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Conductive Two-Dimensional Supramolecular Polymers via Cation-πdriven Self-Aligned Aromatic Brick-Like Stacking

CCS Chemistry 2025年第3期7卷 807-818页

作者： Bin Mu Zhongke Yang Zechen Liang Renjie Xue Laju Bu Haiming Zhang Lifeng Chi Hongxia Yan Wei Tian Shanxi Key Laboratory of Macromolecular Science and Technology Xi’an Key Laboratory of Hybrid Luminescent Materials and Photonic DeviceMOE Key Laboratory of Material Physics and Chemistry under Extraordinary ConditionsSchool of Chemistry and Chemical EngineeringNorthwestern Polytechnical UniversityXi’an 710072 School of Chemistry Engineering Research Center of Energy Storage Materials and DevicesMinistry of EducationXi’an Key Laboratory of Sustainable Energy Material ChemistryXi’an Jiaotong UniversityXi’an 710049 Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices Institute of Functional Nano and Soft Materials(FUNSOM)Soochow UniversitySuzhou 215123

Achieving molecular self-assembly to produce functional supramolecular polymers with defined dimensions and structural periodicity is crucial,particularly for two-dimensional supramolecular polymers(2DSPs).However,a major challenge to their application has been poor electrical conductivity due to weakπ-electron delocalization in existing synthetic ***,we overcome this limitation by demonstrating the controlled construction of conductive 2DSPs through self-aligned brick-like stacking of doubly chargedπ-conjugated monomers driven by aromatic cation-πinteractions.A key feature of this approach is the upright molecular orientation,a notable departure from the horizontal orientation typical of conventional 2D *** versatile method is compatible with various molecular building blocks,enabling modulation of 2DSP conformation from flat to *** have also prepared free-standing single-layer nanosheets of 2DSPs via solution-assisted exfoliation from their *** resulting 2DSPs demonstrate efficient in-planeπ-electron delocalization,leading to impressive electrical conductivity properties,holding significant promise for optoelectronic applications.

关键词： self-assembly two-dimensional supramolecular polymers cation-πinteractions singlelayer nanosheets electrical conductivity

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Zincophilic and hydrophobic bifunctional PFA-COOH-CNT artificial SEI film for highly stable Zn anode

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Nano Research 2025年第2期18卷 346-357页

作者： Lingyao Kuang Bohui Xu Long Zhang Zheshuai Lin Xingxing Gu Xiaolei Ren Yanglong Hou Chongqing Key Laboratory of Catalysis and New Environmental Materials College of Environment and ResourcesChongqing 400067China Functional Crystals Lab Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China School of Materials Shenzhen Campus of Sun Yat-Sen UniversityShenzhen 518107China Beijing Key Laboratory for Magnetoelectric Materials and Devices(BKL-MMD) School of Materials Science and EngineeringPeking UniversityBeijing 100871China

Aqueous zinc-ion batteries(AZIBs)are regarded as one of the most promising rivals in the upcoming high-energy secondary battery market because of their safety and ***,the zinc dendrites growth and hydrogen evolution corrosion of the Zn anode have seriously restricted the application of ***,to overcome these constraints,a three-dimensional(3D)porous PFA-COOH-CNT artificial solid electrolyte interface(SEl)film with high hydrophobic and zincophilic properties was constructed on Zn anode surface by in-situ polymerization of furfuryl alcohol(FA)and carboxyl carbon nanotubes(COOH-CNT).A series of in-situ,ex-situ characterizations as well as the density functional theory(DFT)calculations reveal that the formed PFA-COOH-CNT SEI film with an abundant oxygen-containing group can provide abundant zincophilic sites and induce homogeneous deposition of Zn^(2+),as well as the hydrophobic alkyl and carbon skeleton in PFA-COOH-CNT SEI film can isolate the direct contact of H_(2)O with Zn anode,and inhibit the occurrence of hydrogen evolution reaction(HER).Accordingly,the Zn anode with PFA-COOH-CNT layer can attain an ultra-long cycle life of 2200 h at 1 mA·cm^(-2),1 mAh·cm^(-2).Simultaneously,the assembled PFA-COOH-CNT@ZnllV2Os full cell can also achieve a high reversible capacity of up to 150.2 mAh•g^(-1) at 1 A·g^(-1) after 400 cycles,with a high average coulombic efficiency(CE)of 98.8%.The designed PFA-COOH-CNT artificial SEI film provides a broad prospect for highly stable zinc anode,and can also be extended to other energy storage systems based on metal anodes.

