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Tetraphenylethylene-derived organic cages with persistent photogenic radicaloids and efficient photothermal conversion

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Science China Chemistry 2025年第2期68卷 661-669页

作者： Suqiong Yan Bo Yang Fanda Feng Yuan Zhang Shirong Ban Hui Ma Wei Huang state Key Laboratory of Coordination Chemistry School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210093China Shenzhen Research Institute of Nanjing university Shenzhen 518057China

Transformation of the electronic spin states has received significant interest in recent years because of its applications in the magnetic information storage materials and optical response ***,it can be formidably challenging to use ultraviolet(UV)light as a contactless stimulus to alter the electronic spin states of the supramolecular *** by the approach on the radical cation mechanism of the Scholl reaction and the photocyclization reactivity of tetraphenylethylene(TPE)derivatives,we report two photochromic cages(cage-TPE-1 and cage-TPE-2)that can be photochemically transformed from electron paramagnetic resonance(EPR)-silent to EPR-active form via UV irradiation due to the photo-induced electron transfer process at the TPE *** provided a strong single-electron signal with a g value of 2.003 in cage-TPE-1 and cage-TPE-2 but no signal was detected for the pristine samples without the *** transformation can be monitored by ultraviolet–visible–near-infrared(UV–vis–NIR)and photoluminescence(PL)*** photogenic radical cage intermediate was unstable in solution resulting in the degradation and intramolecular cyclization of the reactive species,while the radicals were found to be stable and persistent in the solid state due to the spin delocalization,the steric protection of confined cavities,and the oxygen *** theoretical calculations and spectral measurements suggest that the photogenic radical cage-TPE-2(•+)experiences photocyclization on the TPE *** with the close-shell cage,the radical cage-TPE-1(•+)and cage-TPE-2(•+)exhibit better photothermal conversion performance due to the incubated infrared absorption from open-shell electron feature and reduced band gap.

关键词： supramolecular cage photogenic radical photocyclization photothermal conversion

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Tandem asymmetric dearomatized functionalization reaction of phenols with Evans-ynamides enabled by divergent electrophiles

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Science China Chemistry 2025年第2期68卷 649-660页

作者： Ying-Qi Zhang Gan-Lu Qian Yun Liu Jia-Hui Li Xin Hong Zhou Xu Bo Zhou Long-Wu Ye state Key Laboratory of Physical Chemistry of Solid Surfaces Key Laboratory of Chemical Biology of Fujian Provinceand College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Center of Chemistry for Frontier Technologies Department of ChemistryState Key Laboratory of Clean Energy UtilizationZhejiang UniversityHangzhou 310027China Jiangsu Key Laboratory of New Drug Research and Clinical Pharmacy School of PharmacyXuzhou Medical UniversityXuzhou 221004China state Key Laboratory of Elemento-Organic Chemistry Nankai UniversityTianjin 300071China state Key Laboratory of Organometallic Chemistry Chinese Academy of SciencesShanghai 200032China

Herein,we disclose a highly regio-/chemoselective tandem asymmetric dearomatized halofunctionalization reaction of phenoltethered ynamides with diverse electrophilic halogenation sources in a catalyst-free manner for the practical and rapid assembly of a series of halogenated spirocyclic ***,the related dearomatized selenation and protonation are also achieved,affording the corresponding selenated and protonated spirocycles in high ***,the enantioselectivities of these products can be perfectly induced by Evans auxiliaries(99%ees).Significantly,this protocol not only represents the first tandem asymmetric halofunctionalization reaction of phenol derivatives,but also constitutes the first asymmetric halogenation/selenation of *** calculations indicate a remote induction model of Evans chiral auxiliary-attached keteniminium.

