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Effects of length alteration of OPE-containing mono- and dinuclear alkynylplatinum(II) terpyridine complexes on photophysical, structural and morphological properties

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Nano Research 2024年第10期17卷 8893-8903页

作者： Jason Koon-Lam Poon Sammual Yu-Lut Leung Eric Ka-Ho Wong Vivian Wing-Wah Yam Institute of Molecular Functional materials State Key Laboratory of Synthetic Chemistry and Department of ChemistryThe University of Hong KongHong Kong 999077China

A series of mononuclear complexes and unsymmetric dinuclear alkynylplatinum(II)terpyridine complexes with oligo(paraphenylene ethynylene)(OPE)-derived backbone with a variation of the lengths of alkoxy chains and OPE backbones was *** morphological properties,packing lattice and gelation behaviors of the mononuclear complexes were systematically studied,and the thermodynamic parameters and packing lattices of the dinuclear complexes were also investigated,providing further insights into the roles of the non-covalent interactions and their delicate balance in constructing sophisticated supramolecular *** and nanotube formation have been observed upon a delicate control of the intermolecular interactions by altering the lengths and structural dimensions of the complexes.

关键词： supramolecular chemistry self-assembled nanostructures platinum(II)complexes metallogel

High-rate lithium-ion battery performance of a ternary sea urchin-shaped CoNiO_(2)@NiP_(6)Mo_(18)/CNTs composites

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Journal of Energy chemistry 2024年第9期96卷 516-525页

作者： Li-ping Cui Shuang Sun Kai Yu Shu Zhang Mei-lin Wang Jia-jia Chen Bai-bin Zhou Key laboratory for Photonic and Electronic Bandgap materials Ministry of EducationSchool of Chemistry and Chemical EngineeringHarbin Normal UniversityHarbin 150025HeilongjiangChina State Key laboratory of Physical chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringCollaborative Innovation Centre of Chemistry for Energy MaterialsXiamen UniversityXiamen 361005FujianChina

Bimetallic oxides are attractive anode materials for lithium-ion batteries(LIBs)due to their large theoretical ***,the low conductivity,short cycle life,and poor rate capability are the bottlenecks for their further *** overcome above issues,the basket-like polymolybdate(NiP_(6)Mo_(18))and carbon nanotubes(CNTs)were uniformly embedded on the urchin-shaped CoNiO_(2)nanospheres to yield a ternary composites CoNiO_(2)@NiP_(6)Mo_(18)/CNTs via electrostatic *** multi-level morphology of urchin spinules accelerates the diffusion rate of Li^(+);CNT improves the conductivity and enhances cycle stability of the material;and heteropoly acid contributes more redox activity ***,CoNiO_(2)@NiP_(6)Mo_(18)/CNTs as an anode of LIBs exhibits a high initial capacity(1396.7 mA h g^(−1)at 0.1 A g^(−1)),long-term cycling stability(750.2 mA h g^(−1)after 300 cycles),and rate performance(450.3 mA h g^(−1)at 2 A g^(−1)),which are superior to reported metallic oxides anode of *** density functional theory(DFT)and kinetic mechanism suggest that CoNiO_(2)@NiP_(6)Mo_(18)/CNTs delivers an outstanding pseudocapacitance and rapid Li^(+)diffusion behaviors,which is due to the rich surface area of the urchin-like CoNiO_(2)with the uniform embeddedness of NiP_(6)Mo_(18)and *** study provides a new idea for optimizing the performance of bimetallic oxides and developing high-rate lithium-ion battery composites.