关键词： Zn anode PFA-COOH-CNT solid electrolyte interface(SEI)film zincophilic hydrophobic

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An electrically activable nanochip to intensify gas-ionic-immunotherapy

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Science Bulletin 2025年第3期70卷 390-406页

作者： Gang Wang Jingrui Li Shumin Sun Yuqi Yang Zhihui Han Zifan Pei Liang Cheng Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China

Excess intracellular H_(2)S induces destructive mitochondrial toxicity,while overload of Zn^(2+)results in cell pyroptosis and potentiates the tumor immunogenicity for ***,the precise delivery of both therapeutics remains a great ***,an electrically activable ZnS nanochip for the controlled release of H_(2)S and Zn^(2+)was developed for enhanced gas-ionic-immunotherapy(GIIT).Under an electric field,a locality with particularly high concentrations of H_(2)S and Zn^(2+)was established by the voltage-controlled degradation of the ZnS nanoparticles(NPs).Consequently,the ZnS nanochip-mediated gas-ionic therapy(GIT)resulted in mitochondrial membrane potential depolarization,energy generation inhibition,and oxidative stress imbalance in tumor ***,the cyclic guanosine monophosphate-adenosine monophosphate synthase-stimulator of interferon genes(cGAS-STING)signaling pathway was activated due to the mitochondrial ***,the released Zn^(2+)resulted in the increase of the intracellular Zn levels and cell pyroptosis,which enhanced the immunogenicity via the release of damage-associated molecular patterns(DAMPs).In vitro and in vivo studies revealed that the ZnS nanochip-based GIT effectively eliminated the tumors under an electric field and mobilized the cytotoxic T lymphocytes for *** combination withαCTLA-4 further promoted the adaptive immune response and inhibited tumor metastasis and long-term tumor *** work presented an electrically activable ZnS nanochip for combined immunotherapy,which might inspire the development of electric stimulation therapy.

关键词： H_(2)S gas therapy lonic interference therapy Electrically controll eddelivery Cell pyroptosis CGAS-STING pathway

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Efficient hydrogen peroxide production enabled by exploring layered metal telluride as two electron oxygen reduction reaction electrocatalyst

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Journal of Energy Chemistry 2023年第12期87卷 247-255,I0007页

作者： Yingming Wang Hongyuan Yang Zhiwei Liu Kui Yin Zhaowu Wang Hui Huang Yang Liu Zhenhui Kang Ziliang Chen Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-based Functional Materials and DevicesJoint International Research Laboratory of Carbon-Based Functional Materials and DevicesSoochow UniversitySuzhou 215123JiangsuChina School of Physics and Engineering Longmen Laboratory Henan University of Science and TechnologyLuoyang 471023HenanChina Macao Institute of Materials Science and Engineering(MIMSE) MUST-SUDA Joint Research Center for Advanced Functional MaterialsMacao University of Science and TechnologyTaipa 999078MacaoChina Suzhou Weimu Intelligent System Co. Ltd.Suzhou 215123JiangsuChina

It is of great interest to develop the novel transition metal-based electrocatalysts with high selectivity and activity for two electron oxygen reduction reaction(2e^(-) ORR).Herein,the nickel ditelluride(NiTe_(2)) with layered structure was explored as the 2e^(-) ORR electrocatalyst,which not only showed the highest 2e^(-) selectivity more than 97%,but also delivered a slight activity decay after 5000 cycles in alkaline ***,when NiTe_(2) was assembled as the electrocatalyst in H-type electrolyzer,the on-site yield of H_(2)O_(2) could reach up to 672 mmol h^(-1)g^(-1) under 0.45 V *** in situ Raman spectra,theoretical calculation and post microstructural analysis synergistically unveiled that such a good 2e^(-) ORR performance could be credited to the intrinsic layered crystal structure,the high compositional stability,as well as the electron modulation on the active site Ni atoms by neighboring Te atoms,leading to the exposure of active sites as well as the optimized adsorption free energy of Ni to –*** inspiringly,such telluride electrocatalyst has also been demonstrated to exhibit high activity and selectivity towards 2e^(-) ORR in neutral media.

关键词： Transition metal telluride Oxygen reduction reaction Charge polarization Activity and selectivity Hydrogen peroxide

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Artificial intelligence for the understanding of electrolyte chemistry and electrode interface in lithium battery

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National Science Open 2024年第2期3卷 74-97页

作者： Yawei Chen Yue Liu Zixu He Liang Xu Peiping Yu Qintao Sun Wanxia Li Yulin Jie Ruiguo Cao Tao Cheng Shuhong Jiao Hefei National Laboratory for Physical Science at Microscale CAS Key Laboratory of Materials for Energy ConversionDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesJoint International Research Laboratory of Carbon-Based Functional Materials and DevicesSoochow UniversitySuzhou 215123China Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow UniversitySuzhou 215123China

