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Isomeric fluorescence sensors for wide range detection of ionizing radiations

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Defence Technology（防务技术） 2024年第4期34卷 247-257页

作者： Jimin han Tianyu Yang Li Yang Yuanjian Li State Key Laboratory of Explosion Science and Technology of China Beijing Institute of TechnologyBeijing 100081China Chongqing Innovation Center Beijing Institute of TechnologyChongqing 401120China

In order to achieve a wider range of ionizing radiations detection,novel fluorescence sensing materials have been developed that utilize the fluorescence enhancement phenomenon caused by the intramolecular photoinduced electron transfer(PET)*** perylene diimide isomers PDI-P and PDI-B were designed and synthesized,and their molecular structures were characterized by high-resolution Fourier transform mass spectrometry(hRMS),nuclear magnetic resonance hydrogen and carbon spectroscopy(~1h and~(13)C NMR).The interaction between ionizing radiation and fluorescent molecules was simulated by hCl *** results show that combining PDIs and hCl can improve fluorescence through the retro-PET *** the similarities in chemical structures,the fluorescent enhancement multiple of PDI-B with aromatic amine as electron donor is much higher than that of PDI-P with alkyl *** the direct irradiation experiments of ionizing radiation,the emission enhancement multiples of PDI-P and PDI-B are 2.01 and 45.4,***,density functional theory(DFT)and time-dependent density functional theory(TDDFT)calculations indicate that the hOMO and hOMO-1 energy ranges of PDI-P and PDI-B are 0.54 e V and 1.13 e V,respectively.A wider energy range has a stronger driving force on electrons,which is conducive to fluorescence *** femtosecond transient absorption spectroscopy(fs-TAS)and transient fluorescence spectroscopy(TFS)tests show that PDI-B has shorter charge separation lifetime and higher electron transfer rate *** both isomers can significantly reduce LOD during PET process,PDI-B with aromatic amine has a wider detection range of 0.118—240 Gy due to its larger emission enhancement,which is a leap of three orders of *** breaks through the detection range of gamma radiation reported in existing studies,and provides theoretical support for the further study of sensitive and effective new materials for ionizing radiation dete

关键词： Perylene imide Intramolecular PET Ionizing radiation detection Fluorescence sensor Isomers

Origin of water in the Moon

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National Science Review 2024年第6期11卷 10-12页

作者： hejiu hui Ziyan han Kang Shuai State Key Laboratory of Mineral Deposits Research & Lunar and Planetary Science Institute School of Earth Sciences and Engineering Nanjing University CAS Center for Excellence in Comparative Planetology CAS Key Laboratory of Earth and Planetary Physics Institute of Geology and Geophysics

It has been well known since the Apollo era that the Moon is relatively depleted in volatiles as a result of the Moonformation impact and the subsequent planetary differentiation. The lunar interior was believed to have been extremely dry [1]. The discovery of indigenous water (a collective term for h-bearing species Oh, h2O, etc.) in various lunar materials [2–5] has driven a paradigm shift in our knowledge of water in the Moon, from a dry to a wet Moon.

关键词： LUNAR hYDROGEN TERRESTRIAL INTERIOR

Sulfate-assisted Ni/Fe-based electrodes for anion exchange membrane saline splitting

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Nano Research 2024年第7期17卷 5985-5995页

作者： Yujun han Li Shao Yuhang Liu Guodong Li Tongzhou Wang Xuerong Zheng Jihong Li Xiaopeng han Wenbin hu Yida Deng School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin UniversityTianjin 300072China State Key Laboratory of Marine Resource Utilization in South China Sea School of Materials Science and EngineeringHainan UniversityHaikou 570228China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China

Saline water electrolysis is an appealing strategy for hydrogen production,attracting more attention in recent ***-based electrodes exhibit promise as catalysts for saline water ***,they suffer from the inferior service life of the oxygen evolution reaction(OER).herein,we report an oxygen-evolution electrode consisting of a sulfate-modulated nickel-iron hydroxide(NiFeOOh)affording as the catalytic active layer and Fe-Ni_(3)S_(2) as the corrosion-proof *** developed electrode only requires overpotentials of 220 and 292 mV to deliver the current density of 10 and 500 mA·cm^(−2),*** importantly,it presents long-term stability exceeding 140 and 100 h in 1 M KOh at high current densities of 500 and 1000 mA·cm^(−2),respectively,as well as 120 h for saline water electrolysis at 100 mA·cm^(−2).Experimental results reveal that the generated sulfate plays an indispensable role in improving stability and corrosion *** assembled and tested an anion exchange membrane electrolyzer with Pt/C and NiFeS/NIF as the cathode and anode,respectively,under industrial *** overall water-splitting electrolyzer achieves an impressive energy conversion efficiency of 75%±0.5%.This report offers fresh insights into the design of stable NiFe-based electrodes,which may further promote its practical applications for saline water electrolysis.

