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Metal size effects over metal/zeolite bifunctional catalysts in the selective hydroalkylation of benzene

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Frontiers of chemical Science and engineering 2024年第4期18卷 107-114页

作者： Junjie Li Chuang Liu Zhenlong Jia Yingchun Ye Dawei Lan Wei Meng Jianqiang Wang Zhendong Wang Yongfeng Hu Weimin Yang state key laboratory of green chemical engineering and industrial catalysis Sinopec Shanghai Research Institute of Petrochemical Technology Co.Ltd.Shanghai 201208China School of chemical engineering East China University of Science and TechnologyShanghai 200237China

Bifunctional metal/zeolite materials are some of the most suitable catalysts for the direct hydroalkylation of benzene to *** overall catalytic performance of this reaction is strongly influenced by the hydrogenation,which is dependent on the metal ***,systematically investigating the metal size effects in the hydroalkylation of benzene is *** this work,we successfully synthesized Ru and Pd nanoparticles on Sinopec Composition Materials No.1 zeolite with various metal *** demonstrated the size-dependent catalytic activity of zeolite-supported Ru and Pd catalysts in the hydroalkylation of benzene,which can be attributed to the size-induced hydrogen spillover capability *** work presents new insights into the hydroalkylation reaction and may open up a new avenue for the smart design of advanced metal/zeolite bi-functional catalysts.

关键词： size effects bifunctional catalysts metal/zeolite hydroalkylation

The interaction of the structure-directing agent with the zeolite framework determines germanium distribution in SCM-15 germanosilicate

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Frontiers of chemical Science and engineering 2024年第5期18卷 105-114页

作者： Stoyan P.Gramatikov Petko St.Petkov Zhendong Wang Weimin Yang Georgi N.Vayssilov Faculty of Chemistry and Pharmacy University of Sofia1126 SofiaBulgaria state key laboratory of green chemical engineering and industrial catalysis Sinopec Shanghai Research Institute of Petrochemical Technology Co.Ltd.Shanghai 201208China

We report results from computational modeling of the relative stability of germanosilicate SCM-15 structure due to different distribution of germanium heteroatoms in the double four-member rings(D4Rs)of the framework and the orientation of the structure directing agent(SDA)molecules in the as-synthesized *** calculated relative energies of the bare zeolite framework suggest that structures with germanium ions clustered in the same D4Rs,e.g.,with large number of Ge–O-Ge contacts,are the most *** simulations of various orientations of the SDA in the pores of the germanosilicate zeolite show different stability order-the most stable models are the structures with germanium spread among all ***,for SCM-15 the stabilization due to the presence of the SDA and their orientation,is thermodynamic factor directing both the formation of specific framework type and Ge distribution in the framework during the *** relative stability of bare structures with different germanium distribution is of minor *** differs from SCM-14 germanosilicate,reported earlier,for which the stability order is preserved in presence of ***,even for zeolites with the same chemical composition and SDA,the characteristics of their framework lead to different energetic preference for germanium distribution.

关键词： zeolite density functional theory structure-directing agent SCM-15

Electronic structure regulation and built-in electric field synergistically strengthen photocatalytic nitrogen fixation performance on Ti-BiOBr/TiO_(2)heterostructure

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Rare Metals 2024年第3期43卷 1125-1138页

作者： Ru-Qi Li Yu-Jie Bian Chun-Ming Yang Li Guo Tao-Xia Ma Chuan-Tao Wang Feng Fu Dan-Jun Wang College of Chemistry and chemical engineering Yan’an UniversityYan’an Key Laboratory of Green Catalysis and Quality Improvement and Utilization of Low Rank CoalYan’an716000China

