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chemical and engineering bases for green H2O2 production and related oxidation and ammoximation of olefins and analogues

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National science Review 2024年第8期11卷 304-321页

作者： Minghua Qiao Xinggui Zhou Zexue Du Peng Wu Baoning Zong Collaborative Innovation Center of Chemistry for Energy Materials Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University State Key Laboratory of Chemical Engineering East China University of Science and Technology State Key Laboratory of Petroleum Molecular& Process Engineering Research Institute of Petroleum ProcessingSINOPEC State Key Laboratory of Petroleum Molecular& Process Engineering School of Chemistry and Molecular Engineering East China Normal University

Plastics,fibers and rubber are three mainstream synthetic materials that are essential to our daily lives and contribute significantly to the quality of our *** production of the monomers of these synthetic polymers usually involves oxidation or ammoximation reactions of olefins and ***,the utilization of C,O and N atoms in current industrial processes is <80%,which represents the most environmentally polluting processes for the production of basic *** innovation and integration of catalytic materials,new reaction pathways,and reaction engineering,the Research Institute of Petroleum Processing,Sinopec Co.,Ltd.（RIPP） and its collaborators have developed unique H2O2-centered oxidation/ammoximation technologies for olefins and analogues,which has resulted in a ￥500 billion emerging industry and driven trillions of ￥s' worth of downstream *** chemical and engineering bases of the production technologies mainly involve the integration of slurry-bed reactors and microsphere catalysts to enhance H2O2production,H2O2propylene/chloropropylene epoxidation for the production of propylene oxide/epichlorohydrin,and integration of H2O2cyclohexanone ammoximation and membrane separation to innovate the caprolactam production *** review briefly summarizes the whole process from the acquisition of scientific knowledge to the formation of an industrial production technology by ***,the scientific frontiers of H2O2production and related oxidation/ammoximation processes of olefins and analogues are reviewed,and new technological growth points are envisaged,with the aim of maintaining China's standing as a leader in the development of the science and technologies of H2O2production and utilization.

关键词： hydrogen peroxide oxidation ammoximation propylene oxide epichlorohydrin cyclohexanone oxime

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In-situ forming ultra-mechanically sensitive materials for high-sensitivity stretchable fiber strain sensors

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National science Review 2024年第6期11卷 254-263页

作者： Rouhui Yu Changxian Wang Xiangheng Du Xiaowen Bai Yongzhong Tong Huifang Chen Xuemei Sun Jing Yang Naoji Matsuhisa Huisheng Peng Meifang Zhu Shaowu Pan State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and Engineering Donghua University MOE Key Lab of Disaster Forecast and Control in Engineering School of Mechanics and Construction Engineering Jinan University State Key Laboratory of Molecular Engineering of Polymers Department of Macromolecular Science and Institute of Fiber Materials and Devices Fudan University Department of Cardiology Shanghai Xuhui Central HospitalZhongshan-Xuhui Hospital Fudan University Research Center for Advanced Science and Technology and Institute of Industrial Science The University of Tokyo

Fiber electronics with flexible and weavable features can be easily integrated into textiles for wearable applications. However, due to small sizes and curved surfaces of fiber materials, it remains challenging to load robust active layers, thus hindering production of high-sensitivity fiber strain sensors. Herein, functional sensing materials are firmly anchored on the fiber surface in-situ through a hydrolytic condensation *** anchoring sensing layer with robust interfacial adhesion is ultra-mechanically sensitive, which significantly improves the sensitivity of strain sensors due to the easy generation of microcracks during stretching. The resulting stretchable fiber sensors simultaneously possess an ultra-low strain detection limit of 0.05%, a high stretchability of 100%, and a high gauge factor of 433.6, giving 254-folds enhancement in sensitivity. Additionally, these fiber sensors are soft and lightweight, enabling them to be attached onto skin or woven into clothes for recording physiological signals, e.g. pulse wave velocity has been effectively obtained by them. As a demonstration, a fiber sensor-based wearable smart healthcare system is designed to monitor and transmit health status for timely intervention. This work presents an effective strategy for developing high-performance fiber strain sensors as well as other stretchable electronic devices.

