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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

Engineered spidroin-derived high-performance fibers for diverse applications

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Nano Research 2024年第2期17卷 492-502页

作者： Dawen Qin Jingjing Li Huanrong Li hongjie zhang Kai Liu National-Local Joint Engineering Laboratory for Energy Conservation in Chemical Process Integration and Resources Utilization Tianjin Key Laboratory of Chemical Process SafetySchool of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300130China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Engineering Research Center of Advanced Rare Earth Materials Ministry of EducationDepartment of ChemistryTsinghua UniversityBeijing 100084China University of Science and Technology of China Hefei 230026China

Spider silks are well known for their exceptional mechanical properties that are tougher than Kevlar and ***,the restricted production amounts from their native sources limit applications of spider *** the decades,there have been significant interests in fabricating man-made silk fibers with comparable performance to natural silks,inspiring many efforts both for biosynthesizing recombinant spider silk proteins(spidroins)in amenable heterologous hosts and biomimetic spinning of artificial spider *** strategies provide promising routes to produce high-performance and functionally optimized fibers with diverse ***,we summarize the hosts that have been applied to produce recombinant *** addition,the fabrication and mechanical properties of recombinant spidroin fibers and their composite fibers are also ***,we demonstrate the applications of recombinant spidroin-based ***,facing the challenges in biosynthesis,scalable production,and hierarchical assembly of high-performance recombinant spidroins,we give a summary and perspective on future development.

关键词： spider silk recombinant spidroin heterologous expression fiber fabrication mechanical property

All-inorganic nitrate electrolyte for high-performance lithium oxygen battery

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Nano Research 2024年第5期17卷 4163-4170页

作者： Dongyue Yang Jiayi Du Kai Chen Haoran zhang Gang Huang Tong Liu Xinbo zhang 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

Lithium-oxygen(Li-O_(2))batteries have been regarded as an expectant successor for next-generation energy storage systems owing to their ultra-high theoretical energy ***,the comprehensive properties of the commonly utilized organic salt electrolyte are still unsatisfactory,not to mention their expensive prices,which seriously hinders the practical production and application of Li-O_(2) ***,we have proposed a low-cost all-inorganic nitrate electrolyte(LiNO_(3)-KNO_(3)-DMSO)for Li-O_(2) *** inorganic nitrate electrolyte exhibits higher ionic conductivity and a wider electrochemical stability window than the organic salt *** existence of K+can stabilize the O_(2)-intermediate,promoting the discharge process through the solution pathway with an enlarged *** at an ultra-low concentration of 0.01 M,the K+can still remain stable to promote the solution discharge process and also possess a new function of inhibiting the dendrite growth by electrostatic shielding,further enhancing the battery stability and contributing to the long cycle *** a result,in the 0.99 M LiNO_(3)-0.01 M KNO_(3)-DMSO electrolyte,the Li-O_(2) batteries exhibit prolonged cycling performance(108 cycles)and excellent rate performance(2 A·g^(-1)),significantly superior to the organic salt one.

关键词： Li-O_(2)batteries potassium ions inorganic nitrate electrolyte solution pathway mechanism

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

S1-supported Pd@CeO_(2) quasi-core@shell materials as advanced catalysts for selective hydrogenation of furfural

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Chinese Chemical Letters 2024年第3期35卷 493-496页

作者： Xiang Chu Lingling zhang Ke Wang Rui 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

Bare Pd metal nanoparticles invariably suffer from poor selectivity in furfural hydrogenation by forming flat configurations,with the aromatic ring of the substrate molecules parallel to the metal ***,we put forward a promising solution by using CeO_(2)as promoters to modify Pd nanoparticles for modulating the adsorption behaviors of furfural *** achieve the highly-desired ultra-small Pd@CeO_(2)core@shell nanostructure,a“constrained auto-redox”synthesis is developed,in which silicalite-1 supports play the key role of providing their surface as the landing place of PdO_(x)precursors for inhibiting the overgrowth and the *** the best of our knowledge,this is one of the smallest core@shell materials obtained from aqueous *** evaluated as catalysts,Pd@CeO_(2)/S-1 gives 98.9%conversion of furfural with 94.3%selectivity for furfural alcohol in 15 h,which is much better than that of Pd/S-1(88.6%conversion with 44.3%selectively).The DFT simulation reveals a strong interaction between the defects of CeO_(2)and the oxygen atom of the–CHO group in furfural molecules,which benefits the selective hydrogenation occurred in the–CHO group rather than the furan ring.

