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Recent progress in single-molecule fluorescence technology in nanocatalysis

Nano Research 2022年第12期15卷 10316-10327页

作者： Jing Cao Dezheng Zhang Weilin Xu State Key Laboratory of Electroanalytical Chemistry and Jilin Province Key Laboratory of Low Carbon Chemical Power Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China University of Science and Technology of China Hefei230026China

Nanoparticles(NPs)play a vital role in the energy catalysis process,so understanding the heterogeneous catalytic properties of nanocatalysts is of great significance for rationally guiding the design of catalysts.However,the traditional method obtains the average information based on the whole and cannot study the catalytic activity of a single nanoparticle.It is critical to investigate the catalytic activity of individual nanoparticles using in situ techniques.This review summarizes some of Prof.Xu's recent accomplishments in studying the catalytic behavior of nanoparticles at the single-particle level using single-molecule fluorescence microscopy(SMFM).These achievements include revealing the effect of size,shape,and surface atoms of Pd nanoparticles on catalytic kinetics and dynamics as well as obtaining the activation energy of single Au nanoparticles for catalytic reactions by single-molecule methods.It is the first time to study the kinetics and dynamics of single-atom Pt catalysts.Furthermore,the method was extended to study the Pt deactivation process for hydrogen oxidation reactions as well as the catalytic kinetics of two-electron oxygen reduction reactions of individual Fe3O4 nanoparticles in electrocatalysis.Finally,single-molecule super-resolution techniques were used to observe the evolution of the activity of single Sb doped TiO2 nanorod domains.These studies are of guiding significance for in-depth understanding and realization of rational design of optimal catalysts.

关键词： single-molecule fluorescence microscopy nanocatalysis kinetics and dynamics activation energy electrocatalysis super-resolution imaging

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Catalyst-free multicomponent polymerization of sulfonyl azide,aldehyde and cyclic amino acids toward zwitterionic and amphiphilic poly(N-sulfonyl amidine)as nanocatalyst precursor

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Science China Chemistry 2022年第9期65卷 1798-1806页

作者： Erli Tian Ming Li Wangze Song Nan Zheng State Key Laboratory of Fine Chemicals School of Chemical EngineeringDalian University of TechnologyDalian 116024China

Polymers with metal coordination ability are outstanding precursors of nanocatalysts,attracting numerous attention in nanocatalysis area.It has been rarely reported for the poly(N-sulfonyl amidines)as macromolecular ligands for nanocatalysis.Herein,a catalyst-free multicomponent polymerization(MCP)strategy is developed to facilely prepare a library of amphiphilic poly(Nsulfonyl amidines)with zwitterionic properties starting from disulfonyl azide,hydrophilic dialdehyde and cyclic amino acids including proline and pipecolinic acid.Metals or additives can be thorougly avoided through this method.All the obtained polymers have well-defined structures,high yields and weight-average molecular weights(M_(w)s,up to 99,300 g/mol).The unique zwitterionic property,amphiphilicity and Cu(Ⅰ)coordination ability of the obtained poly(N-sulfonyl amidines)endow them to form the polymer-Cu(Ⅰ)complexes as nanocatalysts.Such nanocatalysts exhibit high catalytic efficiency in aqueous Cucatalyzed azide-alkyne cycloaddition(CuAAC)reaction at a low Cu(Ⅰ)loading of 50 ppm.Nanocatalysts with a high ratio of polymers to Cu(Ⅰ)have also been demonstrated with Cu(Ⅰ)stabilization ability.This work provides a“green”MCP method toward zwitterionic and amphiphilic poly(N-sulfonyl amidines),and highlights their unique potentials for nanocatalysis.