关键词： alkynes cyclization dearomatization Evans chiral auxiliary spirocycles

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Uncovering fantastic synergistic lithium adsorption with manganese-titanium based composite nanospheres:Mild synthesis and molecular dynamics simulation insights

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Journal of Energy Chemistry 2025年第2期101卷 52-67页

作者： Yameng Wang Zi-Yu Liu Yubei Su Yu Liu Aoqun Liu Xiaoye Zhang Yugang Huang Liyun Zhang Haisheng Chen Wancheng Zhu Department of Chemical Engineering Qufu Normal University Institute of Engineering Thermophysics Chinese Academy of Sciences state Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology

In light of the burgeoning energy technology sector and the ever-growing demand for lithium across diverse industrial domains,conventional lithium extraction methods have been proven inadequate due to their limited production capacity and high operational *** work introduces a novel approach to the manganese-titanium based composite HMTO（Mn:Ti=1:4） lithium ion-sieve（LIS） nanospheres,employing lithium acetate dihydrate,manganese carbonate and titanium dioxide P25 as the primary *** nanospheres exhibit relatively uniform spherical morphology,narrow size distribution,small average particle size（ca.55 nm）,large specific surface area(43.58 m2g-1) and high surface O2-content（59.01%）.When utilized as the adsorbents for Li+ions,the HMTO（Mn:Ti=1:4） LIS demonstrates a fast adsorption rate,approaching equilibrium within 6.0 h with an equilibrium adsorption capacity（qe）of 79.5 mg g-1and a maximum adsorption capacity（qm） of 87.26 mg g-1(initial concentration CO:1.8 g L-1).In addition,the HMTO（Mn:Ti=1:4） also delivers a high lithium extraction from the simulated high magnesium-lithium molar ratio salt lake brine（Mg:Li=103）,achieving a qeof 33.85 mg g-1along with a remarkable selectivity(αMgLi=2192.76).Particularly,the HMTO（Mn:Ti=1:4） LIS showcases a satisfactory recycling adsorption *** adsorption capacity remains at a high level,even that determined after the 5th cycle(55.45 mg g-1) surpasses that of the most recently reported ***,the fantastic synergistic lithium adsorption mechanism is deliberately uncovered by leveraging the ion exchange principles and molecular dynamics（MD） simulations.

关键词： Adsorption performance Ion exchange Lithium ion-sieves Manganese titanium composite Salt lake brine lithium extraction

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Tailoring BaCe0.7Zr0.1(Dy0.1|Yb0.1)0.2O3-δ electrolyte through strategic Cu doping for low temperature proton conducting fuel cells:Envisioned theoretically and experimentally

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Journal of Energy Chemistry 2025年第2期101卷 692-701页

作者： Zaheer Ud Din Babar Muhammad Bilal Hanif Yan'an Li Wan-Ting Wang Hanchen Tian Cheng-Xin Li state Key Laboratory for Mechanical Behavior of Materials School of Materials Science and Engineering Xi'an Jiaotong University Department of Inorganic Chemistry Faculty of Natural Sciences Comenius University Bratislava

This study addresses the challenge of high sintering temperatures in proton-conducting fuel cells（PCFCs）with BaCeO3-doped *** demonstrate that 1 mol% copper（Cu） doping at the B-site of BaCe0.7Zr0.1(Dy0.1|Yb0.1)0.2O3-δ（BCZDYb） improves sintering behavior,enabling densification at1400℃.However,Cu doping disrupts stoichiometry,creating barium vacancies and reducing protonaccepting cations,affecting overall *** mechanism is confirmed through density functional theory（DFT） calculations and various experimental techniques,including crystal structure analysis using X-ray diffraction（XRD） and morphology and elemental analysis via field emission scanning electron microscopy（FESEM） and energy-dispersive X-ray spectroscopy（EDS）.Electrochemical measurements are performed using the electrochemical impedance spectroscopy（EIS）.The ionic conductivity of1 mol% Cu-doped BCZDYb（BCZDYb-1） is 1.49×10-2S cm-1at 650℃,which is～3.58 times higher than that of BCZDYb sintered at 1200℃.The BCZDYb-1 exhibits ～16 times higher grain boundary conductivity when sintered at 1400℃,compared to undoped *** single cell employing BCZDYb-1 as the electrolyte achieved a power density of ～606 mW cm-2at 550℃.These results indicate that a controlled amount of Cu doping can enhance densification while maintaining high ionic co nductivity,making it suitable for practical applications in PCFCs operating at lower temperatures.

