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Construction of highly dispersed Pt single sites and high-efficiencyheterocatalysis silylation of alcohols with silanes

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Nano Research 2023年第4期16卷 4643-4649页

作者： Qiulian Wei Yunqiang Sun Shan Wang Zunfu Hu Qingyun Liu Xiuwen Zheng School of Chemical and Biological Engineering Shandong University of Science and TechnologyQingdao 266510China Key Laboratory of Functional Nanomaterials and Technology in Universities of Shandong College of Chemistry and Chemical EngineeringLinyi UniversityLinyi 276000China

The construction of silicon-oxygen bonds has been highlighted as an exciting achievement in organosilicon and green chemistry,but their synthetic efficiency has great improvement potential,so it is crucial to explore and achieve an effective approach for synthesizing such compounds.In this study,we successfully prepared the highly dispersed platinum single-atom catalyst(Pt SAC/N-C)through a coordination-assisted strategy with a mixture of ligands(H2bpdc and H2bpydc),which were used for the Osilylation of alcohols with silanes.The strong coordination between Pt2+and the Pyridine N at the skeleton of UiO-67 plays a critical role in accessing the atomically isolated dispersion of Pt sites.Without the assistance of the H2bpydc ligands,the Pt/UiO-67-bpdc precursor is prone to aggregation during the pyrolysis process,resulting in the formation of Pt nanoparticles.Aided by advanced characterization techniques of high-angle annular dark-field scanning transmission electron microscopy(HAADFSTEM)and X-ray absorption fine structure(XAFS)spectroscopy,it has been demonstrated that atomically dispersed Pt was formed on the UiO-67 through a local structure of four-coordinated Pt-N4,exhibiting a high actual Pt loading content(0.6962 wt.%).In the oxidation of silanes,the Pt SAC/N-C catalyst showed a high turnover frequency(TOF)value(up to 9,920 h−1)when the catalyst loading decreased to 0.005%.Excellent performance was maintained during recycling experiments,indicating high stability of the catalyst.

关键词： high-dispersion single-atom catalysis O-silylation heterogeneous catalysis

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用于能源转化和环境修复的TiO_(2)基梯型异质结光催化剂

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Science China Materials 2024年第2期67卷 424-443页

作者：张宝龙孙彬刘方璇高婷婷周国伟 key laboratory of Fine Chemicals in universities of shandong Jinan Engineering Laboratory for Multi-scale Functional MaterialsSchool of Chemistry and Chemical EngineeringQilu University of Technology(Shandong Academy of Sciences)Jinan 250353China

太阳能驱动的半导体光催化技术被认为是缓解能源短缺和环境污染的潜在策略.因此,探索高效的光催化剂是推动光催化技术发展和实际应用的关键.作为一种典型的半导体光催化剂,TiO_(2)因其化学稳定、环境友好、成本低廉等特性而备受关注.然... 详细信息

太阳能驱动的半导体光催化技术被认为是缓解能源短缺和环境污染的潜在策略.因此,探索高效的光催化剂是推动光催化技术发展和实际应用的关键.作为一种典型的半导体光催化剂,TiO_(2)因其化学稳定、环境友好、成本低廉等特性而备受关注.然而,TiO_(2)光生载流子的快速复合、光吸收范围窄以及还原能力不足等缺点严重阻碍了其光催化性能.通过将TiO_(2)与其他半导体复合以构建梯型异质结可以有效的解决上述问题.在此光催化体系中,梯型异质结不仅可以整合各组分的优点,实现光生载流子的有效分离和光捕获能力的增强,而且还能保留最强的氧化还原能力.基于此,本文综述了利用构建梯型异质结来提高TiO_(2)光催化性能的最新研究进展,着重介绍了TiO_(2)基梯型异质结光催化剂的分类,主要包括金属氧化物、金属硫属化物、有机半导体和其他类型半导体.在此基础上,本文还总结了TiO_(2)基梯型异质结光催化剂在析氢、CO_(2)还原、H_(2)O_(2)生成和污染物降解等领域中的应用.同时,为了更好地理解光生载流子的转移途径,本文还简要介绍了梯型异质结的一些表征方法.最后,对TiO_(2)基梯型异质结光催化剂所面临的问题和未来的发展方向进行了展望.综上,本文旨在为构建用于能源转换和环境修复的高效TiO_(2)基梯型异质结光催化剂提供参考.