关键词： multicomponent polymerization zwitterion catalyst-free nanocatalysis poly(N-sulfonyl amidines)

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Thiol-stabilized atomically precise, superatomic silver nanoparticles for catalysing cycloisomerization of alkynyl amines

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National Science Review 2018年第5期5卷 694-702页

作者： Juanzhu Yan Jun Zhang Xumao Chen Sami Malola Bo Zhou Elli Selenius Xiaomin Zhang Peng Yuan Guocheng Deng Kunlong Liu Haifeng Su Boon K.Teo Hannu Hkkinen Lansun Zheng Nanfeng Zheng State Key Laboratory for Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materialsand Engineering Research Center for Nano-Preparation Technology of Fujian ProvinceCollege of Chemistry and Chemical EngineeringXiamen University School of Materials and Chemical Engineering Anhui Jianzhu University Departments of Physics and Chemistry Nanoscience CenterUniversity of Jyvskyl

Both the electronic and surface structures of metal nanomaterials play critical roles in determining their chemical properties. However, the non-molecular nature of conventional nanoparticles makes it extremely challenging to understand the molecular mechanism behind many of their unique electronic and surface properties. In this work, we report the synthesis, molecular and electronic structures of an atomically precise nanoparticle, [Ag206 L72]~q(L = thiolate, halide; q = charge). With a four-shell Ag7@Ag32@Ag77@Ag90 Ino-decahedral structure having a nearly perfect D5hsymmetry, the metal core of the nanoparticle is co-stabilized by 68 thiolate and 4 halide ligands. Both electrochemistry and plasmonic absorption reveal the metallic nature of the nanoparticles, which is explained by density functional theory calculations.Electronically, the nanoparticle can be considered as a superatom, just short of a major electron shell closing of 138 electrons(q = –4). More importantly, many of ligands capping on the nanoparticle are labile due to their low-coordination modes, leading to high surface reactivity for catalysing the synthesis of indoles from 2-ethynylaniline derivatives. The results exemplify the power of the atomic-precision nanocluster approach to catalysis in probing reaction mechanisms and in revealing the interplay of heterogeneous reactivities,electronic and surface structural dynamics, thereby providing ways for optimization.

关键词： metal nanoclusters atomically precise nanoparticles nobel metal superatom nanocatalysis

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Pd-Ni nanoparticles supported on titanium oxide as effective catalysts for Suzuki-Miyaura coupling reactions

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Frontiers of Chemical Science and Engineering 2018年第1期12卷 24-31,F0004页

作者： Dongxu Han Zhiguo Zhang Zongbi Bao Huabin Xing Qilong Ren Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological Engineering Zhejiang University Hangzhou 310027 China

We have successfully prepared a series of Pd- Ni/TiO2 catalysts by a one-step impregnation-reduction method. Among these catalysts with different compositions of Ni and Pd, the one with the Ni：Pd ratio of 2.95 showed the best activity. Small monodispersed Pd-Ni bimetallic nanoparticles were loaded on the surface of titanium oxide nanopowder as confirmed with TEM and EDS mapping. The XPS analysis demonstrated that Pd exists as 31% Pd（II） species and 69% Pd（0） species and all nickel is Ni（II）. The prepared Pd-Ni/TiO2 exhibited enhanced catalytic activity compared to an equal amount of Pd/TiO2 for Suzuki-Miyaura reactions together with excellent applicability and reusability.

关键词： Pd-Ni bimetallic nanoparticles nanocatalysis Suzuki-Miyaura reaction titanium oxide

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Composition-tuned oxidation levels of Pt-Re bimetallic nanoparticles for the etherification of allylic alcohols

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Nano Research 2018年第11期11卷 5902-5912页

作者： Yuhao Wang Lindong Li Ke Wu Rui Si Lingdong Sun Chunhua Yan Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and Applications PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry College of Chemistry and Molecular Engineering Peking University Beijing 100871 China Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied Physics Chinese Academy of Sciences Shanghai 201204 China

The catalytic performance of metal nanoparticles is often affected by surface oxidation levels. Instead of post-synthesis oxidation/reduction, we propose an efficient method to modulate the oxidation levels by tuning the composition of bimetallic nanoparticles. Here we report a series of Pt–Re bimetallic nanoparticles synthesized via a facile thermal co-reduction process, with a uniform size of approximately 3 nm. The investigation of the growth of the Pt–Re nanoparticles suggests that the Re atoms were enriched on the surface, as confirmed by X-ray photoelectron spectroscopy. Furthermore, X-ray absorption spectroscopy showed that metallic Re was decreased and high-valency ReOx species were increased in particles with higher Re/Pt ratios. In the etherification of allylic alcohols catalyzed by Pt–Re nanoparticles of different compositions under ambient conditions, particles with higher Re/Pt ratios exhibited significantly better performances. The highest mass activity of Pt–Re bimetallic nanoparticles (127 μmol·g−1·s−1) was more than forty times that of the industrial catalyst CH3ReO3 (3 μmol·g−1·s−1). The catalytically active sites were associated with ReOx and could be tuned by adjusting the Pt ratio.