关键词： Bi-metal oxides Transition metal oxides Polyoxometalates Nanocomposite LIBs

Precise immobilization of metal single atoms into a porphyrinic metal-organic framework for an efficient alkene hydrosilylation

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Nano Research 2024年第7期17卷 5914-5921页

作者： Chun-Ying Chen Qi-Jie Mo Fu-Zhen Li Hai-Li Song Li Zhang MOE laboratory of Bioinorganic and Synthetic chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-Sen UniversityGuangzhou 510006China

Alkene hydrosilylation is one of the most concise and atom-economical methods to synthesize organosilicon ***,we reported the precise immobilization of metal single atoms(M-SAs;M=Ru,Rh,Ir,Pd,Pt,and Au)into a porphyrinic metalorganic framework(MOF)of PCN-222(PCN=porous coordination network),and then applied the resultant MOF composites of M-SAs@PCN-222 to alkene *** solvent-free conditions,Pt-SAs@PCN-222 displayed an especially high catalytic efficiency with the turnover frequency up to 119 s−1 and the maximum turnover number of 906,250 at room *** and theoretical studies revealed that there existed strong interactions between Pt-SAs@PCN-222 and the substrates,which helped to condense the substrates in the cavities of the porous *** density functional theory calculations and molecular dynamics simulations disclosed that PCN-222 could transfer electrons to Pt-SAs to enhance the silane oxidative addition and drive the reaction to proceed smoothly via Chalk–Harrod pathway.

关键词： alkene hydrosilylation single atom catalysts metal-organic frameworks precision chemistry synergistic catalysis

Designed imidazole-based supramolecular catalysts for accelerating oxidation/hydrolysis cascade reactions

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Nano Research 2024年第6期17卷 4916-4923页

作者： Yuanxi Liu Wenjie Xu Shichao Xu Haifeng Wu Baoli Zhang Li Song Zhen-Gang Wang State Key laboratory of Organic-inorganic Composites Key Lab of Biomedical Materials of Natural Macromolecules(Ministry of Education)Beijing Laboratory of Biomedical MaterialsCollege of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China National Synchrotron Radiation laboratory CAS Center for Excellence in NanoscienceUniversity of Science and Technology of ChinaHefei 230029China

Reconstructing enzymatic active sites presents a significant challenge due to the intricacies involved in achieving enzyme-like scaffold folding and spatial arrangement of essential functional *** is also a growing interest in building biocatalytic networks,wherein multiple enzymatic active sites are localized within a single artificial system,allowing for cascaded *** this work,we report the self-assembly of imidazole or its derivatives with fluorenylmethyloxycarbonyl-modified histidine and Cu2+to fabricate a supramolecular catalyst,which possesses catechol oxidase-like dicopper center with multiple imidazole as the coordination *** electron microscopy,low-temperature X-band continuous-wave electron paramagnetic resonance,K-edge X-ray absorption spectra/the extended X-ray absorption fine structure analysis,and density functional theory modeling were used for the structural characterization of the *** phenol derivatives and the dissolved oxygen were used as the substrates,with the addition of 4-aminoantipyrine to generate a red adduct with a maximum absorbance at 510 nm,for obtaining time-dependent absorbance change curves and estimating the *** results reveal that the addition of imidazole synergistically accelerates the oxidative activity about 10-fold and the hydrolysis activity about 14-fold than fluorenylmethyloxycarbonyl modified-histidine/Cu2+.The supramolecular nanoassembly also exhibits the ability to catalyze oxidation/hydrolysis cascade reactions,converting 2′,7′-dichlorofluorescin diacetate into 2′,7′-*** process can be regulated through the methylation of the imidazole component at various *** work may contribute to the design of advanced biomimetic catalysts,and shed light on early structural models of the active sites of the primitive copper-dependent enzymes.

关键词： enzyme mimic self-assembly supramolecular catalyst cascade reactions

Controllable selective anchoring of subnanometric Ru clusters or single-atoms/clusters on tungsten nitride for the hydrogen oxidation

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Science China chemistry 2024年

作者： Qijiao Sun Chuanqiang Wu Yiqiang Sun Yuan Shen Lei Zhao Xiaodong Yang Li Yang Yunxiang Lin Keke Mao Kun Xu School of chemistry and Chemical Engineering Key Laboratory of Functional Inorganic Material Chemistry of Anhui Province Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education Anhui University Information materials and Intelligent Sensing laboratory of Anhui Province Institutes of Physical Science and Information TechnologyAnhui University School of chemistry and Chemical Engineering University of Jinan School of Energy and Environment Anhui University of Technology

