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Subnanometric bimetallic Pt-Pd clusters in zeolites for efficient hydrogen production and selective tandem hydrogenation of nitroarenes

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Science China Chemistry 2024年第9期67卷 2911-2917页

作者： Jiafu Li Tao Cai Yanran Feng Xia liu Ning Wang Qiming sun Institute of Sustainable Energy and Resources College of Chemistry and Chemical EngineeringKey Laboratory of Shandong Provincial Universities for Functional Molecules and MaterialsQingdao UniversityQingdao 266071China Innovation Center for Chemical Sciences College of ChemistryChemical Engineering and Materials ScienceJiangsu Key Laboratory of Advanced Negative Carbon TechnologiesSoochow UniversitySuzhou 215123China

The solvolysis of ammonia borane(AB)and the hydrogenation of nitroarenes represent significant reactions for hydrogen generation and value-added chemical *** strategic engineering of the catalysts is imperative for surmounting obstacles associated with their stability and catalytic *** this work,subnanometric bimetallic Pt–Pd clusters were encapsulated within silicalite-1(S-1)zeolites through a ligand-protected in-situ hydrothermal synthesis *** synergetic effect of bimetallic composition and zeolite confinement markedly enhances the catalytic performance of representative Pt_(0.5)Pd_(0.5)@S-1-H catalyst,affording exceptional turnover frequency(TOF)values of 1,043 and 573 mol_(H_(2))mol_(metal)^(-1)min^(-1)for AB hydrolysis and methanolysis at ambient conditions,respectively,surpassing most of the state-of-the-art Pt-based *** and isotopic experiments reveal that the bimetallic catalytic system remarkably boosts the O-H cleavage of water,thereby facilitating the H_(2) production from AB ***,a conspicuous synergistic effect is demonstrated in the shape-selective tandem hydrogenation of nitroarenes,with the bimetallic catalyst facilitating both AB hydrolysis and nitroarene hydrogenation,giving a high TOF value of 1,260 h^(-1)under atmospheric *** study not only demonstrates the effectiveness of bimetallic nanocatalysts encapsulated in zeolites for hydrogen production from chemical hydrogen storage materials,but also paves the way for the design of catalysts with multifunctional active sites capable of synergistically promoting tandem catalytic processes.

关键词： subnanometer bimetallic cluster zeolite synergistic effect ammonia borane solvolysis selective tandem hydrogenation

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Micro-sized nanoaggregates:Spray-drying-assisted fabrication and applications

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Particuology 2024年第2期85卷 22-48页

作者： Dan-Lei Yang Rong-Kun liu Yan Wei Qian sun Jie-Xin Wang School of Life Sciences and Chemical Engineering Jiangsu Second Normal UniversityNanjing210013China State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing100029China Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology School of Chemistry and Chemical EngineeringGuangxi UniversityNanning530004China

The applications of nanoparticles suffer from their extremely small size and intrinsic trend of *** nanoparticles to form micro-sized nanoaggregates(MNAs)with increased size,ordered structure,as well as controllable size,shape,and morphology is a crucial step in various fields of science and technology to maintain the unique characteristics of nanoparticles while obtaining greatly enhanced or new performance at the *** structure of MNAs prominently affects their functionality,which is determined by the arrangement of nanoparticles and the interaction between primary *** methods have been proposed to prepare the MNAs,in which spray-drying technology stands out considering the feasibility,scalability for industry,cost,and *** assembly of nanoparticles through spray-drying under tunable process parameters yields diverse physical properties and structural arrangements of nanoparticles of the MNAs,they therefore exhibit enormous potential in a wide range of application *** review presents the construction and applications of spray-dried *** factors that influence the size,morphology,and structure of the MNAs are discussed in *** addition,the outstanding application performance resulting from the tightly packed nanoparticles in regular-shaped MNAs obtained by the spray-drying process is illustrated.

关键词： Spray-drying Micro-sized nanoaggregates Applications

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Hydroxyl radical production by abiotic oxidation of pyrite under estuarine conditions:The effects of aging,seawater anions and illumination

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Journal of Environmental Sciences 2024年第1期135卷 715-727页

作者： Ruixue liu Yinshun Dai Yucheng Feng Shiwen sun Xiaodong Zhang Chunjiang An Shan Zhao Shandong Key Laboratory of Water Pollution Control and Resource Reuse School of Environmental Science and EngineeringShandong UniversityQingdao 266237China Department of Building Civil and Environmental EngineeringConcordia UniversityMontrealQC H3G 1M8Canada

