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Combining anodic alcohol oxidative coupling for C-C bond formation with cathodic ammonia production

National Science Review 2024年第5期11卷 217-226页

作者： Leitao Xu Wei Chen Cairong Wang Wenjie Wu Yelin Yao Zhifeng Huang Jingcheng Wu Ming Yang Yandong Wu Dianke Xie Yuqin Zou Shuangyin Wang State Key Laboratory of Chemo/bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringAdvanced Catalytic Engineering Research Center of the Ministry of Education Hunan University

Electrocatalytic oxidation of alcohols using heterogeneous catalysts is a promising aqueous, energy-efficient and environmentally friendly approach, especially for coupling different alcohols to prolong the carbon chain via co-oxidation. Precisely regulating critical steps to tailor electrode materials and electrolyte composition is key to selectively coupling alcohols for targeted synthesis. However, selectively coupling different alcohols remains challenging due to the lack of effective catalyst and electrolyte design promoting specific pathways. Herein, we demonstrate a paired electrolysis strategy for combining anodic oxidative coupling of ethanol（EtOH） and benzyl alcohol（PhCH2OH） to synthesize cinnamaldehyde（CAL） and cathodic ammonia production. The strategies involve:（i） utilizing the salt-out effect to balance selective oxidation and coupling rates;（ii） developing platinum-loaded nickel hydroxide electrocatalysts to accelerate intermediate coupling kinetics;（iii） introducing thermodynamically favorable nitrate reduction at the cathode to improve coupling selectivity by avoiding hydrogenation of products while generating valuable ammonia instead of hydrogen. We achieved 85% coupling selectivity and 278 μmol/h NH3productive rate at 100 m A/cm2with a low energy input（～1.63 V）. The membrane-free, low energy, scalable approach with a wide substrate scope highlights promising applications of this methodology. This work advances heterogeneous electrocatalytic synthesis through rational design principles that integrate anodic oxidative coupling with cathodic nitrate reduction reactions, having synergistic effects on efficiency and selectivity.

关键词： anodic alcohol oxidative coupling C–C bond formation cinnamaldehyde cathodic ammonia production

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Convergent synthesis and immunological study of oligosaccharide derivatives related to galactomannan from Antrodia cinnamomea

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Chinese Chemical Letters 2024年第5期35卷 155-160页

作者： Shuying Li Weiwei ZhuGe Xuan Sun Chongzhen Sun Zhaojun Liu Chenghe Xiong Min Xiao Guofeng Gu National Glycoengineering research center and Shandong Key Laboratory of Carbohydrate chemistry and Glycobiology Shandong UniversityQingdao 266237China NMPA Key Laboratory for Quality research and Evaluation of Carbohydrate-based Medicine Shandong UniversityQingdao 266237China

The galactomannan from Antrodia cinnamomea(AC)is characterized as one of the important bioactive components that exhibits potential immunostimulatory *** biological function of its corresponding oligosaccharide fragments has not been revealed *** this study,we reported the first chemical synthesis of the series of oligosaccharide fragments related to AC galactomannan via the convergent glycosylation *** preliminary immunological evaluation of these synthesized AC oligosaccharides disclosed that the backbone tetrasaccharide 1d showed the best immunomodulatory ability on enhancing proliferation,phagocytosis and cytokines secretion of Raw264.7 macrophages in vitro,indicating its immense potential as an immunostimulant candidate.

