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Synergetic Control of Li+ Transport Ability and Solid Electrolyte Interphase by Boron-Rich Hexagonal Skeleton Structured All-Solid-State Polymer Electrolyte

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Energy & Environmental Materials 2024年第3期7卷 158-167页

作者： Yanan Li Shunchao Ma Yuehua Zhao Silin Chen Tingting Xiao Hongxing Yin Huiyu Song Xiumei Pan Lina Cong Haiming Xie department of chemistry National & Local United Engineering Laboratory for Power BatteryNortheast Normal University State Key laboratory of Electroanalytical chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences

High Li+transference number electrolytes have long been understood to provide attractive candidates for realizing uniform deposition of Li+.However,such electrolytes with immobilized anions would result in incomplete solid electrolyte interphase （SEI） formation on the Li anode because it suffers from the absence of appropriate inorganic components entirely derived from anions ***,a boron-rich hexagonal polymer structured all-solid-state polymer electrolyte （BSPE+ 10%LiBOB）with regulated intermolecular interaction is proposed to trade off a high Li+transference number against stable SEI *** Li+transference number of the as-prepared electrolyte is increased from 0.23 to 0.83 owing to the boron-rich cross-linker （BC） *** intriguingly,for the first time,the experiments combined with theoretical calculation results reveal that BOB-anions have stronger interaction with B atoms in polymer chain than TFSI-,which significantly induce the TFSI-decomposition and consequently increase the amount of LiF and Li3N in the SEI ***,a LiFePO4|BSPE+ 10%LiBOBlLi cell retains 96.7%after 400 cycles while the cell without BC-resisted electrolyte only retains 40.8%.BSPE+ 10%LiBOB also facilitates stable electrochemical cycling of solid-state Li-S *** study blazes a new trail in controlling the Li+transport ability and SEI properties,synergistically.

关键词： all-solid-state electrolyte boron-rich polymer lithium metal batteries lithium-ion transference number solid electrolyte interphase layer

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Electric-field-controlled highly regioselective thiocyanation of N-containing heterocycles

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Science China chemistry 2024年第4期67卷 1263-1269页

作者： Ming Gong Qian Wu Jung Keun Kim Mengmeng Huang Yabo Li Yangjie Wu Jong Seung Kim Henan Key laboratory of Chemical Biology and Organic chemistry Key Laboratory of Applied Chemistry of Henan UniversitiesCollege of ChemistryZhengzhou UniversityZhengzhou 450052China department of chemistry Korea UniversitySeoul 02841Korea

Achieving highly regioselective synthesis in organic chemistry is challenging due to the uncontrollable orientation between reacting *** electric fields(EEFs)can influence the reactivity and selectivity of the substrate by causing directional ***,scalable and efficient techniques for using EEFs as“smart catalysts”have been lacking,hindering their *** this study,we present a novel method for modifying the regioselectivity of quinoxaline-2(1H)-ones by functionalizing their C7-position using the electric double layer(EDL)*** approach led to moderate to good yields of the corresponding C7-thiocyanation *** calculations and control experiments demonstrated that EEFs could reverse the regioselectivity of quinoxaline-2(1H)-ones,allowing the C7-thiocyanation to proceed via a radical reaction ***,the resulting 7-thiocyano-1-methylquinoxaline-2(1H)-ones exhibited promising AIE *** work showcases a promising strategy for achieving highly regioselective functionalization by aligning the electric field with the desired reaction/bond axis.

关键词： electric fields reaction-axis rule electric double layer C7-thiocyanation C-S bond formation

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Analysis of synthetic parameters for coating aluminum powders with phenyltriethoxysilane coupling agent and their effects on powder flow behavior

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Particuology 2024年第7期90卷 412-417页

作者： Lillian M.Mawby Bellamarie Ludwig Benjamin J.Lear department of chemistry The Pennsylvania State UniversityUniversity ParkPA16802USA applied research laboratory The Pennsylvania State UniversityUniversity ParkPA16802USA