Pyrite is widely distributed in estuarine sediments as an inexpensive natural Fenton-like reagent,however,the mechanism on the hydroxyl radical(HO^(·))production by pyrite under estuarine environmental conditions is still poorly *** batch experiments were performed to investigate the effects of estuarine conditions including aging(in air,in water),seawater anions(Cl^(-),Br^(-)and HCO_(3)^(-))and light on the HO^(·)production by pyrite *** one-electron transfer dominated the process from O_(2) to HO^(·)induced by oxidation of *** Fe(oxyhydr)oxide coatings on the surface of pyrite aged in air and water consumed hydrogen peroxide while mediating the electron transfer,and the combined effect of the two resulted in a suppression of HO^(·)production in the early stage of aging and a promotion of HO^(·)production in the later stage of *** of the surface oxide layers by aggressive anions was the main reason for the inhibition of HO^(·)production by Cl^(-)and Br^(-),and the generation of Cl^(·)and Br^(·)may also play a role in the scavenging of HO^(·).HCO_(3)^(-)increased the average rate of HO^(·)production through surface-CO_(2) complexes formed by adsorption on the surface of *** significant enhancement of HO^(·)production under light was attributed to the formation of photoelectrons induced by photochemical reactions on pyrite and its surface oxide *** findings provide new insights into the environmental chemical behavior of pyrite in the estuary and enrich the understanding of natural remediation of estuarine environments.

关键词： Hydroxyl radical Pyrite oxidation Aging Anions Irradiation

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Effective protective agents against the organ toxicity of T-2 toxin and corresponding detoxification mechanisms:A narrative review

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Animal Nutrition 2024年第1期16卷 251-266页

作者： Pengju Wang Lv-hui sun Xu Wang Qinghua Wu Aimei liu Hubei Key Laboratory of Diabetes and Angiopathy Medicine Research InstituteXianning Medical CollegeHubei University of Science and TechnologyXianning 437100China Hubei Hongshan Laboratory College of Animal Science and TechnologyHuazhong Agricultural UniversityWuhan430070China National Reference Laboratory of Veterinary Drug Residues(HZAU)and MAO Key Laboratory for Detection of Veterinary Drug Residues Huazhong Agricultural UniversityWuhan430070China College of Life Science Yangtze UniversityJingzhou 434025China

T-2 toxin is one of the most widespread and toxic fungal toxins in food and *** can cause gastrointestinal toxicity,hepatotoxicity,immunotoxicity,reproductive toxicity,neurotoxicity,and nephrotoxicity in humans and animals.T-2 toxin is physicochemically stable and does not readily degrade during food and feed ***,suppressing T-2 toxin-induced organ toxicity through antidotes is an urgent *** agents against the organ toxicity of T-2 toxin have been recorded widely in the literature,but these protective agents and their molecular mechanisms of detoxification have not been comprehensively *** this review,we provide an overview of the various protective agents to T-2 toxin and the molecular mechanisms underlying the detoxification *** appropriate targets to antagonize T-2 toxin toxicity is also an important *** review will provide essential guidance and strategies for the better application and development of T-2 toxin antidotes specific for organ toxicity in the future.

关键词： T-2 toxin Organ toxicity Protective agent Detoxification mechanism

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Analytical solutions of equatorial geodesic motion in Kerr spacetime

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Chinese Physics C 2024年第4期48卷 222-239页

作者：刘岩孙兵 Department of Physics Yantai UniversityYantai 264005China Department of Basic Courses Beijing University of AgricultureBeijing 102206China CAS Key Laboratory of Theoretical Physics Institute of Theoretical PhysicsChinese Academy of SciencesBeijing 100190China

The study of Kerr geodesics has a long history,particularly for those occurring within the equatorial plane,which are generally ***,when compared with the classification introduced by one of the authors[***.D 105,024075(2022)],it becomes apparent that certain classes of geodesics,such as trapped orbits,still lack analytical ***,in this study,we provide explicit analytical solutions for equatorial timelike geodesics in Kerr spacetime,including solutions of trapped orbits,which capture the characteristics of special geodesics,such as the positions and conserved quantities of circular,bound,and deflecting ***,we determine the precise location at which retrograde orbits undergo a transition from counter-rotating to prograde motion due to the strong gravitational effects near a rotating black ***,the trajectory remains prograde for orbits with negative energy despite the negative angular ***,we investigate the intriguing phenomenon of deflecting orbits exhibiting an increased number of revolutions around the black hole as the turning point approaches the turning point of the trapped ***,we find that only prograde marginal deflecting geodesics are capable of traversing through the *** summary,our findings present explicit solutions for equatorial timelike geodesics and offer insights into the dynamics of particle motion in the vicinity of a rotating black hole.