关键词： fiber strain sensor stretchable wearable healthcare

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Porphyrin-Grafted Poly(ethylene terephthalate) as a Reusable and Highly Selective Colorimetric Probe for Mercuric Ion Contaminants in Aqueous Samples

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ACS Applied materials and Interfaces 2024年第30期16卷 39195-39205页

作者： Atayde, Eduardo C. Takenaka, Yasumasa Abe, Hideki Wu, Ming-Rou Wu, Kevin C.-W. Molecular Science and Technology Program Taiwan International Graduate Program Academia Sinica Department of Chemistry National Tsing Hua University Department of Chemical Engineering National Taiwan University Bioplastic Research Team RIKEN Center for Sustainable Resource Science Department of Chemical Engineering and Materials Science Yuan Ze University Department of Chemical Engineering Chung Yuan Christian University

Heavy metals are the most hazardous water pollutants, with severe health and environmental consequences. Among these, mercuric (Hg2+) ions are known to cause detrimental health issues in both humans and aquatic life. ... 详细信息

Heavy metals are the most hazardous water pollutants, with severe health and environmental consequences. Among these, mercuric (Hg²⁺) ions are known to cause detrimental health issues in both humans and aquatic life. Due to this, several analytical techniques have been devised to detect and quantify the amount of this ion. However, most of these require advanced instrumentation, prolonged analysis time, and sample preparation. In this study, a low-cost and highly reusable colorimetric probe was developed by grafting porphyrin to poly(ethylene terephthalate) sheets using an oxazoline polymer as covalent adhesive. Upon exposure to trace amounts of Hg²⁺ in solution, the fabricated material visually transitioned from faint brownish pink to green by the complexation mechanism. Additionally, the transparency of this probe allowed the quantitative spectrophotometric determination of the Hg²⁺ concentration in aqueous samples. It was also shown that the material is highly stable, which can be reused for more than 50 times without significant decline in its performance, hence, making it suitable for the onsite monitoring of mercuric ion contamination in different bodies of water. © 2024 The Authors. Published by American chemical Society.

关键词： colorimetric probe mercuric ion oxazoline PET porphyrin

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Interfacial reactions in the Sn-9.0 wt.% Zn/Cu-Ti alloy (C1990 HP) couple

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Soldering and Surface Mount Technology 2024年第1期36卷 30-38页

作者： Laksono, Andromeda Dwi Chen, Chih-Ming Yen, Yee-Wen Department of Materials Science and Engineering National Taiwan University of Science and Technology Taipei Taiwan Department of Chemical Engineering National Chung Hsing University Taichung Taiwan Study Program of Material and Metallurgical Engineering Institut Teknologi Kalimantan Balikpapan Indonesia

Purpose: The purpose of this study was to examine the influence of adding a small amount of Ti to a Cu-based alloy, specifically the commercial Hyper Titanium Copper alloy (C1990 HP), which contains Cu-3.28 wt.% Ti, on its interfacial reaction with Sn-9.0 wt.% Zn (SnZn) solder, using the liquid/solid reaction couple technique. Design/methodology/approach: The SnZn/C1990 HP couples were subjected to a reaction temperature of 240–270°C for a duration of 0.5–5 h. The resulting reaction couple was characterized using a scanning electron microscope, energy dispersive spectrometer, electron probe microanalyzer and X-ray diffractometer. Findings: It was observed that the scallop-shaped CuZn5 and planar Cu5Zn8 phases were formed in almost all SnZn/C1990 HP couples. With increased reaction duration and temperature, the Cu-rich intermetallic compound (IMC)-Cu5Zn8 phase became a dominant IMC formed at the interface. The total thickness of the IMCs was increased with the increase in the reaction duration and temperature. The IMC growth obeyed the parabolic law, and the IMC growth mechanism was diffusion controlled. The activation energy of the SnZn/C1990 HP couple was 64.71 kJ/mol. Originality/value: This article presents an analysis of the IMC thickness in each sample using ImageJ software, followed by kinetic analysis using Origin software at various reaction temperatures of SnZn/C1990 HP in liquid/solid couples. The study also includes detailed reports on the morphology, interface composition and X-ray diffraction analysis, as well as the activation energy. The findings can serve as a valuable reference for electronic packaging companies that utilize C1990 HP substrates. © 2023, Emerald Publishing Limited.

关键词： Binary alloys

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Rechargeable Multivalent-Ion Batteries

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Energy Material Advances 2024年第1期5卷 283-284页

作者： Juchen Guo Jennifer LSchaefer Yuyan Shao Department of Chemical and Environmental Engineering Materials Science and Engineering ProgramUniversity of CaliforniaRiversideRiversideCA 92521USA Department of Chemical and Biomolecular Engineering University of Notre DameNotre DameIN 46556USA Pacific Northwest National Laboratory RichlandWA 99352USA

Rechargeable batteries based on multivalent metal anodes including earth-abundant magnesium(Mg),calcium(Ca),zinc(Zn),and aluminum(Al)are potential new“beyond lithium(Li)”electrochemical energy storage technologies for large-scale energy storage *** multivalent elements are more earth abundant,and therefore promising candidates for reducing global dependence on Li for our growing energy storage *** the seminal work by Aurbach and coworkers[1]demonstrating the first prototype rechargeable Mg batteries,tremendous efforts have been made to the research and development of rechargeable multivalent-ion batteries.