关键词： nanocatalysis Re Pt oxidation level composition allylic alcohol

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Single Ti atoms coupled with Ti-O clusters enable low temperature hydrogen cycling by sodium alanate

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Rare Metals 2024年第6期43卷 2671-2681页

作者： Zhuang-He Ren Xin Zhang Wen-Xuan Zhang Zhen-Guo Huang Li-Mei Yang Ya-Xiong Yang Zheng-Long Li Juan Li Wen-Ping Sun Ming-Xia Gao Hong-Ge Pan Yong-Feng Liu State Key Laboratory of Silicon and Advanced Semiconductor Materials Zhejiang University School of Materials Science and Engineering Zhejiang University School of Civil & Environmental Engineering University of Technology Sydney Institute of Science and Technology for New Energy Xi'an Technological University College of Materials Science and Engineering Zhejiang University of Technology

Ti-based catalysts are known to improve the hydrogen storage performance of NaAlH4by facilitating the dissociation/recombination of H-H and Al-H bonds.The catalytic activity of metallic Ti species strongly depends on its particle size and dispersity.Ti clusters and even single atoms are therefore highly desirable,but their controllable fabrication has been highly challenging.He rein,we demonstrate a novel facile sonochemical synthesis of a Ti-O clusters featuring single Ti atom catalyst at room temperature.Through reducing TiCl4by MgBu2with ultrasound instead of heating as driving force,numerous single Ti atoms coupled with Ti-O clusters with Ti loading on graphene(Ti1/Ti-O@G) up to 22.6 wt% have been successfully obtained.The prepared Ti1/Ti-O@G contributes high reactivity and superior catalytic activity,therefore enabling full dehydrogenation of NaAlH4at 80 ℃ in thermogravimetric mode and re-hydrogenation at 30 ℃ and 10 MPa with 4.9 wt% H2.This fact indicates for the first time that single Ti atom catalyst with high loading is highly effective in catalyzing hydrogen cycling of NaAlH4at remarkably reduced temperatures.

关键词： Hydrogen storage nanocatalysis Transition metals Single Ti atoms NaAlH 4

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Understanding nano effects in catalysis

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National Science Review 2015年第2期2卷 183-201页

作者： Fan Yang Dehui Deng Xiulian Pan Qiang Fu Xinhe Bao State Key Laboratory of Catalysis iChEM(Collaborative Innovation Center of Chemistry for Energy Materials)Dalian Institute of Chemical PhysicsChinese Academy of Sciences

Catalysis, as a key and enabling technology, plays an increasingly important role in ields ranging from energy, environment and agriculture to health care. Rational design and synthesis of highly eicient catalysts has become the ultimate goal of catalysis research. hanks to the rapid development of nanoscience and nanotechnology, and in particular a theoretical understanding of the tuning of electronic structure in nanoscale systems, this element of design is becoming possible via precise control of nanoparticles’ composition, morphology, structure and electronic states. At the same time, it is important to develop tools for in situ characterization of nanocatalysts under realistic reaction conditions, and for monitoring the dynamics of catalysis with high spatial, temporal and energy resolution. In this review, we discuss coninement efects in nanocatalysis, a concept that our group has put forward and developed over several years. Taking the conined catalytic systems of carbon nanotubes, metal-conined nano-oxides and 2D layered nanocatalysts as examples, we summarize and analyze the fundamental concepts, the research methods and some of the key scientiic issues involved in nanocatalysis. Moreover, we present a perspective on the challenges and opportunities in future research on nanocatalysis from the aspects of:(1) controlled synthesis of nanocatalysts and rational design of catalytically active centers;(2) in situ characterization of nanocatalysts and dynamics of catalytic processes;(3) computational chemistry with a complexity approximating that of experiments; and (4) scale-up and commercialization of nanocatalysts.

