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Low-cost and fluoride-free synthesis of MFI zeolite nanosheets with enhanced stability for benzene alkylation with ethanol

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Journal of Energy Chemistry 2025年第1期100卷 458-468页

作者： Peng Zhu Cun Liu Yiren Yu Guoshu Gao Yumeng Zhao Xiongfu Zhang Guodong Liu Guohui Yang state key laboratory of fine chemicals School of Chemical Engineering Dalian University of Technology state key laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences

Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive structure-directing agents(SDAs), pricey raw materials, and eco-unfriendly fluorine-containing additives. Here, we contributed a cost-effective and fluoride-free synthesis method for synthesizing high-quality MFI zeolite nanosheets through a Silicalite-1(Sil-1) seed suspension and urea cooperative strategy, only with inexpensive colloidal silica as the Si source. Our approach was effective for synthesizing both Sil-1 and aluminum-containing ZSM-5 nanosheets. By optimizing key synthesis parameters,including seed aging time, seed quantity, and urea concentration, we achieved precise control over the crystal face aspect ratio and b-axis thickness. We also revealed a non-classical oriented nanosheet growth mechanism, where Sil-1 seeds induced the formation of quasi-ordered precursor particles, and the(010)crystal planes of these particles facilitated urea adsorption, thereby promoting c-axis-oriented *** obtained ZSM-5 nanosheets exhibited exceptional catalytic performance in the benzene alkylation with ethanol, maintaining stability for over 500 h, which is 5 times longer than traditional ZSM-5 catalysts. Furthermore, large-scale production of ZSM-5 nanosheets was successfully carried out in a 3 L highpressure autoclave, yielding samples consistent with those from laboratory-scale synthesis. This work marks a significant step forward in the sustainable and efficient production of MFI nanosheets using inexpensive and environmentally friendly raw materials, offering the broad applicability in catalysis.

关键词： MFI zeolite ZSM-5 Nanosheets Scale-up synthesis Aromatic alkylation

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Visualization of the protective role of estrogen against female liver fibrosis via an ER viscosity NIR fluorescent probe

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Science China Chemistry 2025年第1期 360-368页

作者： Zheng Liu Changyu Zhang Zipeng Li Wanying Ma Jia Liu Xiang Xia Ning Xu Wen Sun Jianjun Du Jiangli Fan Xiaojun Peng state key laboratory of fine chemicals Dalian University of Technology Ningbo Institute of Dalian University of Technology

Endoplasmic reticulum(ER) viscosity has emerged as a new potential biomarker for hepatic fibrosis(HF). Herein, we report the first ER-targeting viscosity-responsive near-infrared(NIR) fluorescent probe HBT-PP for investigations of HF *** twisted intramolecular charge transfer(TICT) and the excited state intramolecular proton transfer(ESIPT) are combined to endow HBT-PP with the selective response towards viscosity(～62-fold) and a super large stokes shift(～320 nm). HBT-PP mainly targets organelle ER and is able to image the drug-or alcohol-induced viscosity elevation in living cells. Significantly,HBT-PP was successfully applied to visualize the gender difference in HF and the protective role of estrogen in restraining HF progression. Of note, after 10 min of stain with HBT-PP, HF lesions showed a stage-based response, indicating the potential of this probe in fast and early diagnosis of HF. These results clearly demonstrated the promising application of HBT-PP as a new tool for exploring ER viscosity-involved physiological and pathological processes.

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Mechanistic insight into the synergy between nickel single atoms and nanoparticles on N-doped carbon for electroreduction of CO2

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Journal of Energy Chemistry 2025年第1期100卷 327-336页

作者： Mingdong Sun Wenwen Guan Cailing Chen Chao Wu Xiaoling Liu Biao Meng Tao Chen Yu Han Jun Wang Shibo Xi Yu Zhou state key laboratory of Materials-Oriented Chemical Engineering College of Chemical Engineering Nanjing Tech University Advanced Membranes and Porous Materials Center Physical Sciences and Engineering Division King Abdullah University of Science and Technology Institute of Sustainability for chemicals Energy and Environment A*STAR (Agency for Science Technology and Research) College of Materials Science and Engineering Sichuan University