关键词： energy storage calcium batteries rechargeable batteries multivalent elements multivalent metal anodes energy storage technologies magnesium batteries

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Efficient predictions of formation energies and convex hulls from density functional tight binding calculations

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Journal of materials science & Technology 2023年第10期141卷 236-244页

作者： Anshuman Kumar Zulfikhar A.Ali Bryan M.Wong Materials Science&Engineering Program University of California-RiversideRiverside92521CAUSA Department of Physics&Astronomy University of California-RiversideRiverside92521CAUSA Materials Science&Engineering Program Department of Chemical&Environmental EngineeringDepartment of Physics&Astronomyand Department of ChemistryUniversity of California-RiversideRiverside92521CAUSA

Defects in materials significantly alter their electronic and structural properties,which affect the per-formance of electronic devices,structural alloys,and functional ***,calculating all the possible defects in complex materials with conventional Density Functional Theory(DFT)can be compu-tationally *** enhance the efficiency of these calculations,we interfaced Density Functional Tight Binding(DFTB)with the Clusters Approach to Statistical Mechanics(CASM)software package for the first *** SiC and ZnO as representative examples,we show that DFTB gives accurate results and can be used as an efficient computational approach for calculating and pre-screening formation ener-gies/convex *** DFTB+CASM implementation allows for an efficient exploration(up to an order of magnitude faster than DFT)of formation energies and convex hulls,which researchers can use to probe other complex systems.

关键词： CASM DFTB DFT Formation energy Convex hull

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Recent advances on the systems metabolically engineered Pseudomonas species as versatile biosynthetic platforms for the production of polyhydroxyalkanoates

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Systems Microbiology and Biomanufacturing 2024年第2期4卷 473-499页

作者： Hye Min Song Seo Young Jo Haeyoung Lee Subeen Jeon Dohye Yun Chaerin Kim Jina Son Yu Jung Sohn Jong-Il Choi Si Jae Park Department of Chemical Engineering and Materials Science Graduate Program in System Health Science and EngineeringEwha Womans UniversitySeoul 03760Republic of Korea Department of Biotechnology and Bioengineering Chonnam National UniversityGwangju 61186Republic of Korea

Pseudomonas *** been considered one of the most promising microbial platform strains due to its versatile metabolism,enabling the valorization of waste materials into value-added chemical *** the native producer of polyhydroxyal-kanoates(PHAs),the biodegradable biopolyesters,it has been widely engineered by various metabolic engineering tools for the production of PHAs composed of short-chain-length and medium-chain-length monomers with adjustable composition from diverse carbon sources,ranging from pure sugars to crude oils and fatty *** review discusses the feasibility of Pseudomonas *** the industrial host strain and the recent advances regarding the systems metabolic engineering strategies for PHAs production in Pseudomonas sp.

关键词： Pseudomonas sp. Polyhydroxyalkanoates Systems metabolic engineering Synthetic biology Fermentation

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Oxidation Evolution and Activity Origin of N-Doped Carbon in the Oxygen Reduction Reaction

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Transactions of Tianjin University 2024年第4期30卷 369-379页

作者： Jiaqi Wu Chuanqi Cheng Shanshan Lu Bin Zhang Yanmei Shi Department of Chemistry School of ScienceInstitute of Molecular PlusTianjin UniversityTianjin 300072China School of Materials Science and Engineering Institute of New Energy MaterialsTianjin UniversityTianjin 300072China Tianjin Key Laboratory of Molecular Optoelectronic Science Collaborative Innovation Center of Chemical Science and EngineeringTianjin 300072China

N-doped carbon materials,with their applications as electrocatalysts for the oxygen reduction reaction(ORR),have been extensively ***,a negletcted fact is that the operating potential of the ORR is higher than the theoretical oxida-tion potential of carbon,possibly leading to the oxidation of carbon ***,the infl uence of the structural oxidation evolution on ORR performance and the real active sites are not *** this study,we discover a two-step oxida-tion process of N-doped carbon during the *** fi rst oxidation process is caused by the applied potential and bubbling oxygen during the ORR,leading to the oxidative dissolution of N and the formation of abundant oxygen-containing functional *** oxidation process also converts the reaction path from the four-electron(4e)ORR to the two-electron(2e)***,the enhanced 2e ORR generates oxidative H_(2)O_(2),which initiates the second stage of oxidation to some newly formed oxygen-containing functional groups,such as quinones to dicarboxyls,further diversifying the oxygen-containing functional groups and making carboxyl groups as the dominant *** also reveal the synergistic eff ect of multiple oxygen-containing functional groups by providing additional opportunities to access active sites with optimized adsorption of OOH*,thus leading to high effi ciency and durability in electrocatalytic H_(2)O_(2) production.