关键词： TiO_(2) step-scheme heterojunction photocatalysis energy conversion environmental remediation

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Diatomic active sites nanozymes:Enhanced peroxidase-like activity for dopamine and intracellular H2O2 detection

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Nano Research 2022年第5期15卷 4266-4273页

作者： Shan Wang Zunfu Hu Qiulian Wei Huimin Zhang Weina Tang Yunqiang Sun Haiqiang Duan Zhichao Dai Qingyun Liu Xiuwen Zheng Key Laboratory of Functional Nanomaterials and Technology in Universities of Shandong College of Chemistry and Chemical EngineeringLinyi UniversityLinyi 276000China School of Chemical and Biological Engineering Shandong University of Science and TechnologyQingdao 266510China School of Materials Science and Engineering Linyi UniversityLinyi 276000China

Considering intracellular hydrogen peroxide(H_(2)O_(2))plays pivotal roles in the regulation of serial biological processes,the in-situ detection of intracellular H2O2 has attracted an extensive attention.In the present work,an atomically dispersed diatomic active sites Nanozymes(FeN_(3)/PtN_(4)-single-atom nanozymes(SAzyme))was prepared exhibiting enhanced peroxidase-like activity.The obvious synergistic effect between Fe-Pt heteronuclear diatomic active sites was confirmed by series of characterization and density functional theory(DFT).The peroxidase-like activity of Fe-sites could be substantially enhanced by the bonded Pt-sites via the modulation effect.As a consequence,the gap between the d-band centre(εd)of Fe 3d orbitals and the Fermi energy level was narrowed and the electronic interaction could be strengthened,leading to a lower free energy barrier and a lower activation energy as well as fortified metal-O bonding in the kinetic pathway.Therefore,the constructed FeN3/PtN4-SAzyme exhibited higher peroxidase-like activity than that of FeN4-SAzyme.The FeN3/PtN4-SAzyme-assisted oxidation of 3,3',5,5'-tetramethylbenzidine(TMB)facilitated the colorimetric detection of dopamine(DA),an important biomolecule.The linear detection range and limit of detection(LOD)of DA and H_(2)O_(2) were 1-10 μM,0.01-1.0 mM and 0.109 μM,7.97 μM,respectively.In addition,the constructed SAzymes were also applied for the in-situ detection of intracellular H2O2,expanding the application scope of the newborn SAzymes.

关键词： single-atom nanozymes heteronuclear diatomic active sites peroxidase-like dopamine intracellular H_(2)O_(2)

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Layer-by-layer growth of ZIF-8 on electrospun carbon nanofiber membranes for high-performance supercapacistor electrode

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Journal of Energy Chemistry 2020年第8期29卷 221-224,I0008页

作者： Kan Mi Lanlan Song Hongjiao Nie Tao Liu Xianfeng Li Key Laboratory of Functional Nanomaterials and Technology in Universities of Shandong School of Chemistry and Chemical EngineeringLinyi UniversityLinyi 276000ShandongChina Division of Energy Storage Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina

In the past few decades, supercapacitor(SC) has attracted great attention due to its significant advantages over traditional rechargeable battery systems, such as high power density, fast charge-discharge rate, long cycle life and environmental friendliness [1]. Up to now, supercapacitors have been widely used in backup power, electric vehicles, mobile power and so on [2,3].

关键词： Supercapacitor ZIF-8 Electrospinning Ozone treatment Layer-by-layer

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Review on multi-dimensional assembled S-scheme heterojunction photocatalysts

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Journal of Materials Science & technology 2023年第29期160卷 214-239页

作者： Jiani Lu Shaonan Gu Hongda Li Yinan Wang Meng Guo Guowei Zhou key laboratory of Fine Chemicals in universities of shandong Jinan Engineering Laboratory for Multi-scale Functional MaterialsSchool of Chemistry and Chemical EngineeringQilu University of Technology(Shandong Academy of Sciences)Jinan 250353China Liuzhou key laboratory for New Energy Vehicle Power Lithium Battery School of Electronic EngineeringGuangxi University of Science and TechnologyLiuzhou 545006China

S-scheme heterostructure photocatalysts utilize the synergistic and superposition effects of materials,ef-fectively separating electrons and holes,maintaining strong redox capacity,and addressing issues en-countered by current photocatalytic reactions.This review explores the origins and unique benefits of S-scheme heterojunctions.Specifically,we summarized and discussed the effects of different dimensions of semiconductors constituting S-scheme heterojunctions and the similarities and differences in elec-tron transfer processes when constructing heterojunctions.Additionally,we analyzed several methods for proving the formation of S-scheme heterojunctions and the electron transfer process,both directly and indirectly.Finally,we review the applications of S-scheme heterojunctions in various fields of photo-catalysis,including photocatalytic water splitting,pollution degradation,CO_(2) reduction and other related photocatalytic applications.Our hope is that this review will provide an essential reference for the devel-opment and application of S-scheme heterojunction photocatalysis.