关键词： saline water electrolysis oxygen evolution reaction anode material water splitting

An unexpected approach to enhance specific surface area and mesopore amount of polyaniline by Zn doping

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Rare Metals 2024年第9期43卷 4585-4594页

作者： Zhi-Da Zhu Yu-Zhe han Xiao-Bi Jing School of Mechanical Engineering Yangzhou UniversityYangzhou 225127China School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China

Poly-p-anisidine could be easily fabricated via the oxidative polymerization reaction of p-anisidine using h_(2)O_(2)as the green *** was unexpectedly found that zinc doping could significantly improve the adsorption ability of the material versus heavy metals such as Pb,Cu,Pd,Ag and *** of nitrogen adsorption–desorption experiments demonstrated that Zn doping could enhance the specific surface area and mesopore amount of the prepared material,which might facilitate its absorption to *** work not only provides a novel material for the treatment of heavy metal-polluted water but also leads to a nice mesoporous catalyst support for environment protection and organic synthesis,*** Zn-doped poly-panisidine can be employed as the catalyst support to prepare Cu@PANI-OMe/Zn or Pd@PANI-OMe/Zn for the oxidative degradation reaction of phenol or Suzuki–Miyaura coupling reactions,*** discloses a new strategy for fabricating the mesoporous polyaniline materials with profound application potential.

关键词： Surfaces Porous materials Rare metal concentration Adsorption Catalysis

Aggregation-regulated bioreduction process of graphene oxide by Shewanella bacteria

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Chinese Journal of Chemical Engineering 2024年第5期69卷 56-62页

作者： Kaixin han Yibo Zeng Yinghua Lu Ping Zeng Liang Shen Department of Chemical and Biochemical Engineering College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Pen-Tung Sah Institute of Micro-Nano Science and Technology Xiamen UniversityXiamen 361005China Chinese Research Academy of Environmental Sciences Beijing 100012China

The bioreduction of graphene oxide(GO)using environmentally functional bacteria such as Shewanella represents a green approach to produce reduced graphene oxide(rGO).This process differs from the chemical reduction that involves instantaneous molecular *** bioreduction,the contact of bacterial cells and GO is considered the rate-limiting *** reveal how the bacteria-GO integration regulates rGO production,the comparative experiments of GO and three Shewanella strains were carried ***-transform infrared spectroscopy,X-ray photoelectron spectroscopy,Raman spectroscopy,and atomic force microscopy were used to characterize the reduction degree and the aggregation *** results showed that a spontaneous aggregation of GO and Shewanella into the condensed entity occurred within 36 h.A positive linear correlation was established,linking three indexes of the aggregation potential,the bacterial reduction ability,and the reduction degree(ID/IG)comprehensively.

关键词： Graphene oxide Reduced graphene oxide Bioreduction Aggregation Shewanella

Electrolyte-gated SrCoO_(x) FET sensor for highly sensitive detecting ph in extreme alkalinity solution

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Nano Research 2024年第4期17卷 3079-3086页

作者： han Zhou Gaocan Qi Wenbin Li Yuhang Wang Zhihao Yuan School of Materials Science and Engineering Tianjin Key Lab of Photoelectric Materials&Devicesand Key Laboratory of Display Materials and Photoelectric Devices(Ministry of Education)Tianjin University of TechnologyTianjin 300384China

The ph monitoring is significantly important in chemical industry,biological process,and pollution ***,it remains a great challenge to measure ph in extreme alkalinity ***,we employ an electrolyte-gated field-effect-transistor(FET)strategy using non-stoichiometric SrCoO_(x) with rich oxygen-vacancy defects as channel materials for detecting extreme *** corresponding channel can provide effective oxygen-ion-migration sites for reversible transformation of Oh-↔O_(2)-+h^(+)driven by electric *** resultant electrolyte-gated FET sensor exhibits a sensitive linear response to high concentrations of alkaline solution,1–20 ***,the sensor has the ability to directly indicate the ph values ranging from 14.0 to 17.0 in consideration of ion-activity coefficient *** work offers a great possibility for directly detecting base concentration as well as ph values in extreme alkaline solutions.

