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Peroxidase-like active Cu-ZIF-8 with rich copper(I)-nitrogen sites for excellent antibacterial performances toward drug-resistant bacteria

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Nano Research 2024年第8期17卷 7427-7435页

作者： Xiaoze Wang Hui Wang Jingkun Zhang Ning Han Wenjun Ma Donghai Zhang Mingshui Yao Xianliang Wang yunfa chen State Key Laboratory of Mesoscience and Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China University of the Chinese Academy of Sciences Beijing 100049China Laboratory of Theoretical and Computational Nanoscience CAS Key Laboratory of Nanosystem and Hierarchial FabricationCAS Center for Excellence in NanoscienceNational Center for Nanoscience and TechnologyBeijing 100190China China CDC Key Laboratory of Environment and Population Health National Institute of Environmental HealthChinese Center for Disease Control and PreventionBeijing 100021China

Bacterial pathogens pose a serious threat to human health,and there is an urgent need to develop highly effective antibacterial materials to eliminate the increasingly serious contamination of drug-resistant ***,a Cu-doped ZIF-8 particle with unsaturated copper exhibits high peroxidase-like activity.99.998%antibacterial efficiency against *** can be achieved for 30 min at a low concentration of 50μg·mL^(−1),as well as complete sterilization against ***(up to 8 log).99.999%antibacterial efficiency against Methicillin-resistant Staphylococcus aureus can be achieved,performing orders of magnitude higher than *** mechanism shows that the unsaturated Cu-Nx sites are enzyme-like active centers,which could promote the consumption of bacteria reducing substances by H_(2)O_(2),and the generated*OH further aggravates bacterial oxidative stress and membrane *** importantly,the oxidation activity of adsorbed oxygen species on Cu-ZIF-8 is enhanced by charge transfer and structural changes between the ligand and copper center like natural ***-doped ZIF-8 with peroxidase-like activity shows great potential in antibacterial application and the revealed catalytic mechanism is helpful for understanding the high antibacterial activity of nanoparticles with Cu-Nx sites.

关键词： Cu-doped ZIF-8 peroxidase-like reactive oxygen species(ROS) catalytic mechanism antibacterial activity

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Balancing electron transfer and intermediate adsorption ability of metallic Ni-Fe-RE-P bifunctional catalysts via 4f-2p-3d electron interaction for enhanced water splitting

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Journal of Energy Chemistry 2024年第7期94卷 458-465页

作者： Hong-Rui Zhao cheng-Zong Yuan chenliang Zhou Wenkai Zhao Lunliang Zhang Cong-Hui Li Lei Xin Fuling Wu Shufeng Ye Xiaomeng Zhang yunfa chen School of Rare Earths University of Science and Technology of ChinaHefei 230026AnhuiChina Jiangxi Province Research Institute of Rare Earths Ganjiang Innovation AcademyChinese Academy of SciencesGanzhou 341119JiangxiChina State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

Balancing electron transfer and intermediate adsorption ability of bifunctional catalysts via tailoring electronic structures is crucial for green hydrogen production,while it still remains challenging due to lacking efficient ***,one efficient and universal strategy is developed to greatly regulate electronic structures of the metallic Ni-Fe-P catalysts via in-situ introducing the rare earth(RE)atoms(Ni-Fe-RE-P,RE=La,Ce,Pr,and Nd).Accordingly,the as-prepared optimal Ni-Fe-Ce-P/CC self-supported bifunctional electrodes exhibited superior electrocatalytic activity and excellent stability with the low overpotentials of 247 and 331 mV at 100 mA cm^(-2) for HER and OER,*** the assembled electrolyzer,the Ni-Fe-Ce-P/CC as bifunctional electrodes displayed low operation potential of 1.49 V to achieve a current density of 10 mA cm^(-2),and the catalytic performance can be maintained for 100 *** results combined with density functional theory(DFT)calculation reveal that Ce doping leads to electron decentralization and crystal structure distortion,which can tailor the band structures and d-band center of Ni-Fe-P,further increasing conductivity and optimizing intermediate adsorption *** work not only proposes a valuable strategy to regulate the electron transfer and intermediate adsorption of electrocatalysts via RE atoms doping,but also provides a deep under-standing of regulation mechanism of metallic electrocatalysts for enhanced water splitting.