关键词： S-scheme heterojunctions Multi-dimensional assembled structures Photocatalysis Water splitting Pollution degradation Co_(2)reduction

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BiVO_(4),Bi_(2)WO_(6) and Bi_(2)MoO_(6) photocatalysis:A brief review

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Journal of Materials Science & technology 2020年第21期56卷 45-68页

作者： Xintong Liu Shaonan Gu Yanjun Zhao Guowei Zhou Wenjun Li key laboratory of Fine Chemicals in universities of shandong School of Chemistry and Pharmaceutical EngineeringQilu University of Technology(Shandong Academy of Sciences)Jinan273100China Beijing key laboratory for Science and Application of functional Molecular and Crystalline Materials University of Science and Technology BeijingBeijing100083China

In recent years,photocatalytic technologies have been extensively studied and diffusely used in water splitting,decomposition of organic pollutants,reduction of carbon dioxide,etc.As a type of eye-catching semiconductors,BiVO_(4),Bi_(2)WO_(6),and Bi_(2)MoO_(6) (denoted as BiaAOb)have become a hotspot in photocatalytic researches due to their crystal structure stability,high light quantum and electronic transmission efficiency,and outstanding energy utilization capacity.However,pristine BiaAOb(A=V,W,and Mo)possesses several drawbacks,such as low separation efficiency of photo-excited electron-hole pairs,low specific surface area,as well as the poor quantum utilization,which restrict their photocatalytic performance.Considerable efforts,such as nanostructure modification,surface engineering,and heterojunction/homojunction fabrication,have been conducted to solve these problems.This integrated review aims to sum up recent advances in current studies on fabrication of high efficiency BiaAOb photocatalysts to accelerate the developments of BiaAOb-based materials in the photocatalysis(PC)field.The current challenges and prospects of BiaAOb are emphasized which stretches the existing fundamental theories of PC as well as provide a promising strategy to fabricate high efficiency BiaAOb catalysts to control environmental pollution and assist the sustainable development of energy.

关键词： Photocatalyst Bismuth vanadate Heterojunction Solar fuels

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Self-template formation of porous yolk-shell structure Mo-doped NiCo2O4 toward enhanced lithium storage performance as anode material

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Journal of Materials Science & technology 2022年第7期102卷 186-194页

作者： Yongqiang Ren Xiuyan Li Yinan Wang Qinghua Gong Shaonan Gu Tingting Gao Xuefeng Sun Guowei Zhou key laboratory of Fine Chemicals in universities of shandong Jinan Engineering Laboratory for Multi-scale Functional MaterialsSchool of Chemistry and Chemical EngineeringQilu University of Technology(Shandong Academy of Sciences)Jinan 250353China School of Chemical Engineering and Environment Shandong Peninsula Engineering Research Center of Comprehensive Brine UtilizationWeifang University of Science and TechnologyWeifang 262700China

Hollow ternary metal oxides have shown enormous potential in lithium-ion batteries(LIBs),which is ascribed to their complex chemical composition,abundant active defect sites,and the synergy effect be-tween metals.In this work,we synthesized Mo-doped NiCo_(2)O_(4) porous spheres with yolk-shell structure by using a simple self-templating method.Surprisingly,other than the yolk-shell structure we had ob-tained,the inner core of the yolk-shell was also porous,which could fully enhance the electrolyte infil-tration and promote the transmission of lithium ions(Li+)and electrons(e−).The diameter of the porous core in the yolk-shell sphere was about 530 nm,and the outer shell’s thickness was up to 110 nm.In addition,the unique pores in the core appeared in the diameter of about 85 nm.With this structure,the volume expansion of the anode could be well inhibited during charge/discharge.It exhibited prominent electrochemical performance with high reversible capacity(1338 mA h g^(−1) at 100 mA g^(−1)),satisfactory cycle life(1360 mA h g^(−1) after 200 cycles at 100 mA g^(−1)),and exceptional rate capability(820 mA h g^(−1) at 2000 mA g^(−1))as anode material in LIBs.

关键词： Ternary metal oxides Yolk-shell structure Porous inner core Anode material Lithium-ion batteries

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一体式自漂浮多孔泡沫作为隔热层用于高效光热转换和太阳能脱盐

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Science Bulletin 2023年第22期68卷 2760-2768,M0005页

作者：任丽萍周卫王蕾林阔徐亚超武佳星谢颖付宏刚 key laboratory of functional Inorganic Material Chemistry(Ministry of Education) Heilongjiang UniversityHarbin 150080China shandong Provincial key laboratory of Molecular Engineering School of Chemistry and Chemical EngineeringQilu University of Technology(Shandong Academy of Sciences)Jinan 250353China

