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Lithiophilic CoF2@C hollow spheres towards spatial lithium deposition for stable lithium metal batteries

Journal of Energy Chemistry 2024年第10期97卷 55-67页

作者： Jianxing Wang Shuhao Yao Runming Tao Xiaolang Liu Jiazhi Geng Chang Hong Huiying Li Guiyun Yu Haifeng Li Xiao-Guang Sun Jianlin Li Jiyuan Liang School of Optoelectronic Materials & technology Jianghan University Institute for Advanced Materials and Manufacturing University of Tennessee Applied Materials division Argonne National Laboratory School of Chemistry & chemical Engineering Yancheng Institute of Technology chemical Sciences division Oak Ridge National Laboratory

Lithium metal（LM） is a promising anode for next-generation batteries due to its high theoretical capacity and low electrode ***,side reactions,volume change,and unwanted lithium dendrite growth seriously limit the practical application of ***,with the aid of a hard template approach,a novel lithiophilic CoF2-carbon hollow sphere（CoF2@C-HS） composite material is successfully prepared via a facile in-situ fluorination and etching *** lithiophilic CoF2acts as nucleation sites to reduce nucleation overpotential as well as induces the spatial Li deposition and the formation of LiFrich solid electrolyte interphase（SEI）,and the hollow carbon matrix can enhance the electrical conductivity and offer free space for LM *** simulations reveal that the synergistic effect of lithiophilic CoF2and hollow carbon matrix homogenizes the electric field distribution and Li+*** from these advantages,the CoF2@C-HS-modified copper substrate electrode delivers an enhanced Coulombic efficiency（CE） of 93.7% for 280 cycles at 1 mA cm-2and 1 mA h *** symmetrical cell using CoF2@C-HS can stably cycle more than 1800 h with a low voltage hysteresis of 11 mV at a current density of 0.5 MA cm-2and an areal capacity of 0.5 mA h ***,the Li@CoF2@C-HS composite anode enables more than 300 stable cycles at 1 C with a capacity retention of 95% in LiFePO4-based full cell and 110 stable cycles at 1 C in LiNi0.8Co0.1Mn0.1O2（NCM811）-based highvoltage full *** work might shed a new light on designing lithiophilic hosts to spatially confine LM deposition,realizing dendrite-free LM anodes and the practical applications of LM batteries.

关键词： Lithiophilic CoF2 Lithium metal anode Nanocomposite Spatial deposition, Stability

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New approach for particle size and shape analysis of iron-based oxygen carriers at multiple oxidation states

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Particuology 2024年第7期90卷 493-503页

作者： Victor Purnomo Marcelo Dal Belo Takehara Robin Faust Lidiya Abdisa Ejjeta Henrik Leion division of Energy and Materials Department of Chemistry and Chemical EngineeringChalmers University of TechnologyGöteborg 41258Sweden division of Energy Science Department of Engineering Sciences and MathematicsLuleåUniversity of TechnologyLuleå97187Sweden

One of the crucial issues in the chemical looping technology lies in its bed material:the oxygen *** size analysis of an oxygen carrier is important since in a fluidized bed the material can only work well within a specific size *** the favorable size ranges for oxygen carrier materials have already been reported,none of the published studies has analyzed the particle size and shape of oxygen carriers in ***,the effect of oxygen carriers'oxidation degree on such properties has not been considered *** study aimed to report the particle size and shape analysis of five iron-based oxygen carriers,one natural ore,one synthetic material,and three residue products,at different oxidation degrees using dynamic image analysis(DIA).The oxygen carriers were prepared at different mass conversion degrees in a fluidized bed batch *** size distribution,sphericity,and aspect ratio of the oxygen carrier particles were examined experimentally using a Camsizer *** results show that the DIA method was successfully able to analyze the particle size and shape of our oxygen carriers with satisfying accuracy for *** oxidation state of the investigated materials seems to only affect the particle size and shape of oxygen carriers to a minor ***,exposures to redox cycles in a fluidized bed reactor may alter the particle size and shape of most oxygen carriers.