关键词： RE atoms Electron transfer Adsorption energy Oxygen evolution Hydrogen evolution

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Heterojunctioned CuO/Cu_(2)O catalyst for highly efficient ozone removal

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Journal of Environmental Sciences 2023年第3期125卷 340-348页

作者： Guojun Ma Wenxiang Tang AnqiWang Le Zhang Jian Guan Ning Han yunfa chen Key Laboratory of Science and Technology on Particle Materials Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Center for Excellence in Regional Atmospheric Environment Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical Engineering Sichuan UniversityChengdu 610065China

In recent years, near surface ozone pollution, has attracted more and more attention,which necessitates the development of high efficient and low cost catalysts. In this work,Cu O/Cu_(2)O heterojunctioned catalyst is fabricated by heating Cu_(2)O at high temperature, and is adopted as ozone decomposition catalyst. The results show that after Cu_(2)O is heated at180℃conversion of ozone increases from 75.2% to 89.3% at mass space velocity 1,920,000cm^(3)/(g·hr) in dry air with 1000 ppm V ozone, which indicates that this heterojunction catalyst is one of the most efficient catalysts reported at present. Catalysts are characterized by electron paramagnetic resonance spectroscopy and ultraviolet photoelectron spectroscopy,which confirmed that the heterojunction promotes the electron transfer in the catalytic process and creates more defects and oxygen vacancies in the Cu O/Cu_(2)O interfaces. This procedure of manufacturing heterostructures would also be applicable to other metal oxide catalysts, and it is expected to be more widely applied to the synthesis of high-efficiency heterostructured catalysts in the future.

关键词： Cu_(2)O Ozone decomposition CuO Heterojunction

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化工冶金跨行业耦合二氧化碳循环利用技术

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洁净煤技术 2024年第4期30卷 171-178页

作者：李双德李振荣董笑陈为刘一凡李少鹏程景才李会泉陈运法中国科学院过程工程研究所北京100190 中国科学院大学北京100049 中国科学院山西煤炭化学研究所山西太原030001 中国科学院上海高等研究院上海201210

双碳战略是国家重大战略,也是推动国家经济高质量可持续发展的必由之路。我国碳达峰到碳中和时间短、任务重。我国化工冶金每年碳排放约36亿t,约占全国工业碳排放量的36%,此外化工冶金废气、固废、废热产生量大、堆存量多、难利用、循... 详细信息

双碳战略是国家重大战略,也是推动国家经济高质量可持续发展的必由之路。我国碳达峰到碳中和时间短、任务重。我国化工冶金每年碳排放约36亿t,约占全国工业碳排放量的36%,此外化工冶金废气、固废、废热产生量大、堆存量多、难利用、循环利用率低。发展化工冶金低碳化转型和变革,是我国工业领域双碳目标实现的根本保证。我国化工冶金历时百年,已发展成熟,仅通过原料燃料替代及绿色工艺转型减碳容量有限,亟需开展化工冶金跨行业耦合与循环利用技术变革,深入推动工业领域减碳。我国化工冶金大多是孤立、非循环连续工艺过程,引起跨行业耦合难、循环利用难度大的问题。针对上述问题,首先分析了化工冶金行业碳排放治理现状及国家战略需求;其次,提出了废气与废热耦合热化学转化制高质气体、废气与废气耦合定向催化制高端化学品、废气与固废耦合制低碳材料3个减碳增效策略。结合其技术发展现状和趋势,提出了拟重点发展的化工冶金跨行业耦合二氧化碳循环利用技术,以期为工业低碳绿色发展提供支撑。

关键词：化工冶金二氧化碳碳减排跨行业耦合循环利用

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Highly efficient ozone elimination by metal doped ultra-fine Cu_(2)O nanoparticles

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Journal of Environmental Sciences 2023年第12期134卷 108-116页

作者： Anqi Wang Le Zhang Jian Guan Xiaoze Wang Guojun Ma Guijun Fan Hang Wang Ning Han yunfa chen State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China Key Laboratory of Science&Technology on Particle Materials Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Metallurgical Engineering Xi’an University of Architecture and TechnologyXi’an 710055China