The synergy of single atoms （SAs） and nanoparticles （NPs） has demonstrated great potential in promoting the electrocatalytic carbon dioxide reduction reaction （CO2RR）;however,the rationalization of the SAs/NPs proportion remains one challenge for the catalyst ***,a Ni2+-loaded porous poly（ionic liquids）(PIL) precursor synthesized through the free radical self-polymerization of the ionic liquid monomer,1-allyl-3-vinylimidazolium chloride,was pyrolyzed to prepare the Ni,N co-doped carbon materials,in which the proportion of Ni SAs and NPs could be facilely modulated by controlling the annealing *** catalyst Ni-NC-1000 with a moderate proportion of Ni SAs and NPs exhibited high efficiency in the electrocatalytic conversion of CO2into *** Ni K-edge X-ray absorption near-edge structure （XANES） spectra and theoretical calculations were conducted to gain insight into the synergy of Ni SAs and *** charge transfer from Ni NPs to the surrounding carbon layer and then to the Ni SAs resulted in the electron-enriched Ni SAs active *** the electroreduction of CO2,the coexistence of Ni SAs and NPs strengthened the CO2activation and the affinity towards the key intermediate of*COOH,lowering the free energy for the potential-determining*CO2→*COOH step,and therefore promoted the catalysis efficiency.

关键词： Single atom catalyst Synergy effect Carbon catalyst Electrocatalysis

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Electrochemical conversion of methane to bridge the gap in the artificial carbon cycle

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Journal of Energy Chemistry 2025年第1期100卷 286-308页

作者： Yuhao Peng Yuefeng Song Ihar Razanau Juanxiu Xiao Wei Xiao Di Hu Guoxiong Wang College of Chemistry and Molecular Sciences Hubei Key Laboratory of Electrochemical Power Sources Wuhan University state key laboratory of Catalysis Dalian National Laboratory for Clean Energy iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Dalian Institute of Chemical Physics Chinese Academy of Sciences laboratory of Physical-Chemical Technologies SSPA Scientific and Practical Materials Research Centre of NAS of Belarus state key laboratory of Marine Resources Utilization in South China Sea Collaborative Innovation Center of Marine Science and Technology School of Marine Science and Engineering Hainan University Department of Chemical and Environmental Engineering University of Nottingham Ningbo China

Methane, an abundant one-carbon（C1） resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO2emissions and coke deposition. Electrochemical conversion of methane（ECM） using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO2emission.

关键词： Methane Electrochemical conversion Reaction mechanism Catalyst design Electrode Electrocatalysis

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Manipulation of successive crystalline transformations to control electron transfer and switchable functions

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National Science Review 2018年第4期5卷 507-515页

作者： Cheng-Qi Jiao Wen-Jing Jiang Yin-Shan Meng Wen Wen Liang Zhao Jun-Li Wang Ji-Xiang Hu Gagik G.Gurzadyan Chun-Ying Duan Tao Liu state key laboratory of fine chemicals Dalian University of Technology Institute of Artificial Photosynthesis State Key Laboratory of Fine Chemicals Dalian University of Technology

Electron transfer in solid is crucial to switchable magnetic,electrical,optical and mechanical ***,it is a formidable challenge to control electron-transfer behaviors via manipulation of crystalline phases,especially through dynamic crystalline ***,three crystalline phases of an{Fe2Co2}compound were obtained via enhancement of intermolecularπ···πinteractions inducingsuccessive single-crystal-to-single-crystal transformations,from solvated 1·2CH3OH·4H2O,to desolvated1 and its polymorph 1a accompanying electron transfer.1·2CH3OH·4H2O showed thermally inducedreversible intermetallic electron transfer in mother *** electron-transfer behavior was observed in 1.1a showed reversible intermetallic electron transfer upon thermal treatment or alternative irradiation with808-and 532-nm lasers at cryogenic *** electron-transfer behaviors significantly change the magnetic and optical properties,providing a strategy to realize different electron-transfer behaviors andswitchable functions viaπ···πinteractions manipulated dynamic crystalline transformation.