Recognizing the critical role of electrolyte chemistry and electrode interfaces in the performance and safety of lithium batteries,along with the urgent need for more sophisticated methods of analysis,this comprehensive review underscores the promise of machine learning(ML)models in this research *** explores the application of these innovative methods to studying battery interfaces,particularly focusing on lithium metal *** the limitations of traditional experimental techniques,the review supports a hybrid approach that couples experimental and simulation methods,enabling granular insights into the formation process and characteristics of battery interfaces at the molecular level and harnessing AI to extract patterns from voluminous data *** showcases the utility of such techniques in electrolyte design and battery life prediction and introduces a novel perspective on battery interface *** review concludes by asserting the potential of artificial intelligence(AI)or ML models as invaluable tools in the future of battery research and highlights the importance of fostering confidence in these technologies within the scientific community.

关键词： lithium batteries battery interfaces artificial intelligence machine learning electrolyte chemistry

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The practically renewable and highly efficient electrocatalysts derived from a newly-designed Mo_(8)Pt polyoxometalate compound

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Science China Chemistry 2023年第2期66卷 492-499页

作者： Di Yin Yun-Dong Cao Yi Feng Guang-Gang Gao Hong Liu Lin-Lin Fan Zhen-Hui Kang School of Materials Science and Engineering University of JinanJinan250022China Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-based Functional Materials and DevicesSoochow UniversitySuzhou215123China Macao Institute of Materials Science and Engineering(MIMSE) MUST-SUDA Joint Research Center for Advanced Functional MaterialsMacao University of Science and TechnologyTaipaMacao999078China

Platinum(Pt)catalysts are the most practical electrocatalysts;however,their low abundance and high cost severely limit their large-scale *** recovery is a key issue to be resolved before the use of Pt-based electrocatalysts can be broadly ***,the newly designed polyoxometalate[Pt^(II)(NH_(3))_(4)]_(2)[Mo_(8)O26](Mo_(8)Pt)acts as an ideal recycling medium for renewable and highly effective Pt *** from Mo_(8)Pt,by a facile reduction reaction,the formed Pt/Mo_(2)C/Mo_(2)N@C-N electrocatalyst shows superior electrocatalytic activity as compared to commercial Pt/C(20%)under both acidic and alkaline ***,the reaction of Pt/Mo_(2)C/Mo_(2)N@C-N in H_(2)O_(2)solution can regenerate Mo_(8)Pt for Pt *** is also demonstrated that the Pt electrocatalyst can be used for at least five rounds of recycling and regeneration,showing its efficiency and stability as well as its *** work highlights a recycling medium strategy to the new generation of renewable Pt-based catalysts.

关键词： platinum polyoxometalate electrocatalyst recycling-medium renewability

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A Selective Cation Replacement Strategy for the Growth of 2D Magnetic Cr2Te3 Nanosheets by CVD

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ACS Applied Electronic materials 2025年第11期7卷 4776-4782页

作者： Suonan, Zhaxi Xu, Hua Wu, Hanxiang Chen, Shanshan Cheng, Zhihai Pang, Fei Beijing Key Laboratory of Optoelectronic Functional Materials & Micro-nano Devices School of Physics Renmin University of China Beijing100872 China Key Laboratory of Quantum State Construction and Manipulation Ministry of Education Renmin University of China Beijing100872 China

Cr2Te3 has recently emerged as a new class of two-dimensional (2D) materials due to its inherent long-range ferromagnetic order. Here, we report the synthesis of 2D Cr2Te3 nanosheets from a GeTe precursor by a cation replacement reaction. During the reaction, Cr ions preferentially bind to Te ions and replace Ge along the c-axis of the lattice. When Cr-Te bonds are formed, the binding energy is reduced due to the lower electronegativity of Cr. After the Ge atoms are substituted by Cr atoms, we successfully synthesized Cr2Te3 instead of CrGeTe3. Cr2Te3 nanosheets show a triangular structure with a lateral size of up to 10 μm and a thickness of about 2.2 nm. The structure of Cr 2Te3 nanosheets was confirmed by XRD, Raman spectroscopy, and HRTEM. Cr2Te3 nanosheets exhibit robust magnetic behavior with a Curie temperature (TC) of about 161 K. This cation replacement strategy promotes the development of Cr2Te3 and paves an effective way to fabricate 2D magnetic materials. © 2025 American Chemical Society.