Nowadays,ozone contamination becomes dominant in air and thus challenges the research and development of cost-effective *** this study,metal doped Cu_(2)O catalysts are synthesized via reduction of Cu^(2+)by ascorbic acid in base solutions containing doping metal *** results show that compared with pure Cu_(2)O,the Mg^(2+)and Fe^(2+)dopants enhance the O_(3)removal efficiency while Ni2+depresses the *** specific,Mg-Cu_(2)O shows high O3removal efficiency of 88.4%in harsh environment of 600,000 mL/(g·hr) space velocity and 1500 ppmV O_(3),which is one of the highest in the *** and electron paramagnetic spectroscopy characterization shows higher concentration of crystal defects induced by the Mg^(2+)dopants,favoring the *** in-situ diffuse reflectance Fourier transform infrared spectroscopy shows the intermediate species in the O_(3)degradation process change from O_(2)^(2-)dominant of pure Cu_(2)O to O_(2)^(-)dominant of Mg-Cu2O,which would contribute to the high *** these results show the promising prospect of the Mg-Cu_(2)O for highly efficiency O_(3)removal.

关键词： Ozone catalyst Cu_(2)O Dopant Ultra-fine nanoparticles

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Dynamic apertures with diffusion-regulatory functionality in soft porous crystals:A key to solving the century puzzle on isotopologues separation

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Nano Research 2023年第2期16卷 3254-3255页

作者： Yanhong Li Jianze Xiao Yangyang Guo Ning Han Fangli Yuan yunfa chen Ming-Shui Yao State Key Laboratory of Multi-phase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China CAS Key Laboratory of Green Process and Engineering Institute of Process EngineeringInnovation Academy for Green ManufactureChinese Academy of SciencesBeijing 100190China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesChinese Academy of SciencesBeijing 100049China Key Laboratory of Science and Technology on Particle Materials Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

The separation of water isotopologues has been a“century-old”challenge,also known as“the Holy Grail”in separation *** water(D2O)is a stable non-radioactive water isotopologue that plays a critical role in scientific research,military,nuclear energy,and medical *** water was first reported in 1931 when *** discovered D2 and D2O,for which he was awarded the Nobel Prize in Chemistry in *** in 1933,*** et *** 0.5μL of heavy water at a concentration of around 65.7%when electrolyzing 10 liters of *** 1935,the world's first heavy water plant was built in Norway,producing 2 tons of heavy water by electrolysis,but the separation factor was merely 1.05,which was extremely *** 1943,the first heavy water plant employing the distillation method was built in the United States.

关键词： separation porous distillation

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Effect of acidic surface functional groups on Cr(Ⅵ) removal by activated carbon from aqueous solution

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Rare Metals 2010年第3期29卷 333-338页

作者： ZHOU Hualei chen yunfa School of Applied Sciences University of Science and Technology Beijing Beijing 100083 China State Key Laboratory of Multi-phase Complex System Institute of Process Engineering Chinese Academy of Sciences Beijing 100080 China

The activated carbon with high surface area was prepared by KOH *** was further modified by H2SO4 and HNO3 to introduce more surface functional *** pore structure of the activated carbons before and after modification was analyzed based on the nitrogen adsorption *** morphology of those activated carbons was characterized using scanning electronic microscopy （SEM）.The surface functional groups were determined by Fourier transform infrared spectroscopy （FTIR）.The quantity of those groups was measured by the Boehm titration ***（VI） removal by the activated carbons from aqueous solution was investigated at different pH *** results show that compared with H2SO4,HNO3 destructs the original pore of the activated carbon more seriously and induces more acidic surface functional groups on the activated *** pH value of the solution plays a key role in the Cr（VI） *** ability of reducing Cr（VI） to Cr（III） by the activated carbons is relative to the acidic surface functional *** higher pH values,the Cr（VI） removal ratio is improved by increasing the acidic surface functional groups of the activated *** lower pH values,however,the acidic surface functional groups almost have no effect on the Cr（VI） removal by the activated carbon from aqueous solution.