关键词： electron-transfer dynamic structural transformation successive crystalline transformations reversible polymorphs

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Adjustable crystalline stereocomplexes from enantiopure gradient polycarbonates

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Science China Chemistry 2016年第11期59卷 1415-1420页

作者： Ye Liu Keke He Weimin Ren Rongrong Li Xiaobing Lu state key laboratory of fine chemicals Dalian University of Technology

Stereoselective interaction was observed in the mixture of enantiopure gradient polycarbonate(denoted as PCOPC-g-PCPC, originated from the enantioselective terpolymerization of CO2, 3,4-epoxytetrahydrofuran(COPO) and cyclopentene oxide(CPO)) and various isotactic polycarbonates with opposite configuration in chloroform solution. The resultant crystalline stereocomplexes exhibit enhanced thermal stability and new crystalline behaviors, significantly distinct from their parent polymers. It was found that the cocrystallization selectively occurred between(R)-PCOPC(CO_2/COPO copolymer) and(S)-PCOPC-enriched segment in the gradient terpolymer(S)-PCOPC-g-PCPC, while(R)-PCPC(CO_2/CPO copolymer) selectively complexed with(S)-PCPC-enriched segment. No stereocomplexation was observed between(S)-PCOPC-g-PCPC and(S)-PCOPC or(S)-PCPC. This study is beneficial to finding new routes to prepare various semicrystalline materials having a wide variety of physical properties and degradability.

关键词： crystalline polycarbonates gradient stereocomplex polymer assembly cocrystallization

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Beyond graphene oxides: Emerging 2D molecular sieve membranes for efficient separation☆

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Chinese Journal of Chemical Engineering 2019年第6期27卷 1257-1271页

作者： Yi Liu state key laboratory of fine chemicals Dalian University of Technology

Recent decades witnessed the significant progress made in the research field of 2D molecular sieve *** comparison with their 3D counterparts, 2D molecular sieve membranes possessed several unique advantages like significantly reduced membrane thickness(one atom thick in theory) and diversified molecular sieving mechanisms(in-plane pores within nanosheets & interlayer galleries between nanosheets). M. Tsapatsis first carried out pioneering work on fabrication of lamellar ZSM-5 membrane. Since then, diverse 2D materials typically including graphene oxides(GOs) have been fabricated into membranes showing promising prospects in energy-efficient gas separation, pervaporation, desalination and nanofiltration. In addition to GOs, other emerging 2D materials, including 2D zeolites, 2D metal–organic frameworks(MOFs), 2 D covalent-organic frameworks(COFs), layered double hydroxides(LDHs), transition metal dichalcogenides(TMDCs), MXenes(typically Ti3C2TX), graphitic carbon nitrides(typically g-C3N4), hexagonal boron nitride(h-BN) and montmorillonites(MT) are showing intriguing performance in membrane-based separation process. This article summarized the most recent developments in the field of 2D molecular sieve membranes aside from GOs with particular emphasis on their structure–performance relationship and application prospects in industrial separation.

关键词： Two-dimentional material Molecular sieves Membranes Separation Desalination

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Multiple active components synergistically driven heteroatom-doped porous carbon as high-performance counter electrode in dye-sensitized solar cells

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Journal of Energy Chemistry 2019年第4期28卷 89-94页

作者： Hongyu Jing Danyang Wu Suxia Liang Xuedan Song Yonglin An Ce Hao Yantao Shi state key laboratory of fine chemicals Dalian University of Technology