关键词： Oxygen carrier Size and shape analysis Dynamic image analysis Oxidation state Fluidized bed chemical looping

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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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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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Combined effects of sea urchin-like structure and mixed Cu^(+)/Cu^(0)states on promoting C_(2)formation in electrocatalytic CO_(2)reduction

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Frontiers of chemical Science and Engineering 2024年第3期18卷 63-73页

作者： Mengqing Shan Dongsheng Lu Jiatong Dong Shen Yan Jinyu Han Hua Wang Collaborative Innovation Center of chemical Science and Engineering Key Laboratory for Green Chemical Technology of the Ministry of EducationSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin300354China

Surface engineering and Cu valence regulation are essential factors in improving the C_(2)selectivity during the electrochemical reduction of CO_(2).Herein,we present a sea urchin-like CuO/Cu_(2)O catalyst derived from rhombic dodecahedra Cu_(2)O through one-step oxidation/etching method where the mixed Cu^(+)/Cu^(0)states are formed via in situ reduction during *** combined effects of the morphology and the mixed Cu^(+)/Cu^(0)states on C–C coupling are evaluated by the Faradaic efficiency of C_(2)and the C_(2)/C1 ratio obtained in an H-cell.R-Cu^(O)/Cu_(2)O exhibited 49.5%Faradaic efficiency of C_(2)with a C_(2)/C1 ratio of 3.1 at−1.4 V *** hydrogen electrode,which are 1.5 and 3.2 times higher than those of R-Cu_(2)O,*** a flow-cell,68.0%Faradaic efficiency of C_(2)is achieved at a current density of 500 mA·cm^(−2).The formation of the mixed Cu^(+)/Cu^(0)states was confirmed by in situ Raman ***,the sea urchin-like structure provides more active sites and enables faster electron *** a result,the excellent C_(2)production on R-CuO/Cu_(2)O is primarily attributed to the synergistic effects of the sea urchin-like structure and the stable mixed Cu^(+)/Cu^(0)***,this work presents an integrated strategy for developing Cu-based electrocatalysts for C_(2)production through electrochemical CO_(2)reduction.

关键词： CO_(2)electrolysis sea urchin-like structure Cu^(+)/Cu^(0) C_(2)products

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NaBH4-induced phase transition of CoSe_(2) with abundant Se deficiency for acidic oxygen reduction to hydrogen peroxide

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Rare Metals 2024年第2期43卷 500-510页

作者： Cai-Di Han Yong-Chao Zhang Qian Zhang Jin-Ting Wu Jian Gao Ji-Jun Zou Xiao-Dong Zhu State Key Laboratory Base of Eco-chemical Engineering College of chemical Engineering Qingdao University of Science and TechnologyQingdao266042China Key Laboratory for Green chemical technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

Electrocatalytic oxygen reduction(ORR)via the 2e−pathway to form H_(2)O_(2) in acidic medium has attracted extensive ***,the low activity,insufficient selectivity and high cost of catalysts have been the ***,CoSe_(2) with abundant Se deficiency was synthesized by a simple hydrothermal method,and the addition of NaBH4-induced CoSe_(2) phase transition from orthorhombic to cubic phase with more Se *** cubic phase CoSe_(2) with abundant Se deficiency can effectively regulate the surface electronic structure with suitable binding energies of*OOH and*O,which shows high activity,selectivity and long-term stability for acidic ORR to H_(2)O_(2).The onset potential is as low as 0.73 V *** hydrogen electrode(RHE),the H_(2)O_(2) selectivity is 84%(0 V ***),and the average electron transfer number is about ***,the H_(2)O_(2) yield measured using a flow cell is as high as 115.92 mmol·gcat.^(−1)·h^(−1) and the Faradaic efficiency is 70%at 0 V ***,which presents high potential in electrocatalytic acidic ORR to H_(2)O_(2) and organic pollutant degradation using the electron-Fenton process.

关键词： Se defected CoSe_(2) Crystal phase transition Electrocatalysis Acidic oxygen reduction Hydrogen peroxide

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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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Yolk-shell FeCu/NC electrocatalyst boosting high-performance zinc-air battery

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Nano Research 2024年第9期17卷 7918-7925页

作者： Chen Liang Tianyu Zhang Shilun Sun Aijuan Han Zenghui Qiu Haijun Xu Junfeng Liu State Key Laboratory of chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China College of Mathematics&Physics Beijing University of Chemical TechnologyBeijing 100029China Beijing Bioprocess Key Laboratory Beijing University of Chemical TechnologyBeijing 100029China