本文通过冷冻干燥铸造成型和高温表面氢化策略,构筑了一种自漂浮等离子体Ag/黑色TiO_(2)/碳多孔层状泡沫(Ag-BTCFs)作为高效的太阳能热集流体.这种一体式三维(3D)交联自漂浮多孔层状泡沫材料可以实现全光谱吸收(~95.45%),并有效地阻止... 详细信息

本文通过冷冻干燥铸造成型和高温表面氢化策略,构筑了一种自漂浮等离子体Ag/黑色TiO_(2)/碳多孔层状泡沫(Ag-BTCFs)作为高效的太阳能热集流体.这种一体式三维(3D)交联自漂浮多孔层状泡沫材料可以实现全光谱吸收(~95.45%),并有效地阻止热量向下层水体传导.Ag-BTCFs受益于光照射下Ag的局域表面等离子体效应驱动的“热点”效应,促进了光生热电子(e^(-))和光生空穴(h^(+))在等离子体辅助半导体中的传输.此外,具有亲水性的黑色TiO_(2)可以作为水的传输介质.与层状碳泡沫的耦合不仅提高了材料的吸收率,而且促进了热电子的弛豫和集热.更重要的是,光生h~+被用来光催化降解污染物,在不影响蒸汽产生效率的情况下实现了降解污染物和淡水生产的同步进行,这种高效的新型轻质自漂浮Ag-BTCFs将在太阳能蒸汽发电和海水淡化中具有潜在的应用前景.

关键词： Solar steam generation Self-floating porous foam Heat-blocked layer Black TiO_(2) Photothermal conversion

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Multidimensional defects tailoring local electron and Mg^(2+) diffusion channels for boosting magnesium storage performance of WO_(3)/MoO_(2)

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Journal of Energy Chemistry 2023年第9期84卷 476-485页

作者： Shiqi Ding Yuxin Tian Jiankang Chen He Lv Amin Wang Jingjie Dai Xin Dai Lei Wang Guicun Li Alan Meng Zhenjiang Li College of Materials Science and Engineering Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life ScienceMOECollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina Qingdao Engineering Research Center for New Metallic functional Materials Characteristic Laboratory of Advanced Metal Functional Materials and Processing in Universities of ShandongQingdao Binhai UniversityQingdao 266555ShandongChina College of Electromechanical Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina

Defect engineering presents great promise in addressing lower specific capacity,sluggish diffusion kinetics and poor cycling life issues in energy storage devices.Herein,multidimensional(0D/2D/3D) structural defects are constructed in WO_(3)/MoO_(2) simultaneously via competing for and sharing with O atoms during simple hydrothermal process.OD and 2D defects tailor local electron,activating more sites and generating built-in electric fields to yield ion reservoir,meanwhile,3D defect owning lower anisotropic property tailors Mg^(2+) diffusion channels to fully exploit Mg^(2+) adsorbed sites induced by OD and 2D defects,enhance the kinetics and maintain structural stability.Benefitted from synergistic effect of 0D/2D/3D structural defects,the designed WO_(3)/MoO_(2) shows the higher specific capacity(112.8 mA h g^(-1) at 50 mA g^(-1) with average attenuation rate per cycle of 0.068%),superior rate capability and excellent cycling stability(specific capacity retention of 80% after 1500 cycles at 1000 mA g^(-1)).This strategy provides design ideas of introducing multidimensional structural defects for tailoring local electron and microstructure to improve energy storage property.

关键词： Multidimensional defects Local electron tailoring Heterostructure Cathode Magnesium ions batteries

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Identification of different degrees of processed ginger using GC-IMS combined with machine learning

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Journal of Pharmaceutical Analysis 2024年第1期14卷 149-151页

作者： Shuang Liu Hongjing Dong Minmin Zhang Wei Geng Xiao Wang key laboratory for Applied technology of Sophisticated Analytical Instruments of shandong Province Shandong Analysis and Test CenterQilu University of Technology(Shandong Academy of Sciences)Jinan250014China key laboratory for Natural Active Pharmaceutical Constituents Research in universities of shandong Province School of Pharmaceutical SciencesQilu University of Technology(Shandong Academy of Sciences)Jinan250014China shandong Provincial Maternal and Child Health Care Hospital Affiliated to Qingdao University Jinan250014China

Ginger,the rhizomes of Zingiber officinale Roscoe,was a wellknown edible plant species commonly used in China,which has pungent flavor[1].Ginger has numerous chemical compounds,such as phenolic constituents,volatile compounds(VOCs),and polysaccharides[2].Among them,VOCs are considered one of the effective compounds in ginger due to their functional properties,including anti-inflammatory,antioxidant,and analgesic[3].

关键词： phenolic edible rhizome

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