Though silanization of aluminum powder is currently used to improve its flow properties,for use as an alternative fuel source,there are a wide range of experimental parameters for the process and not all of them have been thoroughly *** this is complete,it is unknown if the process is optimized in terms of time,efficiency,and ***,we report on a study into the effects of changes in humidity,degree of agitation,reaction temperature,and curing time upon the deposition of phenyl triethoxysilane into 20μm(d50)aluminum *** confirm the deposition of the coating via diffuse reflectance infrared spectroscopy and x-ray photoelectron *** then characterize the coated particles using apparent density measurements and Carney flow *** analysis of variance,we find that,of the parameters explored,only changes in cure time and reaction temperature provide meaningful changes to the apparent density,while none of our parameters produced statistically significant changes in Carney flow ***,we conclude that,when optimizing silanization of aluminum particles,environmental control of humidity is unneeded and that the reaction can be run with minimal *** ability to largely ignore these parameters is a benefit to large-scale processing.

关键词： Aluminum powder Silane Fluidization Apparent density Carney flow

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Polypyride intercalation boosting the kinetics and stability of V3O7·H2O cathodes for aqueous zinc-ion batteries

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Journal of Energy chemistry 2024年第10期97卷 361-370页

作者： Qingqing He Jie Bai Mengda Xue Yanxin Liao Huayu Wang Mujun Long Lingyun Chen department of applied chemistry School of Chemistry and Chemical Engineering Chongqing University laboratory of Materials and Metallurgy College of Materials Science and Engineering Chongqing University

V3O7·H2O（VO） is a high capacity cathode material in the field of aqueous zinc ion batteries（AZIBs）,but it is limited by slow ion migration and low electrical *** this paper,polypyridine（PPyd） intercalated VO with nanoribbon structure was prepared by a simple in-situ pre-intercalation,which is noted *** total density of states（TDOS） shows that after the pre-intercalation of PPyd,an intermediate energy level appears between the valence band and conduction band,which provides a step that can effectively reduce the band gap and enhance the electron ***,the density functional theory（DFT） results found that Zn2+is more easily de-intercalated from the V-O skeleton,which proves that the embeddedness of PPyd improves the diffusion kinetics of Zn2+.Electrochemical studies have shown that VO-PPyd cathode materials exhibit excellent rate performance(high specific capacity of 465 and 192 mA h g-1at 0.2 and 10 A g-1,respectively) and long-term cycling performance（92.7%capacity retention rate after 5300 cycles）,due to their advantages in structure and *** importantly,the energy density of VO-PPyd//Zn at 581 and 5806 W kg-1is 375 and 247 W h kg-1,***-PPyd exhibits excellent electrochemical properties compared to previously reported vanadium based cathodes,which makes it highly competitive in the field of high-performance cathode materials of AZIBs.

关键词： Aqueous zinc ion batteries DFT calculation Electrical conductivity Ion migration Polypyridine V3O7·H2O

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Emerging perovskite materials for supercapacitors:Structure,synthesis,modification,advanced characterization,theoretical calculation and electrochemical performance

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Journal of Energy chemistry 2024年第2期89卷 41-70,I0003页

作者： Yuehua Qian Qingqing Ruan Mengda Xue Lingyun Chen department of applied chemistry School of Chemistry and Chemical EngineeringChongqing UniversityChongqing 401331China

As a new generation electrode materials for energy storage,perovskites have attracted wide attention because of their unique crystal structure,reversible active sites,rich oxygen vacancies,and good *** this review,the design and engineering progress of perovskite materials for supercapacitors(SCs)in recent years is ***,the review will focus on four types of perovskites,perovskite oxides,halide perovskites,fluoride perovskites,and multi-perovskites,within the context of their intrinsic structure and corresponding electrochemical performance.A series of experimental variables,such as synthesis,crystal structure,and electrochemical reaction mechanism,will be carefully analyzed by combining various advanced characterization techniques and theoretical *** applications of these materials as electrodes are then featured for various ***,we look forward to the prospects and challenges of perovskite-type SCs electrodes,as well as the future research direction.

