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Microwave-assisted synthesis of nanoscale Eu(BTC)(H_2O)·DMF with tunable luminescence

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Science China Chemistry 2015年第6期58卷 973-978页

作者： song Dang shuyan song Jing Feng Hongjie Zhang State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied Chemistry Chinese Academy of Sciences

Nanoscale europium（Ⅲ） metal-organic frameworks, Eu（BTC）（H20）.DMF, were synthesized by rapid microwave-assisted method. The components of the as-prepared products were confirmed by the elemental analysis, X-ray powder diffraction （XRD）, thermal gravimetric analysis （TGA） and Fourier-transform infrared spectra （FTIR） analyses. Eu（BTC）（H20）.DMF with various morphologies, including particle-like, rod-like, straw-sheaf-like nanostructures, could be simply prepared by con- trolling the concentrations of the starting reactants. The optical measurements on the obtained Eu（BTC）（H20）- DMF indicated that all the nanomaterials show the characteristic emissions of the Eu3＋ ions at 578, 590, 612, 650, and 699 nm, which were at- tributed to 5Do→7FJ （J=0-4） transitions of the Eu3＋ ion, respectively. It was also noticed that the luminescent properties of the as-prepared products were heavily dependent on the morphologies and sizes of the nanomaterials. The assembled straw-sheaf-like architectures displayed the strongest emissions and the longest luminescence lifetime, which was mainly due to the fewest surface defects.

关键词： metal-organic frameworks nanomateriais europium luminescence microwave-assisted synthesis

Cascade-responsive nanobomb with domino effect for anti-tumor synergistic therapies

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National Science Review 2022年第3期9卷 32-41页

作者： Yang Liu Yinghui Wang shuyan song Hongjie Zhang 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 Department of Chemistry Tsinghua University

The development of reactive oxygen species(ROS) generation agents that can selectively produce sufficient ROS at the tumor site without external energy stimulation is of great significance for the further clinical application of ROS-based therapies. Herein, we designed a cascade-responsive ROS nanobomb(ZnO2@Ce6/CaP@CPPO/BSA, designated as Z@Ce6/Ca P@CB) with domino effect and without external stimulation for the specific generation of multiple powerful ROS storms at the tumor site. The calcium phosphate shell and ZnO2core gradually degrade and release Ca2+, Zn2+and hydrogen peroxide(H2O2) under acid stimulation. On the one hand, Zn2+can enhance the generation of endogenous superoxide anions(·O2~–) and H2O2through the inhibition of the mitochondrial electron transport *** the other hand, the generation of large amounts of exogenous H2O2can cause oxidative damage to tumor cells and further activate bis[2,4,5-trichloro-6-(pentyloxycarbonyl)phenyl] oxalate(CPPO)-mediated chemiexcited photodynamic therapy. In addition, the oxidative stress caused by the generated ROS can lead to the uncontrolled accumulation of Ca2+in cells and further result in Ca2+overload-induced cell death. Therefore, the introduction of Z@Ce6/CaP@CB nanobombs triggered the’domino effect’ that caused multiple heavy ROS storms and Ca2+overload in tumors and effectively activated anti-tumor immune response.

关键词： reactive oxygen species immunotherapy chemiexcited photodynamic therapy ion interference therapy biodegradable

Boosting High-Rate Zinc-Storage Performance by the Rational Design of Mn_(2)O_(3) Nanoporous Architecture Cathode

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Nano-Micro Letters 2020年第1期12卷 195-207页

作者： Danyang Feng Tu‑Nan Gao Ling Zhang Bingkun Guo shuyan song Zhen‑An Qiao Sheng Dai State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012JilinPeople’s Republic of China State Key Laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012JilinPeople’s Republic of China Materials Genome Institute Shanghai UniversityShanghai 200444People’s Republic of China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022People’s Republic of China Chemical Sciences Division Oak Ridge National LaboratoryOak RidgeTN 37831USA

Manganese oxides are regarded as one of the most promising cathode materials in rechargeable aqueous Zn-ion batteries(ZIBs)because of the low price and high ***,the practical application of Mn2O3 in ZIBs is still plagued by the low specific capacity and poor rate ***,highly crystalline Mn2O3 materials with interconnected mesostructures and controllable pore sizes are obtained via a ligand-assisted self-assembly process and used as high-performance electrode materials for reversible aqueous *** coordination degree between Mn2+and citric acid ligand plays a crucial role in the formation of the mesostructure,and the pore sizes can be easily tuned from 3.2 to 7.3 *** to the unique feature of nanoporous architectures,excellent zinc-storage performance can be achieved in ZIBs during charge/discharge *** Mn2O3 electrode exhibits high reversible capacity(233 mAh g−1 at 0.3 A g−1),superior rate capability(162 mAh g−1 retains at 3.08 A g−1)and remarkable cycling durability over 3000 cycles at a high current rate of 3.08 A g−***,the corresponding electrode reaction mechanism is studied in depth according to a series of analytical *** results suggest that rational design of the nanoporous architecture for electrode materials can effectively improve the battery performance.