关键词： field-effect-transistor(FET) ph sensor extreme alkaline solution SrCoO_(x) oxygen-ion migration

Evolution Mechanism of Carbon Covalent Bond during Coal Activation Using Mixed Atmosphere of h_(2)O and CO_(2)

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Journal of Thermal Science 2024年第5期33卷 1961-1973页

作者： WANG Mingyue ZhanG Siyuan han Shaobo ZhanG Chi REN Qiangqiang Institute of Engineering Thermophysics Chinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China State Key Laboratory of Coal Conversion Institute of Engineering ThermophysicsChinese Academy of SciencesBeijing 100190China

Adequate destruction of the aromatic structure in coal is key to further reducing the emission of *** this research,activation reactions of Shenmu coal powder were carried out in a vertical tube *** study investigated the evolution mechanism of carbon covalent bonds during the activation process by altering the ratio of h_(2)O to CO_(2)in the activation *** theoretical validation was conducted through density functional *** two gas molecules follow different pathways to increase the reactivity of ***_(2)mainly participates in the cross-linking reaction by intensifying branching,while h_(2)O and char have lower adsorption energy barriers and are more likely to generate oxygen-containing functional *** molecules partially compete for active sites in a mixed gas atmosphere,but there is a synergism between the two *** synergism can be attributed to two *** inclusion of h_(2)O mitigates the generation of five-membered rings to a limited extent,while concurrently enhances the development of oxygen-containing functional *** oxygen-containing functional groups can effectively diminish the adsorption energy barrier associated with the interaction between gas molecules and char,consequently leading to a reduction in the energy demand for subsequent bond cleavage.

关键词： activation reaction carbon structure char CO_(2)/h_(2)O atmosphere density functional theory

hydration lubrication modulated by water structure at TiO2–aqueous interfaces

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Friction 2024年第4期12卷 591-605页

作者： Pingsu MA Yuan LIU Ke han Yu TIAN Liran MA State Key Laboratory of Tribology in Advanced Equipment Department of Mechanical EngineeringTsinghua UniversityBeijing 100084China

The nature of solid-liquid interfaces is of great significance in *** advances have been made in lubrication based on hydration ***,a detailed molecular-level understanding is still ***,we investigated water molecule behaviors at the TiO2-aqueous interfaces by the sum-frequency generation vibrational spectroscopy(SFG-VS)and atomic force microscope(AFM)to elucidate the fundamental role of solid-liquid interfaces in *** contributions of water structures and hydration effects were revealed,where water structures played the dominant role in lubrication for TiO2 surfaces of varying hydrophilicity,while hydration effects dominated with the increasing of ion *** lubrication is observed on the initial TiO2 surfaces with strongly h-bonded water molecules compared to the hydrophilic TiO2 surfaces with more disordered *** stable ordered water arrangement with strong hydrogen bonds and the shear plane occurring between the ordered water layer and subsequent water layer may play a significant role in achieving lower *** adsorbed hydrated molecules with the increasing ionic concentration perturb ordered water but lead to the enhancement of hydration effects,which is the main reason for the improved lubrication for both *** work provides more insights into the detailed molecular-level understanding of the mechanism of hydration lubrication.

关键词： hydration lubrication interfacial water structures hydration effects titanium dioxide(TiO2)

Interplay between geometric and electronic structures of Pt entities over TiO_(2) for CO oxidation

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Science China Chemistry 2024年第2期67卷 705-714页

作者： Xixiong Zhang Wen Shi Shaobo han Yong Li Wenjie Shen School of Chemistry Dalian University of TechnologyDalian116024China State Key Laboratory of Catalysis Dalian Institution of Chemical PhysicsChinese Academy of SciencesDalian116023China

Monodispersed Pt colloids with a mean size of 2 nm were deposited uniformly on the {110} facets of a rod-shaped rutile TiO_(2),forming a well-defined Pt/TiO_(2) *** treatment of this precursor at elevated temperatures re-dispersed the Pt particles into clusters and ***-calcination at 673 K partially oxidized the Pt particle surface,while calcination at 773 K yielded Pt Oxclusters of 1.6 nm in 7–8 atomic *** calcination at 873 K formed a mixture of raft-like PtO_(x) clusters(1.6 nm,1–2 atomic layers) and cationic *** tested for CO oxidation at 373 K,the Pt particles showed a higher activity than the Pt Oxclusters,whereas the cationic single-atoms were much less *** h_(2)-reduction at 473 K converted the partially oxidized Pt particles into the metallic species,but they were encapsulated by TiO_(2)–xoverlayers because of the strong metal–support interactions,which decreased the activity dramatically.h_(2)-reduction of the PtO_(x) clusters at473 K enhanced the fraction of metallic Pt species without changing the size and geometry,and promoted the activity substantially.h_(2)-treatment of Pt single-atoms at 473 K increased the activity only moderately because most Pt species still kept at cationic *** results straightforwardly differentiated the catalytic behavior of Pt particles,clusters and single-atoms at the same metal loading and over the same TiO_(2) support,and further demonstrated that the electronic structures of Pt entities played a decisive role in the catalytic oxidation,in addition to the specified sizes.

关键词： Pt/TiO_(2)catalyst size effect Pt clusters active sites electronic structures CO oxidation