关键词： geodesic motion analytical solutions equatorial plane Kerr spacetime

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Photo-Responsive Carbon Capture over Metalloporphyrin-C_(60) Metal-Organic Frameworks via Charge-Transfer

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Research 2024年第3期2023卷 233-241页

作者： Shi-Chao Qi Zhen sun Zhi-Hui Yang Yun-Jie Zhao Jia-Xin Li Xiao-Qin liu Lin-Bing sun State Key Laboratory of Materials-Oriented Chemical Engineering Jiangsu National Synergetic Innovation Center for Advanced Materials(SICAM)College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China.

Great efforts have been devoted to the study of photo-responsive adsorption,but its current methodology largely depends on the well-defined photochromic units and their photo-driven molecular ***,a methodology to fabricate nondeforming photo-responsive sorbents is successfully *** C_(60)-fullerene doping in metalloporphyrin metal-organic frameworks(PCN-M,M=Fe,Co,or Ni)and intensively interacting with the metalloporphyrin sites,effective charge-transfer can be achieved over the metalloporphyrin-C_(60) architectures once excited by the light at 350 to 780 *** electron density distribution and the resultant adsorption activity are thus changed by excited states,which are also stable enough to meet the timescale of microscopic adsorption *** charge-transfer over Co(II)-porphyrin-C_(60) is proved to be more efficient than the Fe(II)-and Ni(II)-porphyrin-C_(60) sites,as well as than all the metalloporphyrin sites,so the CO_(2) adsorption capacity(CAC;at 0°C and 1 bar)over the C_(60)-doped PCN-Co can be largely improved from 2.05 mmol g^(−1) in the darkness to 2.69 mmol g−1 with light,increased by 31%,in contrast to photo-irresponsive CAC over all C_(60)-undoped PCN-M sorbents and only the photo-loss CAC over C_(60).

关键词： porphyrin adsorption excited

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Fast-Charging Sodium-Ion Batteries Enabled by Molecular-Level Designed Nitrogen and Phosphorus Codoped Mesoporous Soft Carbon

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Research 2024年第2期2023卷 329-337页

作者： Lei liu Zhuzhu Du Jiaqi Wang Hongfang Du Sheng Wu Mengjun Li Yixuan Zhang Jinmeng sun Zhipeng sun Wei Ai Frontiers Science Center for Flexible Electronics(FSCFE)and Shaanxi Institute of Flexible Electronics(SIFE) Northwestern Polytechnical University(NPU)127 West Youyi RoadXi'an 710072China Fujian Cross Strait Institute of Flexible Electronics(Future Technologies) Fujian Normal UniversityFuzhou 350117China School of Materials and Energy Guangdong University of TechnologyGuangzhou510006 GuangdongChina

Soft carbons have attracted extensive interests as competitive anodes for fast-charging sodium-ion batteries(SIBs);however,the high-rate performance is still restricted by their large ion migration barriers and sluggish reaction ***,we show a molecular design approach toward the fabrication of nitrogen and phosphorus codoped mesoporous soft carbon(NPSC).The key to this strategy lies in the chemical cross-linking reaction between polyphosphoric acid and p-phenylenediamine,associated with pyrolysis induced in-situ self-activation that creates mesoporous structures and rich heteroatoms within the carbon *** to the enlarged interlayer spacing,reduced ion diffusion length,and plentiful active sites,the obtained NPSC delivers a superb rate capacity of 215 mAh g-1 at 10 A g-1 and an ultralong cycle life of 4,700 cycles at 5 A g^(-1).Remarkably,the full cell shows 99%capacity retention during 100 continuous cycles,and maximum energy and power densities of 191 Wh kg^(-1)and 9.2 kW kg^(-1),*** believe that such a synthetic protocol could pave a novel venue to develop soft carbons with unique properties for advanced SIBs.

关键词： kinetics carbons linking

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Current Status and Perspectives of Dual-Atom Catalysts Towards Sustainable Energy Utilization

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Nano-Micro Letters 2024年第7期16卷 402-440页

作者： Yizhe Li Yajie Li Hao sun Liyao Gao Xiangrong Jin Yaping Li Zhi LV Lijun Xu Wen liu Xiaoming sun State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science EngineeringCollege of ChemistryBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China Xinjiang Coal Mine Mechanical and Electrical Engineering Technology Research Center Xinjiang Institute of EngineeringUrumqi 830023Xinjiang Uygur Autonomous RegionPeople’s Republic of China

The exploration of sustainable energy utilization requires the imple-mentation of advanced electrochemical devices for efficient energy conversion and storage,which are enabled by the usage of cost-effective,high-performance ***,heterogeneous atomically dispersed catalysts are considered as potential candidates for a wide range of *** to conventional cata-lysts,atomically dispersed metal atoms in carbon-based catalysts have more unsatu-rated coordination sites,quantum size effect,and strong metal-support interactions,resulting in exceptional catalytic *** these,dual-atomic catalysts(DACs)have attracted extensive attention due to the additional synergistic effect between two adja-cent metal *** have the advantages of full active site exposure,high selectiv-ity,theoretical 100%atom utilization,and the ability to break the scaling relationship of adsorption free energy on active *** this review,we summarize recent research advancement of DACs,which includes(1)the comprehensive understanding of the synergy between atomic pairs;(2)the synthesis of DACs;(3)characterization meth-ods,especially aberration-corrected scanning transmission electron microscopy and synchrotron spectroscopy;and(4)electrochemical energy-related *** last part focuses on great potential for the electrochemical catalysis of energy-related small molecules,such as oxygen reduction reaction,CO_(2) reduction reaction,hydrogen evolution reaction,and N_(2) reduction *** future research challenges and opportunities are also raised in prospective section.