关键词： nanocatalysis coninement carbon nanotubes graphene 2D materials inverse catalysts computational chemistry in situ characterizati

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Electrocatalytic acidic oxygen evolution reaction:From nanocrystals to single atoms

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Aggregate 2021年第4期2卷 100-121页

作者： Nadia Ismail Fengjuan Qin Chaohe Fang Dan Liu Bihan Liu Xiangyu Liu Zi-long Wu Zhuo Chen Wenxing Chen Energy&Catalysis Center Department of Materials Physics and ChemistrySchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijingPeople’s Republic of China CNPC Research Institute of Petroleum Exploration&Development BeijingPeople’s Republic of China

Hydrogen is the most preferred choice as an energy source to replace the nonrenewable energy resources such as fossil fuels due to its beneficial features of abundance,ecofriendly,and outstanding gravimetric energy density.Splitting water through a proton exchange membrane(PEM)electrolyzer is a well-known method of hydrogen production.But the major impediment is the sluggish kinetics of oxygen evolution reaction(OER).Currently,scientists are struggling to build out an acid-stable electrocatalyst for OER with low overpotential and excellent stability.In this review,the reaction mechanism and characterization parameters of OER are introduced,and then the improvement method of metal nanocatalysts(noble metal catalysts and noble metal-free catalysts)in acidic media is discussed.Particularly,the application of single-atom catalysts in acidic OER is summarized,which is current researching focus.At the same time,we also briefly introduced the cluster phenomenon,which is easy to occur in the preparation of single-atom catalysts.More importantly,we summarized the in situ characterization methods such as in situ X-ray absorption spectroscopy,in situ X-ray photoelectron spectroscopy,and so forth,which are conducive to further understanding of OER reaction intermediates and active sites.Finally,we put forward some opinions on the development of acidic OER.

关键词： acidic media in situ characterization nanocatalysis oxygen evolution reaction single-atom catalysis

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Nanocatalytic resonance scattering spectral analysis

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Science China Chemistry 2010年第5期53卷 1048-1053页

作者： Jiang, ZhiLiang Li, JiShun Wen, GuiQing Liu, QingYe Liang, AiHui School of Environment and Resources Guangxi Normal University Guilin 541004 China College of Chemistry and Bioengineering Guilin University of Technology Guilin 541004 China

The resonance scattering spectral technique has been established using the synchronous scanning technique on spectrofluorometry.Because of its advantages of simplicity,rapidity and sensitivity,it has been widely applied to analyses of proteins,nucleic acids and inorganic ions.This paper summarizes the application of immunonanogold and aptamer modified nanogold(AptAu) catalytic resonance scattering spectral technique in combination with the work of our group,citing 53 references.

关键词： antibody aptamer nanocatalysis resonance scattering spectral assay

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Pd nanocrystals stabilized by cucurbit[6]uril as efficient heterogeneous catalyst for direct C-H functionalization of polyfluoroarenes

Pd nanocrystals stabilized by cucurbit[6]uril as efficient h...

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中国化学会第九届全国无机化学学术会议

作者： Minna Cao Dongshuang Wu Rong Cao State key laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter the Chinese Academy of Science

Synthesis of biaryl compounds through C-H bond activation of arylation has been the focus and frontier research in the field of green chemistry and Pharmaceutical Synthesis. TAraditional homogeneous catalysts has made great achievements in this field. However, there are many issue to resolve, such as the large amount of catalysts dose, recycle problem of catalysts, and product isolation problems. Moreover, the catalytic process generally requires relatively harsh dry environments, which increases the cost of large-scale synthesis and causes environmental pollution. We succeeded in synthesizing uniformly dispersed Pd nanocomposite with sub-5 nm in size by using cucurbit[n]uril as a carrier via a simple one-pot method. With significantly noble metal loading, such nanocomposite showed high activity towards C-H bond activation with satisfactory yields of the product. The catalytic procedure was safe to air and moisture. Importantly, the developed catalytic system can be effectively recycled multiple times without obvious loss of activity with a broad range of substrates, demonstrating a good efficiency and selectivity. The research group also studied the effect of different type of cucurbit[n]uril（n=5-8） on the structure of Pd nanocomposite as well as the corresponding catalytic performance. The heterogeneous catalytic mechanism of the C-H bond activation was also verified by experimental data.

关键词： C-H functionalization nanocatalysis Cucurbit[n]ruil Polyfluoroarenes

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