关键词： BaCe0.7Zr0.1(Dy0.1|Yb0.1)0.2O3−δ (BCZDYb) Cu-doping Densification Electrical conductivity Proton conducting fuel cells (PCFCs) Sintering

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From Static and Dynamic Perspectives:A Survey on Historical Data Benchmarks of Control Performance Monitoring

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IEEE/CAA Journal of Automatica Sinica 2025年第2期12卷 300-316页

作者： Pengyu Song Jie Wang Chunhui Zhao Biao Huang the state Key Laboratory of Industrial Control Technology College of Control Science and Engineering Zhejiang University IEEE the Department of Chemical and Materials Engineering University of Alberta

In recent decades, control performance monitoring(CPM) has experienced remarkable progress in research and industrial applications. While CPM research has been investigated using various benchmarks, the historical data benchmark(HIS) has garnered the most attention due to its practicality and effectiveness. However, existing CPM reviews usually focus on the theoretical benchmark, and there is a lack of an in-depth review that thoroughly explores HIS-based methods. In this article, a comprehensive overview of HIS-based CPM is provided. First, we provide a novel static-dynamic perspective on data-level manifestations of control performance underlying typical controller capacities including regulation and servo: static and dynamic properties. The static property portrays time-independent variability in system output, and the dynamic property describes temporal behavior driven by closed-loop feedback. Accordingly,existing HIS-based CPM approaches and their intrinsic motivations are classified and analyzed from these two ***, two mainstream solutions for CPM methods are summarized, including static analysis and dynamic analysis,which match data-driven techniques with actual controlling behavior. Furthermore, this paper also points out various opportunities and challenges faced in CPM for modern industry and provides promising directions in the context of artificial intelligence for inspiring future research.

关键词： Control performance monitoring (CPM) data-driven method historical data benchmark (HIS) industrial process performance index static and dynamic analysis

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Fatigue properties and constitutive model of Jintan salt rock subjected to complex cyclic loading

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International Journal of Mining Science and Technology 2025年第1期35卷 121-133页

作者： Qingchuan He Jianfeng Liu Fei Wu Cunbao Li Jie Chen Renbo Gao Chunfeng Ye Shijie Zhu state Key Laboratory of Coal Mine Disaster Dynamics and Control Chongqing UniversityChongqing 400044China state Key Laboratory of Hydraulics and Mountain River Engineering Sichuan UniversityChengdu 610065China state Key Laboratory of Intelligent Construction and Healthy Operation and Maintenance of Deep Underground Engineering College of Civil and Transportation EngineeringShenzhen UniversityShenzhen 518060China state Key Laboratory of Geomechanics and Geotechnical Engineering Institute of Rock and Soil MechanicsChinese Academy of SciencesWuhan 430071China

Salt cavern energy storage technology contributes to energy reserves and renewable energy *** study focuses on salt cavern gas storage in Jintan to assess the long-term stability of its surrounding rock under frequent *** fatigue test results indicate that stress holding significantly reduces fatigue life,with the magnitude of stress level outweighing the duration of holding time in determining peak *** a machine learning approach,the impact of various factors on fatigue life and peak strain was quantified,revealing that higher stress limits and stress holding adversely impact the fatigue index,whereas lower stress limits and rate exhibit a positive effect.A novel fatigue-creep composite damage constitutive model is constructed,which is able to consider stress magnitude,rate,and stress *** model,validated through multi-path tests,accurately captures the elasto-viscous behavior of salt rock during loading,unloading,and stress *** analysis further reveals the time-and stress-dependent behavior of model parameters,clarifying that strain changes stem not only from stress variations but are also influenced by alterations in elasto-viscous *** study provides a new method for the mechanical assessment of salt cavern gas storage surrounding rocks.