Iron-nitrogen-carbon single-atom catalysts(Fe-N-C SACs)are widely acknowledged for their effective oxygen reduction activity,however,their activity requires further ***,additional structural optimization is necessary to enhance mass transport and achieve higher power density in practical ***,using ZIF-8 as a template,we synthesized yolk-shell catalysts featuring complex sites of Fe single atoms and Cu nanoclusters(y-FeCu/NC)via partial etching and liquid-phase *** synthesized y-FeCu/NC catalyst exhibits high specific surface area and mesoporous *** with the advantages of highly active sites and yolk-shell structure,the y-FeCu/NC catalyst demonstrated outstanding catalytic performance in the oxygen reduction reaction,achieving a half-wave potential(E_(1/2))of 0.97 V in 0.1 M *** a practical energy device,Zn-air battery(ZAB)assembled with y-FeCu/NC catalyst achieved a remarkable power density of 356.3 mW·cm^(-2),representing an improvement of approximately 28.5%compared to its solid FeCu/NC ***,it showcased impressive stability,surpassing all control samples.

关键词： atomic Fe-N4 sites Cu nanoclusters yolk-shell structure oxygen reduction reaction zinc-air battery

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Enhanced stability of nitrogen-doped carbon-supported palladium catalyst for oxidative carbonylation of phenol

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Chinese Journal of chemical Engineering 2024年第1期65卷 19-28页

作者： Xiaojing Liu Ruohan Zhao Hao Zhao Zhimiao Wang Fang Li Wei Xue Yanji Wang Hebei Provincial Key Laboratory of Green chemical technology and High Efficient Energy Saving School of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300130China Tianjin Key Laboratory of chemical Process Safety Tianjin 300130China Hebei Industrial technology Research Institute of Green chemical Industry Huanghua 061100China

Enhancing the stability of supported noble metal catalysts emerges is a major challenge in both science and ***,a heterogeneous Pd catalyst(Pd/NCF)was prepared by supporting Pd ultrafine metal nanoparticles(NPs)on nitrogen-doped carbon;synthesized by using F127 as a stabilizer,as well as chitosan as a carbon and nitrogen *** Pd/NCF catalyst was efficient and recyclable for oxidative carbonylation of phenol to diphenyl carbonate,exhibiting higher stability than Pd/NC prepared without F127 *** hydrogen bond between chitosan(CTS)and F127 was enhanced by F127,which anchored the N in the free amino group,increasing the N content of the carbon material and ensuring that the support could provide sufficient N sites for the deposition of Pd *** process helped to improve metal *** increased metal-support interaction,which limits the leaching and coarsening of Pd NPs,improves the stability of the Pd/NCF ***,density functional theory calculations indicated that pyridine N stabilized the Pd^(2+)species,significantly inhibiting the loss of Pd^(2+)in Pd/NCF during the reaction *** work provides a promising avenue towards enhancing the stability of nitrogen-doped carbon-supported metal catalysts.

关键词： Supported Pd catalyst N-doped carbon Amphiphilic triblock copolymer Pyridinic nitrogen Stability

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Insight into the adsorption behavior and mechanism of trace impurities from H_(2)O_(2) solution on functionalized zirconia by tuning the structure of amino groups

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Frontiers of chemical Science and Engineering 2024年第5期18卷 83-94页

作者： Yu Meng Yitong Wang Guozhu Li Guozhu Liu Li Wang Key Laboratory for Green chemical technology of Ministry Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Haihe Laboratory of Sustainable chemical Transformations Tianjin 300192China

Primary,secondary and tertiary amino-functionalized zirconia(ZrO_(2)-NH_(2),ZrO_(2)-NH and ZrO_(2)-N)was synthesized by the postgrafting method for the adsorption removal of typical metallic ions,phosphate and total oxidizable carbon from a real H_(2)O_(2) ***_(2)-NH_(2),ZrO_(2)-NH and ZrO_(2)-N exhibited similar pore sizes and sequentially increased zeta *** adsorption results of single and binary simulated solutions showed that the removal efficiency increased in the order of Fe^(3+)>Al^(3+)>Ca^(2+)>Na^(+).There is competitive adsorption between metallic ions,and Fe^(3+) has an advantage over the other metals,with a removal efficiency of 90.7%.The coexisting phosphate could promote the adsorption of metallic ions,while total oxidizable carbon had no effect on *** adsorption results of the real H_(2)O_(2)solution showed that ZrO_(2)-NH_(2) exhibited the best adsorption affinity for metallic ions,as did phosphate and total oxidizable carbon,with a total adsorption capacity of 120.9 mg·g_(-1).Density functional theory calculations revealed that the adsorption process of metallic ions involves electron transfer from N atoms to metals and the formation of N-metal bonds.

关键词： adsorption metallic ion phosphate total oxidizable carbon zirconia H_(2)O_(2)

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