At present,industrial synthetic ammonia was still obtained through the Hubble-Bosch process,with large energy *** is a research hotspot to realize green synthetic ammonia by using solar *** difficulty of photocatalytic ammonia synthesis was that the photo-excited electrons have not enough energy to active N≡*** this study,Ti was doped into BiOBr by one-step hydrothermal method,which was oxidized into TiO_(2)when the doping amount reaches the maximum,in situ forming Ti_(0.31)B_(0.69)OB/TiO_(2)*** from the synergistic effect of Ti doping and S-scheme heterojunction,the synthetic ammonia efficiency of Ti_(0.31)B_(0.69)OB/TiO_(2)-11.96 reached 1.643 mmol·g_(cat)^(-1)at mild conditions and without hole scavenger for up to 7 h,the efficiency of synthetic ammonia is 115 times,10.5 times and 3.3 times of that of BiOBr,Ti_(0.31)B_(0.69)OB and TiO_(2),***,DFT calculation confirms that Ti doping accurately refine the electronic structure of BiOBr,facilitate nitrogen adsorption activation and reduce hydrogenation reaction energy barrier,thus accelerating the reaction kinetics of photocatalytic nitrogen reduction(NRR),Meanwhile,constructing S-scheme heterojunction boosts the separation and transfer of photogenerated electron-hole pairs,improving the reduction ability of electrons in the conduction band of TiO_(2)and the oxidation ability of holes in the valence band of Ti_(0.31)B_(0.69)OB.

关键词： S-scheme heterostructure Electronic structure regulation Built-in electric field Synergistical stren4gthening Photocatalytic nitrogen fixation

Crystal facet-dependent CO_(2) cycloaddition to epoxides over ZnO catalysts

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Frontiers of chemical Science and engineering 2024年第5期18卷 49-59页

作者： Yongjian Wei Ying Li Yunfei Xu Yinghui Sun Tong Xu Haiou Liang Jie Bai Inner Mongolia key laboratory of industrial catalysis Hohhot 010051China College of chemical engineering Inner Mongolia University of TechnologyHohhot 010051China

With regard to green chemistry and sustainable development,the fixation of CO_(2) into epoxides to form cyclic carbonates is an attractive and promising pathway for CO_(2) *** oxides,renowned as promising eco-friendly catalysts for industrial production,are often undervalued in terms of their impact on the CO_(2)addition *** this work,we successfully developed ZnO nanoplates with(002)surfaces and ZnO nanorods with(100)surfaces via morphology-oriented regulation to explore the effect of crystal faces on CO_(2) *** quantitative data obtained from electron paramagnetic resonance spectroscopy indicated that the concentration of oxygen vacancies on the ZnO nanoplate surfaces was more than twice that on the ZnO nanorod *** functional theory calculations suggested that the(002)surfaces have lower adsorption energies for CO_(2) and epichlorohydrin than the(100)*** a result,the yield of cyclochloropropene carbonate on the ZnO nanoplates(64.7%)was much greater than that on the ZnO nanorods(42.3%).Further evaluation of the reused catalysts revealed that the decrease in the oxygen vacancy concentration was the primary factor contributing to the decrease in catalytic *** on these findings,a possible catalytic mechanism for CO_(2) cycloaddition with epichlorohydrin was *** work provides a new idea for the controllable preparation of high-performance ZnO catalysts for the synthesis of cyclic carbonates from CO_(2) and epoxides.

关键词： carbon dioxide cycloaddition zinc oxide crystal face oxygen vacancy

Current collectors' effects on the electrochemical performance of LiNi0.6Co0.2Mn0.2O2 suspension electrodes for lithium slurry battery

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green Energy & Environment 2024年第8期9卷 1306-1313页

作者： Linshan Peng Yufei Ren Zhaoqiang Yin Zhitong Wang Xiangkun Wu Lan Zhang CAS key laboratory of green Process and engineering Beijing Key Laboratory of Ionic Liquids Clean ProcessState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of Sciences School of chemical engineering University of Chinese Academy of Sciences Hefei University Institute of Mechanics Chinese Academy of Sciences Langfang green industrial Technology Center

Take after the advantages of lithium-ion battery（LIB） and redox flow battery（RFB）, semi-solid flow battery（SSFB） is a promising electrochemical energy storage device in renewable energy utilization. The flowable slurry electrode realizes decouple of energy and power density,while it also brings about new challenge to SSFBs, electron transport between active material and the out circuit. In this consideration, three types of current collectors（CCs） are applied to study the resistance and electrochemical performances of slurry cathodes within pouch cells for the first time. It proves that the electronic resistance（Re） between slurry electrode and the CC plays a decisive role in SSFB operation, and it is so large when Al foil is adopted that the cell cannot even work. Contact angle between Ketjen black（KB） slurry without active material（AM） and the CC is a preliminarily sign for the Re, the smaller the angle, the lower the resistance, and the better electrochemical performance of the cell.