关键词： Oxygen reduction reaction N-doped carbon Reaction path Structural evolution Oxidation in reduction

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Surface-modified Ag@Ru-P25 for photocatalytic CO_(2) conversion with high selectivity over CH_(4) formation at the solid–gas interface

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Carbon Energy 2024年第1期6卷 182-196页

作者： Chaitanya B.Hiragond Sohag Biswas Niket SPowar Junho Lee Eunhee Gong Hwapyong Kim Hong Soo Kim Jin-Woo Jung Chang-Hee Cho Bryan M.Wong Su-Il In Department of Energy Science&Engineering Daegu Gyeongbuk Institute of Science and Technology(DGIST)DaeguRepublic of Korea Department of Chemical&Environmental Engineering Materials Science&Engineering ProgramDepartment of ChemistryDepartment of Physics&AstronomyUniversity of California-RiversideRiversideCaliforniaUSA Department of Physics and Chemistry Daegu Gyeongbuk Institute of Science and Technology(DGIST)DaeguRepublic of Korea NiceScience Corporation DaeguRepublic of Korea

Systematic optimization of the photocatalyst and investigation of the role of each component is important to maximizing catalytic activity and comprehending the photocatalytic conversion of CO_(2) reduction to solar fuels.A surface-modified Ag@Ru-P25 photocatalyst with H_(2)O_(2) treatment was designed in this study to convert CO_(2) and H_(2)O vapor into highly selective *** doping followed by Ag nanoparticles(NPs)cocatalyst deposition on P25(TiO_(2))enhances visible light absorption and charge separation,whereas H_(2)O_(2) treatment modifies the surface of the photocatalyst with hydroxyl(–OH)groups and promotes CO_(2) ***-resonance transmission electron microscopy,X-ray photoelectron spectroscopy,X-ray absorption near-edge structure,and extended X-ray absorption fine structure techniques were used to analyze the surface and chemical composition of the photocatalyst,while thermogravimetric analysis,CO_(2) adsorption isotherm,and temperature programmed desorption study were performed to examine the significance of H_(2)O_(2) treatment in increasing CO_(2) reduction *** optimized Ag1.0@Ru1.0-P25 photocatalyst performed excellent CO_(2) reduction activity into CO,CH4,and C2H6 with a~95%selectivity of CH4,where the activity was~135 times higher than that of pristine TiO_(2)(P25).For the first time,this work explored the effect of H_(2)O_(2) treatment on the photocatalyst that dramatically increases CO_(2) reduction activity.

关键词： gas-phase CO_(2) reduction H_(2)O_(2) treatment plasmonic nanoparticles solar fuel photocatalyst surface modification

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Pd/N-doped carbon dots@dendritic mesoporous silica nanospheres:A highly efficient catalyst for the hydrogenation of 4-nitrophenol

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Nano Research 2024年第9期17卷 7967-7974页

作者： Weiruo Liu Yanbin Zhu Jiwei Wang Haisong Feng Yunpu Zhai Wei Li Dongyuan Zhao College of Chemistry Zhengzhou University100 Kexue AvenueZhengzhou 450001China Department of Chemistry Laboratory of Advanced MaterialsShanghai Key Laboratory of Molecular Catalysis and Innovative Materialsand State Key Laboratory of Molecular Engineering of PolymersFudan UniversityShanghai 200433China State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Highly dispersed Pd/N-doped carbon dots(Pd/NCDs)were successfully immobilized in the mesoporous channels of amino-functionalized dendritic mesoporous silica nanospheres(NMS).The synthesized Pd/NCDs@NMS catalyst exhibits outstanding performance in the catalytic reduction of 4-nitrophenol(4-NP),achieving a turnover frequency of 1461.8 mol·molPd^(-1)·h^(-1),with the conversion rate remaining above 80%after 11 *** and density functional theory calculations reveal that the NCDs significantly affect the electronic structure of Pd nanoparticles,leading to changes in the energy barriers for the adsorption of 4-NP at the Pd sites and the conversion of 4-NP reaction intermediates,which is a key factor contributing to the catalytic *** study offers a new strategy for synthesizing carbon-dot-modified metal-based catalysts.

关键词： palladium nanoparticles nitrogen-doped carbon dots dendritic mesoporous silica catalytic hydrogenation 4-nitrophenol reduction

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