关键词： Dual-atom catalysts Synergetic effect Electrocatalysis Oxygen reduction reaction CO_(2)reduction reaction Hydrogen evolution reaction N2 reduction reaction

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Development of an automatic measurement system using atmospheric pressure photoionization ultrahigh-resolution mass spectrometry and application for on-line analysis of particulate matter

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Journal of Environmental Sciences 2024年第4期138卷 516-530页

作者： Yayuan Dong Ranran liu Ling Xie Xiaole Pan Yele sun Lin Wu ZifaWang State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China College of Earth and Planetary Sciences University of Chinese Academy of SciencesBeijing 100049China Center for Excellence in Regional Atmospheric Environment Chinese Academy of SciencesInstitute of Urban EnvironmentXiamen 361021China

On-line chemical characterization of atmospheric particulate matter(PM)with soft ionization technique and ultrahigh-resolution Mass Spectrometry(UHRMS)provides molecular information of organic constituents in real *** we describe the development and application of an automatic measurement system that incorporates PM_(2.5)sampling,thermal desorption,atmospheric pressure photoionization,and UHRMS *** formulas of detected organic compounds were deducted from the accurate(±10 ppm)molecular weights obtained at a mass resolution of 100,000,allowing the identification of small organic compounds in PM_(2.5).Detection efficiencies of 28 standard compounds were determined and we found a high sensitivity and selectivity towards organic amines with limits of detection below 10 *** a proof of principle,PM_(2.5)samples collected off-line in winter in the urban area of Beijing were analyzed using the Ionization Module and HRMS of the *** automatic system was then applied to conduct on-line measurements during the summer time at a time resolution of 2 *** detected organic compounds comprised mainly CHON and CHN compounds below 350 m/*** seasonal variations in elemental composition were observed with shorter carbon backbones and higher O/C ratios in summer than that in *** result is consistent with stronger photochemical reactions and thus a higher oxidation state of organics in *** variation in signal intensity of each formula provides crucial information to reveal its source and formation *** summary,the automatic measurement system serves as an important tool for the on-line characterization and identification of organic species in PM_(2.5).

关键词： PM_(2.5) Chemical composition On-line measurement technique High resolution mass spectrometry

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In situ reconstruction induced oxygen-deficient multiphase Cu based species hybridized with Ni single atoms as tandem platform for CO_(2) electroreduction

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Nano Research 2024年第5期17卷 3888-3894页

作者： Juzhe liu Yuheng Wang Pengpeng Mo Feng Yang Kaiqi Jiang Zhixiang Cheng Yuxuan liu Zhiyi sun Zheng liu Yimei Zhang Wenxing Chen The Key Laboratory of Resources and Environmental System Optimization Ministry of EducationCollege of Environmental Science and EngineeringNorth China Electric Power UniversityBeijing 102206China Energy&Catalysis Center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 100012China SEPA Key Laboratory of Eco-Industry Chinese Research Academy of Environmental SciencesBeijing 100012China

Tandem catalysis,capable of decoupling individual steps,provides a feasible way to build a high-efficiency CO_(2) electro-conversion system for multicarbons(C_(2+)).The construction of electrocatalytic materials is one of focusing ***,we fabricated a single atom involved multivalent oxide-derived Cu composite material and found it inclined to reconstruct into oxygen-deficient multiphase Cu based species hybridized with monatomic Ni on N doped C *** this prototype,rapid CO generation and C-C coupling are successively achieved on NiN4 sites and surface amorphized Cu species with defects,resembling a micro-production *** this way,the in situ formed tandem catalyst exhibited a high Faradaic efficiency(FE)of~78%for C_(2+)products along with satisfactory durability over 50 ***,the reconstruction-induced amorphous layer with abundant asymmetric sites should be favorable to improve the ethanol selectivity(FE:63%),which is about 10 times higher than that of the non-tandem Cu-based contrast *** work offers a new approach for manipulating tandem catalyst systems towards enhancing C_(2+)products.

关键词： tandem catalysis single atom reconstruction amorphous CO_(2)reduction reaction

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