关键词： Perovskite Modification engineering Oxygen vacancy Theoretical calculation methodology Supercapacitor

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Differentially-grown cobalt regulators cooperatively involved in the tandem catalysis for high-yield production of second amines

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Nano research 2024年第4期17卷 2444-2450页

作者： Jinhui Xu Xiao Wang Ying Wang Fei Wang Lingling Zhang Wenjie Cui Shuyan Song Hongjie Zhang State Key laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China department of chemistry Tsinghua UniversityBeijing 100084China

One-pot tandem catalysis has been regarded as one of the most atomic economic ways to produce secondary amines,the important platform molecules for chemical synthesis and pharmaceutical manufacture,but it is facing serious issues in overall *** promotional effects are highly desired for boosting the activity and regulating the selectivity of conventional tandem *** this work,we report a high-performance tandem catalyst with maximized synergistic effect among each counterpart by preciously manipulating the spatial structure,which involves the active CeO_(2)/Pt component as kernel,the densely-coated N-doped C(NC)layer as selectivity controller,and the differentially-grown Co species as catalytic performance *** comprehensive investigations,the unique growth mechanism and the promotion effect of Co regulators are ***,the surface-landed Co clusters(Cocs)are crucial to selectivity by altering the adsorption configuration of benzylideneaniline ***,the inner Co particles(Cops)are essential for activity by denoting their electrons to neighboring *** from the unique promotion effect,a remarkably-improved catalytic efficiency(100%nitrobenzene conversion with 94%N-benzylaniline selectivity)is achieved at a relatively low temperature of 80℃,which is much better than that of CeO_(2)/Pt(100%nitrobenzene conversion with 12%N-benzylaniline selectivity)and CeO_(2)/Pt/NC(35%nitrobenzene conversion with 94%benzylideneaniline selectivity).

关键词： tandem catalysis CeO_(2) hierarchical structure heterogeneous catalyst dual-site materials

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High-efficiency Ce-modified ZSM-5 nanosheets for waste plastic upgrading

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Nano research 2024年第6期17卷 5645-5650页

作者： Xiaomei Wang Xueting Wu Meng Zhao Rui Zhang Zijian Wang Yuou Li Liangliang Zhang Xiao Wang Shuyan Song Hongjie Zhang State Key laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China department of chemistry Tsinghua UniversityBeijing 100084China

Zeolite-based catalyst hydrocracking of plastics is a potential strategy for mitigating the environmental impacts of plastic wastes and recycling valuable resources,but difficult mass transfer,low concentration of acid sites,and high cost are still barriers to their practical *** this paper,we report an excellent hydrocracking catalyst of ZSM-5 nanosheets(Ce/b-ZSM-5)modified by Ce species with high conversion up to 96.3%,C_(3)−C_(5)selectivity up to 80.9%,and good stability during the hydrogenation of low-density *** comprehensive studies,b-ZSM-5 shows higher molecular diffusion efficiency and acid site concentrations compared with normal ZSM-5(n-ZSM-5)and hollow ZSM-5(h-ZSM-5).The introduction of Ce species into b-ZSM-5 further increases the density of Brønsted(B)and Lewis(L)acid sites as active sites,which enhances the adsorption of substrates and facilitates the formation of intermediates and desorption of *** a result,the hydrocracking activity of Ce/b-ZSM-5 is significantly improved.

关键词： rare earth zeolite plastic degradation catalytic hydrocracking morphology acidic site

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Molecule aging induced by electron attacking

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Journal of Energy chemistry 2024年第6期93卷 519-525,I0013页

作者： Ping Song Yining Dong Xue Gong Mingbo Ruan Baoxin Ni Xuanhao Mei Kun Jiang Weilin Xu State Key laboratory of Electroanalytical chemistry and Jilin Province Key laboratory of Low Carbon Chemical Power Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of applied chemistry and Engineering University of Science and Technology of Chin1Hefei 230026AnhuiChina Shanghai Key laboratory of Molecular Catalysis and Innovative Materials Collaborative Innovation Center of Chemistry for Energy MaterialsDepartment of ChemistryFudan UniversityShanghai 200438China

Here we propose a new concept of"molecule aging":with some special treatment,a molecule could be"aged"by losing some unknown tiny particles or pieces from atoms in the molecule,Such"aging"or loss of unknown tiny particles does not change apparently its molecular structure or chemical composition,but some physicochemical properties could be changed *** further confirm such"molecule aging"via a long-term electron attacking to age water(H_(2)O)*** IR spectra show no structural difference between the fresh water and the aged one,while the NMR spectra show that the electron attacking can decrease the size of water *** facts indicate that the electron attacking indeed can"affect"the structure of water molecule slightly but without damaging to its basic molecule *** exploration reveals that the hydrogen evolution reaction(HER)activity of the aged water molecule is lower than the fresh water on the same Pt/C *** density functional theory calculations indicate that the shortened O-H bond in H_(2)O indeed can present lower HER activity,so the observed size decrease of water clusters from NMR probably could be attributed to the shortening of O-H bond in water *** results indicate significantly that the molecule aging can produce materials with new functions for new possible applications.