关键词： Porous Mn_(2)O_(3) High-rate capability Zn-ion battery Cathode material Zn-storage 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

ZnCo_(2)O_(4) supported low-loading Pd as an enhanced catalyst for low temperature oxidation of carbon monoxide

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Chinese Journal of Structural Chemistry 2023年第7期42卷 23-27页

作者： Xi Liang Lingling Zhang Xiao Wang shuyan song Hongjie Zhang State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022PR China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei230026PR China Department of Chemistry Tsinghua UniversityBeijing100084PR China

We have successfully synthesized a series of Pd/ZnCo_(2)O_(4)supported catalytic materials with low noble metal loading and high activity by the impregnation *** Pd/ZnCo_(2)O_(4)catalysts containing 0.2%Pd have superior performance for oxidizing CO at 80℃,achieving 100%*** is also no loss of activity after four cycles of tests,with the conversion remaining approximately 100%.Aside from that,various advanced physicochemical characterizations indicate that this excellent catalytic performance stems from the interaction between metal Pd and carrier ZnCo_(2)O_(4).Pd provides a higher degree of accessibility to the active site,while ZnCo_(2)O_(4)as a carrier can better stabilize Pd *** 0.2%Pd/ZnCo_(2)O_(4)exhibits higher levels of Pd^(2+)species as the electronic interaction between Pd and ZnCo_(2)O_(4)improves,thus improving CO oxidation catalytic ***,the low loading of Pd is crucial for reducing the cost of noble metal catalysts and ameliorating their practicality in industrial applications.

关键词： Palladium Composite materials Cooperative effect CO oxidation

In situ Synthesis of Ultrasmall Au Clusters on Thiol-modified CeO_(2) with Enhanced Stability and CO Oxidation Activity

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Chemical Research in Chinese Universities 2023年第6期39卷 921-927页

作者： LI Lingling XU Jinhui LIANG Xi WU Xueting WANG Xiao song shuyan ZHANG Hongjie State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022P.R.China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026P.R.China Department of Chemistry Tsinghua UniversityBeijing 100084P.R.

Gold(Au)nanoclusters supported on various supports have been widely used in the fields of energy and ***,the poor thermal stability of Au nanoclusters on the support interface usually leads to a reduction or even loss of catalytic ***,we used an in situ reduction method to synthesize Au nanoclusters on ceria(CeO_(2))*** this method,sulfhydryl groups were used to modify CeO_(2) nanospheres first,and then Au clusters with an average diameter of 1.5 nm were grown on the surface of ceria reduced with sodium *** presence of the Au-S-Ce structure enhances the electron transfer efficiency,making the material exhibit high CO oxidation activity at room ***,due to the strong binding energy of S and Au,the material exhibits a high stability for long time running *** strategy provides an idea for designing stable and active supported ultrasmall Au nanoclusters catalytic materials.

关键词： Au cluster Sulfhydryl Oxygen activation In situ synthesis

Engineering CeO_(2)/CuO heterostructure anchored on upconversion nanoparticles with boosting ROS generation-primed apoptosisferroptosis for cancer dynamic therapy

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Nano Research 2023年第4期16卷 5322-5334页

作者： Xuan Gao Jing Feng Kehong Lv Yifei Zhou Ruohao Zhang shuyan song Hongjie Zhang Daguang Wang 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 Gastric and Intestinal Department General Surgery CenterFirst Hospital of Jilin UniversityChangchun 130021China

Highly toxic reactive oxygen species(ROS)induced apoptosis and ferroptosis have been considered as significant cell death pathways for cancer ***,insufficient amount of intracellular ROS extremely restricts the therapeutic *** this,we report a rationally designed nanocomposite(mUCC)with enhanced ROS generation ability,inducing the combination of apoptosis and ferroptosis through synergistic photodynamic therapy(PDT)and chemodynamic therapy(CDT).Under 808 nm near-infrared(NIR)light irradiation,photocatalytic reaction is triggered starting from the separation of electron-hole pairs on the surface of heterojunction(CeO_(2)/CuO),realizing improved ROS ***,mUCC served as Fenton-like agent exhibits considerable ability to generate highly toxic·OH under tumor microenvironment(TME).The boosted accumulation of ROS disrupts the redox balance within tumor cells and results in the integration of apoptosis and *** addition,mUCC shows satisfactory tumor targeting property benefiting from the cancer cell membrane functionalization under the guidance of magnetic resonance imaging(MRI)and NIR fluorescence *** intelligent mUCC with good biocompatibility and excellent antitumor response achieves efficient tumor elimination under synergistic PDT and *** work offers an elective approach for further development of ROS-based therapeutic nanoplatform in cancer therapy.