关键词： activated carbon surface functional groups removal modification chromium(VI)

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Controlling electrodeposited Ni layers by different-sized graphene oxides enables conductive e-textiles for the highly sensitive electrochemical detection of glucose

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Nano Research 2024年第7期17卷 6258-6264页

作者： Zhen Li Zibo chen Xiaodong Ji Huihui Jin yunfa Si Jingwei Zhang cheng chen Daping He Sanya Science and Education Innovation Park of Wuhan University of Technology Sanya 572000China School of Science Wuhan University of TechnologyWuhan 430070China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070China Hubei Engineering Research Center of RF-Microwave Technology and Application Wuhan University of TechnologyWuhan 430070China

With the increasing popularity of wearable electronic devices,there is an urgent demand to develop electronic textiles(e-textiles)for device ***,the difficulty in reconciliation between conductivity and manufacturing costs hinders their large-scale practical ***,we reported a facile and economic method for preparing conductive ***,nonconductive polypropylene(PP)was wrapped by reduced graphene oxide(rGO),followed by the electrodeposition of Ni nanoparticles(NPs).Notably,modulating the sheet size of graphene oxide(GO)resulted in controllable deposition of Ni NPs with adjustable size,allowing for controlled manipulations over the structures,morphologies,and conductivity of the obtained e-textiles,which influenced their performance in electrochemical glucose detection *** optimal material,denoted as Ni/rGO+(0.2)/PP,exhibited an impressive conductivity of 7.94×10^(4)S·m^(−1).With regard to the excellent conductivity of the as-prepared e-textiles and the high electrocatalytic activity of Ni for glucose oxidation,the asprepared e-textiles were subjected to glucose *** was worth emphasizing that the Ni/rGO_(0.2)/PP-based electrode demonstrated promising performance for nonenzymatic/label-free glucose detection,with a detection limit of 0.36μM and a linear response range of 0.5μM to 1 *** study paves the way for further development and application prospects of conductive etextiles.

关键词： conductive e-textiles nonenzymatic/label-free glucose detection controllable Ni deposition graphene oxides sizedependent effect

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Preparation and Li^+ storage properties of hierarchical hollow porous carbon spheres

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Particuology 2014年第3期12卷 44-50页

作者： Xiaofeng Wu Wenxiang Tang Kejia Jiao yunfa chen State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of Sciences Graduate University of Chinese Academy of Sciences

Hollow ordered porous carbon spheres （HOPCS） with a hierarchical structure were prepared by templating with hollow ordered mesoporous silica spheres （HOMSS）. Scanning electron microscopy （SEM） and transmission electron microscopy （TEM） showed that HOPCS exhibited a spherical hollow morphology. High-resolution TEM, small angle X-ray diffraction （SAXRD） and N2 sorption measurements confirmed that HOPCS inversely replicated the unconnected hexagonal-stacked pore structure of HOMSS, and possessed ordered porosity. HOPCS exhibited a higher storage capacity for Li^＋ ion battery （LIB） of 527.6 mA h/g, and good cycling performance. A large capacity loss during the first discharge-charge cycle was found attributed to the high content of micropores. The cycling performance was derived from the hierarchical structure.

关键词： Hierarchical structure MCM-41 silica Nanostructured carbon Lithium storage

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Extraction of scandium from red mud by modified activated carbon and kinetics study

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Rare Metals 2008年第3期27卷 223-227页

作者： ZHOU Hualei LI Dongyan TIAN Yajun chen yunfa State Key Laboratory of Multi-phase Complex System lnstituteqfProcess Engineering Chinese Academy of Sciences Beijing 100080 China School of Applied Sciences University of Science and Technology Beo＇ing Beijing 100083 China

Activated carbon （AC） was modified by tri-butyl phosphate （TBP） for selectively extracting scandium from red mud and characterized by BET （Brunauer-Emmett-Teller） surface area. The modified AC had a preferential adsorption to scandium. The influences of adsorbent dos- age, adsorption temperature, and time on adsorption capacity and selectivity to scandium were examined. An optimum adsorbent dosage （-6.25 g/L）, adsorption temperature （308 K）, and adsorption time （40 min） were figured out. A pseudo-second-order kinetics model was employed for describing the adsorption process of scandium.

关键词： modified activated carbon adsorption red mud scandium

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