关键词： Semi-solid flow battery Slurry electrode Current collector Electronic resistance Carbon coated Al

Cubic S/N co-doped TiO_(2) with rich oxygen vacancies from Ti-MOFs for efficient elimination of formaldehyde

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Chinese chemical Letters 2024年第2期35卷 512-515页

作者： Qing Gao Lei Sun Zhihua Wang Jiguang Deng state key laboratory of chemical Resource engineering Beijing University of Chemical TechnologyBeijing 100029China Beijing key laboratory for green catalysis and Separation Key Laboratory of Beijing on Regional Air Pollution ControlKey Laboratory of Advanced Functional MaterialsEducation Ministry of ChinaDepartment of Chemical EngineeringBeijing University of TechnologyBeijing 100124China

The cubic S/N co-doped TiO_(2)(TNSx,x is the calcination temperature)photocatalysts with rich oxygen vacancies were obtained by high temperature calcination of sulfur powder and titanium-based MOFs NH_(2)-MIL-125 for the photocatalytic removal of gaseous formaldehyde(a volatile organic compound).Among the obtained catalysts,the presence of oxygen vacancies restricted photogenerated electron and holes recombination.98.00%removal of gaseous formaldehyde in 150 min could be achieved over TNS600 by xenon *** removal efficiency for formaldehyde was well retained for five cycle *** results from PL,TRPL and EIS revealed that TNS600 had the best separation efficiency of photogenerated electrons and holes,and the enhanced charge separation led to a significant increase in photocatalytic *** photocatalytic oxidation mechanism indicated that the ^(•)OH and ^(•)O_(2)−radicals were mainly involved in the efficient elimination of gaseous formaldehyde and were able to mineralize formaldehyde to H_(2)O and CO_(2).

关键词： Metal-organic frameworks Photocatalysis Formaldehyde removal S/N co-doped TiO_(2) Oxygen vacancies

A Web-like Three-dimensional Binder for Silicon Anode in Lithium-ion Batteries

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Energy & Environmental Materials 2024年第1期7卷 21-27页

作者： Liyuan Li Tao Li Yifan Sha Baozeng Ren Lan Zhang Suojiang Zhang CAS key laboratory of green Process and engineering Beijing Key Laboratory of Ionic Liquids Clean ProcessState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of chemical engineering Zhengzhou UniversityZhengzhou 450001China Langfang green industrial Technology Center Langfang 065001China Henan key laboratory of Energy Storage Materials and Processes Zhengzhou Institute of Emerging Industrial TechnologyZhengzhou 450003China

Si anode is of paramount importance for advanced energy-dense lithium-ion batteries(LIBs).However,the large volume change as well as stress generates during its lithiation-delithiation process poses a great challenge to the long-term cycling and hindering its *** this work,a composite binder is prepared with a soft component,guar gum(GG),and a rigid linear polymer,anionic polyacrylamide(APAM).Rich hydroxy,carboxyl,and amide groups on the polymer chains not only enable intermolecular crosslinking to form a web-like binder,A2G1,but also realize strong chemical binding as well as physical encapsulating to Si *** resultant electrode shows limited thickness change of merely 9%on lithiation and almost recovers its original thickness on *** demonstrates high reversible capacity of 2104.3 mAh g^(-1)after 100 cycles at a current density of 1800 mA g^(-1),and in constant capacity(1000 mAh g^(-1))test,it also shows a long life of 392 ***,this soft-hard combining web-like binder illustrates its great potential in the future applications.