关键词： Salt cavern gas storage Cyclic loading Fatigue characteristics Constitutive model

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2D copper-iron bimetallic metal-organic frameworks for reduction of nitrate with boosted efficiency and ammonia selectivity

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Journal of Environmental Sciences 2025年第3期149卷 374-385页

作者： Qian Ma Yinghao Xue Chuning Zhang Yanyan Chen Wei Teng Hua Zhang Jianwei Fan state Key Laboratory of Pollution Control and Resources Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China

Electrocatalytic reduction of nitrate to ammonia has been considered a promising and sustainable pathway for pollutant treatment and ammonia has significant potential as a clean ***,the method has received much *** this work,Cu/Fe 2D bimetallic metal-organic frameworks were synthesized by a facile method applied as cathode materials without high-temperature *** centers(Cu,Fe)with enhanced intrinsic activity demonstrated higher removal ***,the 2D nanosheet reduced themass transfer barrier between the catalyst and nitrate and increased the reaction ***,the catalysts with a 2D structure showed much better removal efficiency than other structures(3D MOFs and BulkMOFs).Under optimal conditions,Cu/Fe-2D MOF exhibited high nitrate removal efficiency(87.8%)and ammonium selectivity(89.3%)*** ammonium yielded up to significantly 907.2μg/(hr·mg_(cat))(7793.8μg/(hr·mg_(metal)))with Faradaic efficiency of 62.8%at an initial 100 mg N/*** catalyst was proved to have good stability and was recycled 15 times with excellent *** simulations confirm the reduced Gibbs free energy of Cu/Fe-2D *** study demonstrates the promising application of Cu/Fe-2D MOF in nitrate reduction to ammonia and provides new insights for the design of efficient electrode materials.

关键词： Metal-organic frameworks Electrochemical denitrification Ammonium selectivity 2D bimetal materials

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A self-adaptive inorganic in-situ separator by particle crosslinking for nonflammable lithium-ion batteries

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Journal of Energy Chemistry 2025年第1期100卷 469-480页

作者： Jiarui Yang Jiuzhou Liu Wenrui Cai Ziyu Zhao Shan Wang Lu He Shanshan Lv Zhiwei Zhu Zhongfeng Ji Guojiang Wen Hua Li Yuanming Zhai Xuewei Fu Wei Yang Yu Wang College of Polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065SichuanChina

All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional liquid-state LIBs. However, the practical success of ASLS-LIBs is bottlenecked by the lack of advanced separator technology that can simultaneously realize high performances in puncturing-tolerability,fire-resistance, and importantly, wetting-capability with non-flammable liquid-electrolytes. Here, we propose a concept of inorganic in-situ separator(IISS) by hybrid-sol physical crosslinking directly onto the electrode surface to address the above challenges. Particularly, the hybrid-sol is designed with silica nanoparticles as the building block and poly(vinylidene difluoride) nanoparticles as the crosslinking agent. The critical factors for controlling the IISS microstructures and properties have been systematically investigated. The advantages of the IISS have been confirmed by its fast wetting with various fireresistant liquid-electrolytes, customizable thickness and porous structures, robust interface with planar or three-dimensional(3D)-structured electrodes, and importantly, unexpected self-adaptability against puncturing. Enabled by the above merits, a fire-resistant ASLS-LIB is successfully assembled and demonstrated with stable electrochemical performance. This sol-crosslinked IISS may open an avenue for the studies on the next-generation separator technology, cell assembling, solid electrolyte processing as well as non-flammable secondary batteries.