关键词： Aging of molecules Electron attacking Full width at half maxima Hydrogen evolution reaction

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Lanthanide-based microlasers:Synthesis,structures,and biomedical applications

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Nano research 2024年第1期17卷 97-111页

作者： Qian Zhang Yawei Liu Kai Liu Hongjie Zhang Engineering research Center of Advanced Rare Earth Materials(Ministry of Education) Department of ChemistryTsinghua UniversityBeijing 100084China State Key laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Xiangfu laboratory Jiaxing 314102China

The large size of lasers limits their applications in confined spaces,such as in biosensing and in vivo brain tissue *** this regard,micron-sized lasers have been *** exhibit great potential for biological detecting,remote sensing,and depth tracking due to their small sizes,sensitive properties of their spectral fingerprints,and flexible positional modulation in the ***-based luminescent materials that possess long excited-state lifetime,narrow emission bandwidth,and upconversion behaviors are promising as gain mediums for novel *** addition,lanthanide-based microlasers could be generated under natural ambient conditions with pumped or continuous light sources,which significantly promotes the practical applications of *** progress in the design,synthesis,and biomedical applications of lanthanide-based microlasers has been outlined in this *** ions doped and upconverted lanthanide-based microlasers are highlighted,which exhibit advantageous structures,miniaturized dimensions,and high lasing *** applications of lanthanide-based microlasers are further discussed,the upconverted microlasers show great advantages for biological applications owing to their tunable excitation and emission characteristics and excellent environmental ***,perspectives and challenges in the field of lanthanide-based microlasers are presented.

关键词： microlasers lanthanide-based luminescent materials upconversion nanoparticles biological applications

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Evoking immune system to potentiate nanocatalytic therapy through activation of cGAS-STING pathway

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Science China chemistry 2024年第10期67卷 3310-3319页

作者： Yi Wei Yuan Liang Pengye Du Shuyu Liu Pengpeng Lei Xiuling Liu Hongjie Zhang School of Materials Science and Engineering Changchun University of Science and Technology State Key laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of Sciences School of applied chemistry and Engineering University of Science and Technology of China research Institute of Changchun University of Science and Technology in Chongqing department of chemistry Tsinghua University

Nanocatalytic therapy shows great potential for therapeutic interventions. However, therapeutic efficiency is often limited by unsatisfactory enzyme activity and lack of the coordination of immune system. Therefore, engineering nanozymes activity enhancement while activating immune system will be an effective strategy to achieve efficient tumor therapy. Herein, we synthesize a DSPE-PEG-FA modified manganese dioxide-based dual-atom nanozyme（MDF）, on which iridium and platinum atoms are anchored. The obtained MDF can simultaneously mimic four enzyme activities of catalase, oxidase, peroxidase, and glutathione oxidase, set off a reactive oxygen species（ROS） storm, cause tumor cell death. The enzyme activity of MDF can be enhanced by its own photothermal effect. Meanwhile, MDF can consume intracellular glutathione and release Mn2+, which can prevent generated ROS from consumption and further activate cyclic guanosine monophosphate-adenosine monophosphate synthase-stimulator of interferon genes（cGAS-STING） pathway and promote the secretion of type I interferon, which will help promote dendritic cells maturation, present antigens to T lymphocytes to help kill tumor cells. Ultimately, MDF shows excellent tumor suppressive effects. This work provides a new paradigm for the field of nanozymes and offers a new reference for involvement of cGAS-STING pathway activation in tumor catalytic therapy.

关键词： single-atom ROS immune activation cGAS-STING pathway nanocatalytic therapy

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