A facile template-free in situ self-activation approach for the multiple active components synergistically driven porous carbon was presented via a feasible annealing *** biomass-derived carbon without additional activation reagents was fabricated using K-rich pomelo peel(PP)as the carbon source,which possesses a high electric conductivity where abundant functional hetero-metal atoms are doped into the carbon framework that playing the role of catalytic *** K^+that exists within the biomass can induce self-activation during pyrolysis apart from the activating gases during the pyrolysis *** resulting electrocatalyst of PP-850(PP was pyrolyzed at 850°C in an N_2atmosphere)with abundant heteroatoms possesses a higher power conversion efficiency(PCE)of 7.81%as the counter electrode(CE)of dye-sensitized solar cells(DSCs)compared with the CEs calcinated at other temperatures and a similar PCE with Pt counterpart(8.24%)based on the liquid I_3^-/I^-*** better electrocatalytic performance is attributed to the synergistic effect between self-activation and the co-doping of nitrogen,sulfur and phosphorus all together in a carbon *** to the feasibility of large-scale production,rich heteroatom doping,the PP-derived carbon,which simplifies the procedure and decreases the cost,has a potential application for an alternative electrocatalyst for high-performance photovoltaic devices.

关键词： Counter electrode Self-activation Biomass-derived carbon Electrocatalytic performance

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Ligand assisted copper-catalyzed Ullmann cross coupling reaction of bromaminic acid with amines

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Chinese Journal of Chemical Engineering 2016年第8期24卷 1000-1006页

作者： Beibei Shao Hongying Du Xinyu Hao Rongwen Lu Yi Luo Shufen Zhang state key laboratory of fine chemicals Dalian University of Technology

Three types of ligands have been developed for copper-catalyzed Ullmann cross coupling reaction of bromaminic acid with amines in aqueous solution. Ligands with large steric hindrance and strong electron-donating capacity were beneficial to the reaction. UV–Vis and CV analyses demonstrated that these ligands had strong coordination with copper(I), implying the effect of ligand coordination ability on the stability and catalytic activity of catalytic system.

关键词： Bromaminic acid Ullmann cross coupling reaction Ligand Copper catalysis

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A mechanical reinforced and antifreezing polyacrylate hydrogel electrolyte for high-performance zinc-ion batteries

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Nano Research 2025年第1期18卷 341-350页

作者： Zili Zhang Ruolin Wang Hongfei Lu Di Zhang Yu Zhao Jing Xu Bin Sun Zhi-Min Dang Yang Jin School of Electrical and Information Engineering Zheng Zhou UniversityZhengzhou 450001China state key Lab of New Ceramics and fine Processing School of Materials Science and EngineeringTsinghua UniversityBeijing 100084China

The operation of aqueous zinc-ion batteries in flexible energy storage field is plagued by the uncontrollable growth of Zn-dendrite and inevitable freeze of water below 0 ℃.Therefore,it is necessary to design a hydrogel electrolyte with good mechanical property and freezing resistance to uniform the Zn-deposition and resist flexibility loss at low *** find that the mechanical property(strength and toughness)of hydrogel electrolyte has a significant impact on the suppression of dendrite growth and the uniform deposition of zinc ***,a polyacrylate hydrogel is prepared in one step by ultraviolet(UV)curing method with Zn(CF_(3)SO_(3))_(2)salt and polyvinyl alcohol(PVA)addition to increase the antifreezing ability and mechanical *** adsorption of water molecules by 2-hydroxyethyl acrylate(HEA)and PVA reduces the freezing point of the hydrogel,which is beneficial for enhancing the electrochemical stability at low *** this basis,the Zn-symmetrical battery with hydrogel electrolyte has a long lifespan of 4710 h at 0.5 mA·cm^(-2)and 0.5 mAh·cm^(-2)at room ***,the hydrogel electrolyte exhibits an outstanding stability at low temperature of^(-2)0 ℃,the lifespan of symmetrical battery reaches to 4000 h at 0.5 mA·cm^(-2)and 0.5 mAh·cm^(-2).The assembled full cell with NaV3O8·1.5H_(2)O(NVO)cathode and hydrogel electrolyte possesses a high capacity retention ratio of 77%after 10,000 cycles at^(-2)0 ℃.The flexible cell can power light-emitting diode(LED)lamp under bending,warping and cutting without liquid leakage and an electronic watch at the operating temperature of^(-2)0 ℃.

关键词： zinc ion battery hydrogel electrolyte mechanical enhancement freezing resistance

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