关键词： anionic polyacrylamide lithium-ion batteries Si anode thickness change web-like binder

Building stabilized Cu_(0.17)Mn_(0.03)V_(2)O_(5−□)·2.16H_(2)O cathode enables an outstanding room‐/low‐temperature aqueous Zn‐ion batteries

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Carbon Energy 2024年第8期6卷 25-35页

作者： Ao Wang Dai‐Huo Liu Lin Yang Fang Xu Dan Luo Haozhen Dou Mengqin Song Chunyan Xu Beinuo Zhang Jialin Zheng Zhongwei Chen Zhengyu Bai key laboratory of green chemical Media and Reactions Ministry of EducationCollaborative Innovation Center of Henan Province for Green Manufacturing of Fine ChemicalsSchool of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiangHenanChina The state key laboratory of catalysis(SKLC) Power Battery and System Research CenterDalian Institute of Chemical PhysicsChinese Academy of SciencesDalianChina

Vanadium oxide cathode materials with stable crystal structure and fast Zn^(2+)storage capabilities are extremely important to achieving outstanding electrochemical performance in aqueous zinc‐ion *** this work,a one‐step hydrothermal method was used to manipulate the bimetallic ion intercalation into the interlayer of vanadium *** pre‐intercalated Cu ions act as pillars to pin the vanadium oxide(V‐O)layers,establishing stabilized two‐dimensional channels for fast Zn^(2+)*** occupation of Mn ions between V‐O interlayer further expands the layer spacing and increases the concentration of oxygen defects(Od),which boosts the Zn^(2+)diffusion *** a result,as‐prepared Cu_(0.17)Mn_(0.03)V_(2)O_(5−□)·2.16H_(2)O cathode shows outstanding Zn‐storage capabilities under room‐and lowtemperature environments(e.g.,440.3 mAh g^(−1)at room temperature and 294.3 mAh g^(−1)at−60°C).Importantly,it shows a long cycling life and high capacity retention of 93.4%over 2500 cycles at 2 A g^(−1)at−60°***,the reversible intercalation chemistry mechanisms during discharging/charging processes were revealed via operando X‐ray powder diffraction and ex situ Raman *** strategy of a couple of 3d transition metal doping provides a solution for the development of superior room‐/lowtemperature vanadium‐based cathode materials.

关键词： aqueous zinc‐ion batteries Cu_(0.17)Mn_(0.03)V_(2)O_(5−□)·2.16H_(2)O oxygen defects room‐/lowtemperature performance stabilized nanostructure

Selective photosynthesis of imines from biomass-derived aldehydes over Ni/TiO_(2)

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Rare Metals 2024年第3期43卷 1116-1124页

作者： Wu-Lin Li Qing-Qing Zhang Lin Dong Wen-Jun Zhang Li-Li Lin Zu-Peng Chen Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources International Innovation Center for Forest Chemicals and MaterialsCollege of Chemical EngineeringNanjing Forestry UniversityNanjing210037China Institute of industrial catalysis State Key Laboratory of Green Chemistry Synthesis TechnologyCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou310014China

Photocatalytic reductive amination of biomass-derived aldehydes is a desirable way to selectively upgrade biomass into value-added nitrogen-containing chemicals under mild ***,it is challenging to produce imines in high selectivity because of the undesirable side reactions caused by the activity of functional ***,we demonstrate the highly reactive and selective production of imines from biomass derived aldehydes via the photocatalytic reductive amination,using a defective TiO_(2)supported nickel *** employment of methanol as the hydrogen donor and ammonia solution as the nitrogen source avoids the use of high-pressure H_(2)and expensive amines,rendering the current catalytic process safe,economical,and environmentally *** depth investigations attribute the improved separation and transfer of photogenerated charge carriers to the presence of oxygen vacancies and decorated Ni nanoparticles,thereby accelerating the production of imines from benzaldehyde amination(conversion,95.8%;seleetivity,95.2%).Furthermore,the developed system could be easily translated to the photocatalytic conversions of various biomass derived aldehydes,which provided an example of a cost-effective and sustainable approach for the valorization of biomass derived feedstocks.

关键词： Photocatalysis Biomass derivatives Imines Reduction amination Heterogeneous catalyst