The impregnation method in the preparation of metal cluster catalysts typically inadvertently introduces single atoms （SAs） into the substrate. However, the question of whether the introduction of SAs will further improve the catalytic activity of cluster systems for specific reactions such as the hydrogen oxidation reaction （HOR） remains unraveled. Herein, we demonstrate Ru clusters anchored on WN nanowires （RuC/WN） show a higher alkaline HOR catalytic activity in comparison with Ru SAs and nanoclusters （NCs）-coupled catalyst anchored on WN nanowires system （RuC,S/WN）. Notably, the RuC/WN exhibits superb intrinsic catalytic activity with a mass-normalized exchange current density of 890 mA mg-1PGM, which is among the top level of well developed Ru-based HOR catalysts. Both theoretical simulation and experimental investigation suggest that RuC/WN owns an optimized H*and OH*reaction intermediates for the alkaline HOR, therefore resulting in the excellent intrinsic HOR catalytic performance.

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Insight into the Role of Isolated Gold Atoms-Ceria Conjunction in Catalyzing the Water-Gas Shift Reaction

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Chinese Journal of chemistry 2024年第6期42卷 636-644页

作者： Xin-Pu Fu Hui-Zhao Wei-Wei Wang Chun-Jiang Jia Key laboratory for Colloid and Interface chemistry Key Laboratory of Special Aggregated MaterialsSchool of Chemistry and Chemical EngineeringShandong UniversityJinanShandong250100 China

As the promising catalysts for the water-gas shift(WGS)reaction,the activity of Au-CeO_(2) composites is susceptible to the aggregation size and electronic state of Au *** reports were extensively focused on the discrepancy between nonmetallic Au and metallic Au nanoparticles,whereas the understanding of the authentic role of the isolated Au atoms was ***,we investigated the catalytic behavior and structural information over two types of Au/CeO_(2) catalysts,in which the predominant conjunctions were isolated Au1-CeO_(2) and Aun-CeO_(2),*** on comprehensive characterizations,particularly by in-situ Raman and in-situ DRIFTS,we found that the isolated Au atoms were responsible for enhancing the reducibility of the CeO_(2) *** CO adsorption ability on the isolated Au sites was significantly inferior to clustered Au atoms,especially at relatively high temperatures(>200°C).As a result,the boosted O vacancy on the isolated Au1-CeO_(2) conjunctions could improve the H2O activation ability for the Au-CeO_(2) catalysts and demonstrate a comparable activity to the clustered Aun-CeO_(2) *** work might deepen understanding of the catalytic function for the isolated Au1 site within Au/CeO_(2) systems while catalyzing the WGS reaction.

关键词： Isolated Au atoms Ceria-based catalysts Water-gas shift reaction Defect Adsorption

Rational design of new in situ reduction of Ni(II)catalytic system for low-cost and large-scale preparation of porous aromatic frameworks

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Carbon Energy 2024年第5期6卷 105-113页

作者： Shanshan Wang Yue Wu Wenxiang Zhang Hao Ren Guangshan Zhu Heping Ma School of Chemical Engineering and Technology Xi'an Jiaotong UniversityXi'anChina State Key laboratory of inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchunChina College of chemistry Northeast Normal UniversityChangchunChina

Porous aromatic framework 1(PAF-1)is an extremely representative nanoporous organic framework owing to its high stability and exceptionally high surface ***,the synthesis of PAF-1 is catalyzed by the Ni(COD)2/COD/bpy system,suffering from great instability and high ***,we developed an in situ reduction of the Ni(II)catalytic system to synthesize PAF-1 in low cost and high *** active Ni(0)species produced from the NiCl_(2)/bpy/NaI/Mg catalyst system can effectively catalyze homocoupling of tetrakis(4-bromophenyl)methane at the room temperature to form PAF-1 with high Brunauer-Emmett-Teller(BET)-specific surface area up to 4948 m^(2) g^(−1)(Langmuir surface area,6785 m2 g−1).The possible halogen exchange and dehalogenation coupling mechanisms for this new catalytic process in PAF's synthesis are discussed in *** efficiency and universality of this innovative catalyst system have also been demonstrated in other PAFs'*** work provides a cheap,facile,and efficient method for scalable synthesis of PAFs and explores their application for high-pressure storage of Xe and Kr.