关键词： Core@shell Palladium Ceria Auto-redox synthesis Hydrogenation

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

High-efficiency PdNi single-atom alloy catalyst toward cross-coupling reaction

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Chinese Chemical Letters 2024年第7期35卷 480-483页

作者： Baokang Geng Xiang Chu Li Liu Lingling zhang Shuaishuai 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

The preparation of Pd-based catalysts with rich electrons and a high atom dispersion rate is of great significance for improving the reactivity of cross-coupling reactions,which is a powerful tool for pharmaceutical and fine chemical ***,we report a PdNi single-atom alloy(SAA)catalyst in which isolated Pd single atoms are anchored onto the surface of Ni nanoparticles(NPs)applied for Suzuki coupling reactions and Heck coupling *** 0.1%PdNi SAA exhibits extraordinary catalytic activity(reaction rate:17,032.25 mmol h^(-1)gPd^(-1))toward the Suzuki cross-coupling reaction between 4-bromoanisole and phenylboronic acid at 80℃for 1 *** excellent activity is supposed to attribute to the 100 percent utilization rate of Pd atoms and the highly stable surface zero-valance Pd atoms,which provides abundant sites and electrons for the adsorption and fracture of the C-X(X=Cl,Br,I)***,our work demonstrates the excellent application prospect of SAAs for cross-coupling reactions.

关键词： Single-atom alloy Cross-coupling reaction Palladium catalysis Heterogeneous catalysis High-efficiency

Large-Scale and Reversible Synthesis of Bright Upconversion Crystals with Almost 100%Yield by a Minimalist Method for Recyclable Application

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CCS Chemistry 2024年第6期6卷 1512-1522页

作者： Pengpeng Lei Yuan Liang Pengye Du Yong zhang hongjie zhang State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022 University of Science and Technology of China Hefei 230026 Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341000 Department of Biomedical Engineering Faculty of EngineeringNational University of SingaporeSingapore 117583 Department of Chemistry Tsinghua UniversityBeijing 100084

Upconversion luminescence(UCL)materials have the potential for many applications due to their unique optical *** technical challenges such as complex synthesis with low yield and nondegradability need to be addressed for practical ***,we report for the first time a minimalist method for large-scale synthesis of Cs_(2)NaErCl_(6)UCL crystals with almost 100%yield,simply by dissolving metal chlorides in water and then drying,referred to as the“dissolve-dry”***_(2)NaErCl_(6)crystals produced under such mild conditions exhibited bright UCL at either 808 or 980 nm *** was achieved through an excited state absorption process,and the excellent performance was mainly attributed to the large unit cells of the crystals and the long lifetime of Er^(3+)excited energy ***,the synthesis was reversible and could be scaled up unlimitedly,making it suitable for industrial applications,with recyclable *** recyclable application of Cs_(2)NaErCl_(6)crystals as a luminescent medium in near-infrared light-emitting diode excitable upconversion devices was demonstrated based on its excellent *** work not only provides a new strategy for large-scale synthesis of UCL crystals but also demonstrates the recyclability of this material and its related applications.

关键词： rare earth upconversion reversible synthesis minimalist method application

Utilizing dual-pathway energy transfer in upconversion nanoconjugates for reinforced photodynamic therapy

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Nano Research 2024年第4期17卷 2941-2948页

作者： Ruohao zhang Yu Lu Yifei Zhou Kehong Lv Xinyu Fu Jitong Gong Shuang Yao Xiaozhen Wang Jing Feng 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 College of Chemistry Jilin UniversityChangchun 130012China Department of Breast Surgery General Surgery Centerthe First Hospital of Jilin UniversityChangchun 130021China Department of Chemistry Tsinghua UniversityBeijing 100084China

Enhancing the therapeutic effect of existing treatments or developing new non-invasive treatments are important measures to achieve high-efficiency treatment of malignant *** therapy(PDT)is an emerging treatment modality,and the key for achieving high-efficiency PDT is to select light with strong tissue penetration depth and enhance the generation of reactive oxygen species(ROS).Although the upconversion nanoparticles(UCNPs)modified with the photosensitizers could achieve PDT with strong penetration depth under near-infrared light irradiation,the ROS generated by traditional single-pathway PDT is still ***,we developed a novel nanoconjugate(UCNP-Ce6/AIEgen)for dual-pathway reinforced PDT,in which the UCNPs were co-modified with chlorin e6(Ce6)and luminogen with aggregation-induced emission(AIEgen).Due to the presence of AIEgen,UCNP-Ce6/AIEgen could avoid aggregation-caused luminescence quenching in biological water environments and convert upconversion luminescence(UCL)of UCNPs to Ce6-activatable ***,under the irradiation of 808 nm laser,UCNP-Ce6/AIEgen can not only undergo direct lanthanide-triplet energy transfer to activate Ce6,but also convert the UCL of UCNPs to the light that can activate Ce6 through Fӧrster resonance energy transfer to generate more ROS,thus promoting tumor cell *** work broadens the applications of nanoconjugates of lanthanide-based inorganic materials and organic dyes,and provides a conception for reinforced PDT of tumors.

关键词： upconversion nanoparticle aggregation-induced emission direct lanthanide-triplet energy transfer Förster resonance energy transfer photodynamic therapy