关键词： Nanosheets

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High-temperature superconductivity in Li2AuH6 mediated by strong electron-phonon coupling under ambient pressure

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Physical Review B 2025年第14期111卷 L140501-L140501页

作者： Zhenfeng Ouyang Bo-Wen Yao Xiao-Qi Han Peng-Jie Guo Ze-Feng Gao Zhong-Yi Lu School of Physics and Beijing Key Laboratory of Opto-electronic Functional Materials & Micro-nano Devices Renmin University of China Beijing 100872 China Key Laboratory of Quantum State Construction and Manipulation (Ministry of Education) Renmin University of China Beijing 100872 China Hefei National Laboratory Hefei 230088 China

We use our developed AI search engine (InvDesFlow) to perform extensive investigations regarding ambient stable superconducting hydrides. A cubic structure Li2AuH6 with Au-H octahedral motifs is identified to be a candidate. After performing thermodynamical analysis, we provide a feasible route to experimentally synthesize this material via the known LiAu and LiH compounds under ambient pressure. The further first-principles calculations suggest that Li2AuH6 shows a high superconducting transition temperature (Tc) ∼ 140 K under ambient pressure. The H-1s electrons strongly couple with phonon modes of vibrations of Au-H octahedrons as well as vibrations of Li atoms, where the latter is not taken seriously in other previously similar cases. Hence, different from previous claims of searching metallic covalent bonds to find high-Tc superconductors, we emphasize here the importance of those phonon modes with strong electron-phonon coupling (EPC). And we suggest that one can intercalate atoms into binary or ternary hydrides to introduce more potential phonon modes with strong EPC, which is an effective approach to find high-Tc superconductors within multicomponent compounds.

关键词： High temperature superconductors

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Effects of phosphorus doping on the physical properties of axion insulator candidate EuIn_(2)As_(2)

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Chinese Physics B 2022年第5期31卷 641-646页

作者： Feihao Pan Congkuan Tian Jiale Huang Daye Xu Jinchen Wang Peng Cheng Juanjuan Liu Hongxia Zhang Laboratory for Neutron Scattering and Beijing Key Laboratory of Optoelectronic Functional Materials and MicroNano Devices Department of PhysicsRenmin University of ChinaBeijing 100872China

We report an investigation on the single crystal growth,magnetic and transport properties of Eu In_(2)(As_(1-x)P_(x))_(2(0≤x≤1).The physical properties of axion insulator candidate Eu In;As;can be effectively tuned by *** increasing x,the c-axis lattice parameter decreases linearly,the magnetic transition temperature gradually increases and ferromagnetic interactions are *** is similar to the previously reported high pressure effect on Eu In_(2)As_(2).For x=0.40,a spin glass state at T_(g)=10 K emerges together with the observations of a butter-fly shaped magnetic hysteresis and slow magnetic ***,magnetic transition has great influence on the charge carriers in this system and negative colossal magnetoresistance is observed for all P-doped *** findings suggest that Eu In_(2)(As_(1-x)P_(x))_(2) is a promising material playground for exploring novel topological states.

关键词： axion topological insulator

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Single-atom Ti doping on S-vacancy two-dimensional CrS_(2) as a catalyst for ammonia synthesis: A DFT study

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Chinese Chemical Letters 2025年第4期36卷 522-529页

作者： Yiwen Xu Chaozheng He Chenxu Zhao Ling Fu Institute of Environment and Energy Catalysis Shanxi Key Laboratory of Optoelectronic Functional Materials and DevicesSchool of Materials Science and Chemical EngineeringXi'an Technological UniversityXi'an 710021China College of Resources and Environmental Engineering Tianshui Normal UniversityTianshui 741001China

Electrocatalytic reduction of NO(NORR) is an effective method for NH_(3) synthesis, due to low bonding energy of N–O bond. In this work, we have investigated many CrS_(2)based catalysts, including pristine CrS_(2),CrS_(2)with one S vacancy(v-CrS_(2)), and Ti doped CrS_(2)(Ti@CrS_(2)). The results have shown that the pristine CrS_(2)exhibits inert character for NO activation. However, v-CrS_(2)and Ti@CrS_(2)can exhibit enhanced interaction with NO, due to increased charge transfer between NO and substrates(0.52–0.75 e) and enhanced adsorption energies of NO on the catalysts(-0.96~-1.64 e V), compared to the situation of CrS_(2)(0.065 e/-0.30 e V). From the free energy profiles of NO electro-reduction to NH3, we can see that the v-CrS_(2)and Ti@CrS_(2)all exhibit ultralow limiting potentials of-0.03~-0.47 V, following both*NOH and*NHO mechanisms. Therefore, introducing vacancy and doping are all promising modification strategies for NORR catalysts. The results have provided a new idea for the search of catalysts for efficient electrocatalytic reduction of NO.

关键词： CrS_(2) NO electrocatalytic reduction First principles calculation Introducing vacancy doping

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