关键词： adsorption carbon material nickel catalysis porous aromatic framework porous organic polymer

Efficient and selective upcycling of waste polylactic acid into acetate using nickel selenide

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Journal of Energy chemistry 2024年第10期97卷 575-584页

作者： Bing Lan Yinfang Chen Nantian Xiao Na Liu Chao Juan Chuan Xia Fan Zhang National Engineering laboratory of Eco-Friendly Polymeric materials College of Chemistry Sichuan University School of materials and Energy University of Electronic Science and Technology of China

The conversion of waste polylactic acid（PLA） plastics into high-value-added chemicals through electrochemical methods is a promising and sustainable ***,developing efficient and highly selective catalysts for lactic acid oxidation reaction（LAOR） and understanding the reaction process are ***,we report the electrooxidation of waste PLA to acetate at a high current density of 100 mA cm-2 with high Faraday efficiency（～95%） and excellent stability（>100 h） over a nickel selenide nanosheet *** addition,a total Faraday efficiency of up to 190% was achieved for carboxylic acids,including acetic acid and formic acid,by coupling with the cathodic CO2reduction *** situ experimental results and theoretical simulations revealed that the catalytic activity center of LAOR was dynamically formed NiOOH species,and the surface-adsorbed SeOxspecies accelerated the formation of Ni3+species,thus promoting catalytic *** mechanism of lactic acid electrooxidation was further *** acid was dehydrogenated to produce pyruvate first and then formed CH3CO due to preferential C-C bond cleavage,resulting in the presence of *** work demonstrated a sustainable method for recycling waste PLA and CO2into high-value-added products.

关键词： Acetic acid Lactic acid electro-oxidation Poly (lactic acid) Waste plastic upcycling

Visible Light-Induced Photocatalysis:Self-Fenton Degradation of p-CIPhOH Over Graphitic Carbon Nitride by a Polyethylenimine Bifunctional Catalyst

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Transactions of Tianjin University 2024年第2期30卷 130-139页

作者： Yuan Bai Shuangjun Li Bolin Yin Jinpeng Zhao Hexing Li Key laboratory of Resource chemistry of Ministry of Education Shanghai Key Laboratory of Rare Earth Functional MaterialsCollege of Chemistry and Materials ScienceShanghai Normal UniversityShanghai 200234China

Deep degradation of organic pollutants by sunlight-induced coupled photocatalytic and Fenton (photo-Fenton) reactions is of immense importance for water purification. In this work, we report a novel bifunctional catalyst (Fe-PEI-CN) by codoping graphitic carbon nitride (CN) with polyethyleneimine ethoxylated (PEI) and Fe species, which demonstrated high activity during p-chlorophenol (p-ClPhOH) degradation via H_(2)O_(2) from the photocatalytic process. The relationship between the catalytic efficiency and the structure was explored using diff erent characterization methods. The Fe modification of CN was achieved through Fe-N coordination, which ensured high dispersion of Fe species and strong stability against leaching during liquid- phase reactions. The Fe modification initiated the Fenton reaction by activating H_(2)O_(2) into ·OH radicals for deep degradation of p-ClPhOH. In addition, it eff ectively promoted light absorption and photoelectron-hole (e-h ^(+) ) separation, corresponding to improved photocatalytic activity. On the other hand, PEI could significantly improve the ability of CN to generate H_(2)O_(2) through visible light photocatalysis. The maximum H_(2)O_(2) yield reached up to 102.6 μmol/L, which was 22 times higher than that of primitive CN. The cooperation of photocatalysis and the self-Fenton reaction has led to high-activity mineralizing organic pollutants with strong durability, indicating good potential for practical application in wastewater treatment.

关键词： Fe-PEI-CN bifunctional catalyst Photo-Fenton p-chlorophenol(p-ClPhOH)degradation Synergetic effect