关键词： upconversion nanoparticles heterojunction reactive oxygen species apoptosis-ferroptosis synergistic dynamic therapy

Metal-Organic Frameworks-derived Indium Clusters/Carbon Nanocomposites for Efficient CO_(2) Electroreduction

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Chemical Research in Chinese Universities 2022年第5期38卷 1287-1291页

作者： GONG Yu PAN Jing ZHANG Lingling WANG Xiao song shuyan ZHANG Hongjie State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022P.R.China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026P.R.China Department of Chemistry Tsinghua UniversityBeijing 100084P.R.China

Electrochemical reduction of carbon dioxide into value-added products is a promising way to recycle the greenhouse gas,thus solving the crisis of global *** challenges remain in regulating the catalytic *** this work,we demonstrated a metal-organic frameworks-assisted approach to synthesizing In species loaded on the surface of N doped carbon *** controlling the particle sizes,the catalytic selectivity can be easily *** obtained Inc/NC possesses the outstanding capability for converting CO_(2)into *** 80.09%Faraday efficiency(FE)of CO can be achieved at 0.8 V *** the In_(2)O_(3)/C exhibits different catalytic behaviors,the main product is formic acid and the FE is more than 50%at 0.8 V *** selectivity reversal can be attributed to the strong interactions between In clusters and N atoms of carbon supports,which efficiently inhibits the formation of the by-product,formic *** research has paved a new way to modulate catalytic selectivity by manipulating the fine structures of the catalysts.

关键词： Indium cluster Indium oxide Electrochemical reduction CO_(2)electroreduction

Construction of trace silver modified core@shell structured Pt-Ni nanoframe@CeO2 for semihydrogenation of phenylacetylene

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Nano Research 2019年第4期12卷 869-875页

作者： Yan Long Jian Li Lanlan Wu Qishun Wang Yu Liu Xiao Wang shuyan song Hongjie Zhang State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied Chemistry Chinese Academy of Sciences Changchun 130022 China University of Chinese Academy of Sciences Beijing 100049 China University of Science and Technology of China Hefei 230026 China

The Pt-Ni nanoframe catalysts have attracted great interest owing to their unique electronic structure and excellent catalytic performance. However, the stability of the tenu ous edges of nano frame-structures is dissatisfactory and their un iversal applicati ons in catalytic market beyond electrocatalytic reactions are yet to be tapped and explored. Herein, we developed a new core@ shell structured Pt-Ni nanoframe@CeO2 (Pt-Ni NF@CeO2) composite via etching the Ni from inhomogeneous Pt-Ni rhombic dodecahedra (Pt-Ni RD) by cerium(lll) acetate hydrate (Ce(OAc)3). In this path, Pt-Ni RD was used as self-sacrificial 怕mplate, while the Ce(OAc)3 serves as the provider of the Ce3* source and OH' for the formation of CeO2 shell, etchant of Pt-Ni RD, and the surface modification agent. By this way, the etching of Pt-Ni RD and the formation of the CeO2 shell are simultaneously proceeded to form the final Pt-Ni NF@CeO2 in one step. The obtained Pt-Ni NF@CeO2 exhibits strong in terfacial charge tran sfer interactio n betwee n Pt-Ni NF core and CeO2 shell eve n without reductio n treatment, leading to enhan ced catalytic activity in the hydrogenation of phenylacetylene. After introduction of trace silver, the Pt-Ni-Ag4.9 NF@CeO2 achieves remarkable catalytic performa nee for the selective con versi on of phe ny lacetyle ne to styrene: high con version (100%), styre ne selectivity (86.5%), and good stability. It reveals that enc apsulatio n n oble metal nano frames into metal oxide to form core @ shell structured hybrids will in deed enhance their stability and catalytic properties. Particularly, this work expends the application of noble metal nanoframes materials to hydrogenation reacti ons.

关键词： CeO2 Pt-Ni nanoframes core@shell sturcuture silver modification hydrogenation of phenylacetylene