CeO_(2),2Pt/Ce_(0.9)Tb_(0.1)O_(2),and 2Pt/Ce_(0.5)Tb_(0.5)O_(2),the 2Pt/Ce_(0.7)Tb_(0.3)O_(2)has higher activity and stability for hydrogen production,on which the conversion of n-dodecane was maintained at about 53.2%after 600 min reaction under 700℃at liquid space velocity of 9 ml·g^(-1)·h^(-1).2Pt/CeO_(2)rapidly deactivated,the conversion of n-dodecane was reduced to only 41.6%after 600 min.

关键词： Steam reforming n-Dodecane Hydrogen production Pt-based catalyst Oxygen vacancy CeO_(2)

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NIR-Ⅱ responsive Janus nanoparticles amplify immunogenic cell death for enhanced cancer immunotherapy

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Science China(Technological Sciences) 2024年第1期67卷 321-329页

作者： CHEN BeiBei GUO KangLi WANG HaoRan XU Fu-Jian WANG JuLin ZHAO NaNa State key laboratory of chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China key laboratory of Biomedical Materials of Natural Macromolecules(Beijing University of chemical Technology) Beijing Laboratory of Biomedical MaterialsBeijing University of Chemical TechnologyBeijing 100029China College of Materials Sciences and Engineering Beijing University of Chemical TechnologyBeijing 100029China Beijing key laboratory of Electrochemical Process and Technology for Materials Beijing University of Chemical TechnologyBeijing 100029China

Immunotherapy brings new hope for tumor treatment by inducing immunogenic cell death(ICD)of tumor ***,insufficient immunogenicity and low immune response rate greatly limit antitumor ***,by optimizing the composition and morphology,the rational design of Janus nanoparticles composed of Fe_(3)O_(4) nanospheres and SiO_(2)nanorods was realized for enhanced cancer immunotherapy through amplified *** glucose oxidase(GOx)was loaded by the Janus nanoparticles,the resultant M-FS-GOx consumes glucose at tumor sites to generate gluconic acid and hydrogen peroxide(H_(2)O_(2))for starvation therapy while the H_(2)O_(2)supply promotes the production of highly toxic·OH to achieve effective chemodynamic therapy(CDT).Under a 1064 nm light irradiation,the photothermal effect of M-FS-GOx enhances the enzyme activity of GOx for improved starvation ***,both tumor-associated antigens released during the process of ICD and the intrinsic immunoadjuvant property of M-FS-GOx stimulate dendritic cell maturation to activate antitumor immune *** work provides a promising strategy for the construction of Janus nanoparticles to achieve enhanced cancer immunotherapy through combination therapy-amplified ICD.

关键词： Janus nanoparticles immunogenic cell death cancer immunotherapy

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