关键词： Safe liquid-state lithium-ion batteries In-situ separator technology Hybrid-sol physical crosslinking Electrode coating Inorganic nonflammable separator

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Dual-phase interface engineering via parallel modulation strategy for highly reversible Zn metal batteries

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Journal of Energy Chemistry 2025年第2期101卷 163-174页

作者： Zhean Bao Yang Wang Kun Zhang Guosheng Duan Leilei Sun Sinan Zheng Bin Luo Zhizhen Ye Jingyun Huang School of Materials Science and Engineering State Key Laboratory of Silicon and Advanced Semiconductor Materials Zhejiang University Institute of Wenzhou Zhejiang University Institute of Thermal Science and Power Systems Zhejiang University Longmen Laboratory of Luoyang

The reversibility and stability of aqueous Zn metal batteries（AZMBs） are largely limited by Zn dendrites and interfacial parasitic ***,we propose a parallel modulation strategy to boost the reversibility of the Zn anode by introducing N,N,N',N'-tetramethylchloroformamidinium hexafluorophosphate（TCFH） as an additive in the *** is composed of PF6-and TN+with opposite ***6-can spontaneously induce the in-situ generation of ZnF2solid electrolyte interface（SEI） on the anode,which can improve the transport kinetics of Zn2+at the interface,thus promoting the rapid and uniform deposition of Zn as well as inhibiting the growth of *** addition,TN+is enriched at the anode surface during Zn deposition through the anchoring effect,which brings a reconfiguration of the ion/molecule *** anchored-TN+reduces the concentrations of H2O and SO42-,sufficiently restraining the parasitic *** to the dual-phase interface engineering constructed of PF6-and TN+in parallel,the symmetric cell with the proposed electrolyte survives long cycling stability over750 h at 20 mA cm-2,10 mAh *** study offers a distinct viewpoint to the multidimensional optimization of Zn anodes for high-performance AZMBs.

关键词： Anchoring effect Aqueous Zn metal batteries Electrolyte additive Solid electrolyte interface Zn anode

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Catalytic detoxification of mitoxantrone by graphitic carbon nitride(g-C_(3)N_(4))supported Fe/Pd bimetallic nanoparticles

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Journal of Environmental Sciences 2025年第2期148卷 614-624页

作者： Qianyu Xu Haoyang Fu Jiyuan Gu Liyu Lei Lan Ling state Key Laboratory for Pollution Control and Resource Reuse College of Environmental Science and EngineeringTongji UniversityShanghai 200092China

The overuse of antibiotics and antitumor drugs has resulted in more and more extensive pollution of water bodies with organic drugs,causing detrimental ecological effects,which have attracted attention towards effective and sustainable methods for antibiotics and antitumor drug ***,the hybrid nanomaterial(g-C_(3)N_(4)@Fe/Pd)was synthesized and used to remove a kind of both an antibiotic and antitumor drug named mitoxantrone(MTX)with 92.0%removal efficiency,and the MTX removal capacity is 450 mg/*** exposing to the hybrid material the MTX aqueous solution changed color from dark blue to lighter progressively,and LC-UV results of residual solutions showthat a newpeak at 3.0min(MTX:13.2min)after removal by g-C_(3)N_(4)@Fe/Pd appears,with the simultaneous detection of intermediate products indicating that g-C_(3)N_(4)@Fe/Pd indeed degrades *** mass spectrometric analysis suggests that the nuclear mass ratio decreased from 445.2(M+1H)to 126.0(M+1H),169.1(M+1H),239.2(M+1H),267.3(M+1H),285.2(M+1H),371.4(M+1H)and 415.2(M+1H),and the maximum proportion(5.63%)substance of all degradation products(126.0(M+1H))is 40-100 times less toxic than MTX.A mechanism for the removal and degradation of mitoxantrone was ***,actual water experiments confirmed that the maximum removal capacity of MTX by g-C_(3)N_(4)@Fe/Pd is up to 492.4 mg/g(0.02 g/L,10 ppm).

关键词： Degradation LC-QTOF-MS Nanoparticles Mitoxantrone Aqueous solution

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