关键词： Antrodia cinnamomea Galactomannan Oligosaccharide Immunostimulatory propriety Chemical synthesis

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Heterostructured Co_(3)Se_(4)/CoSe_(2)@C nanoparticles attached on three-dimensional reduced graphene oxide as a promising anode towards Li-ion batteries

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Frontiers of Materials Science 2024年第2期18卷 101-115页

作者： Mingjun Pang Zhaoyang Song Miaomiao Mao Shang Jiang Ruxia Zhang Runwei Wang Jianguo Zhao Engineering research center of Coal-based Ecological Carbon Sequestration Technology of the Ministry of Education Shanxi Datong UniversityDatong 037009China State Key Laboratory of Inorganic Synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China

In situ carbon-coated Co_(3)Se_(4)/CoSe_(2)(Co_(x)Se_(y))nanoparticles(NPs)attached on three-dimensional(3D)reduced graphene oxide(rGO)sheets were skillfully developed in this work,which involved the environment-friendly hydrothermal method,freeze drying,and selenide *** the structure,the glucose-derived carbon layer exhibited significantly homogeneous dispersion under an argon *** structure not only has enhanced stability,but also can effectively mitigate the volume swell of Co_(x)Se_(y) *** resulted Co_(3)Sea/CoSe_(2)@C/rGO(CSe@C/rGO)exhibited a specific surface area(SSA)of 240.9 m^(2)·g^(-1),offering more electrochemically active sites for the storage of energy related to lithium *** rGO matrix held exceptional flexibility and functional structural rigidity,facilitating the swift ion intercalation and ensuring the high conductivity and recyclability of the *** applied to anodes designed for lithium-ion batteries(LiBs),this material demonstrated distinguished rate and ultra-high reversible capacity(872.98 mA·h·g^(-1) at 0.5 A·g^(-1)).Meanwhile,its capacity retention reached 119.5%after 500 cycles at 2 A·g^(-1),with a coulombic efficiency of 100%.This work potentially paves the way for generating fast and powerful metal selenide anodes and initiating LiBs with good performance.

关键词： CSe@C/rGO lithium-ion battery reduced graphene oxide electrochemicalperformance heterostructure

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Superwetting Ag/α-Fe_(2)O_(3) anchored mesh with enhanced photocatalytic and antibacterial activities for efficient water purification

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Green Energy & Environment 2024年第1期9卷 89-103页

作者： Jiakai Li Changpeng Lv Jiajia Song Xiaoling Zhang Xizhen Huang Yingzhuo Ma Haijie Cao Na Liu Department of chemistry Tsinghua UniversityBeijing100084China Anhui Provincial Engineering Laboratory of Silicon-based Materials Engineering Technology Research Center of Silicon-based Materials(Anhui)School of Material and Chemical EngineeringBengbu UniversityBengbu233030China Institute of Materials for Energy and Environment College of Materials Science and EngineeringQingdao UniversityQingdao266071China

Superwetting materials have drawn unprecedented attention in the treatment of oily wastewater due to their preferable anti-fouling property and selective oil/water ***,it is still a challenge to fabricate multifunctional and environmentally friendly materials,which can be stably applied to purify the actual complicated ***,a Ag/Ag/α-Fe_(2)O_(3) heterostructure anchored copper mesh was intentionally synthesized using a facile two-step hydrothermal *** resultant mesh with superhydrophilicity and underwater superoleophobicity was capable of separating various oil/water mixtures with superior separation efﬁciency and high permeationﬂux driven by ***ﬁting from the joint effects of the smaller band gap of Ag/α-Fe_(2)O_(3) heterojunction,inherent antibacterial capacity of Ag/α-Fe_(2)O_(3) and Ag nanoparticles,favorable conductive substrate,as well as the hierarchical structure with superwettability,such mesh presented remarkably enhanced degradation capability toward organic dyes under visible light irradiation and antibacterial activity against both Escherichia coli(***)and Staphylococcus aureus(***)compared with the pure Ag/α-Fe_(2)O_(3) coated ***,the mesh exhibited bifunctional water puriﬁcation performance,in which organic dyes were eliminated simultaneously from water during oil/water separation in oneﬁltration *** importantly,this mesh behaved exceptional chemical resistance,mechanical stability and long-term ***,this material with multifunctional integration may hold promising potential for steady water puriﬁcation in practice.

关键词： Superwetting Ag/α-Fe_(2)O_(3)heterostructure Enhanced photocatalytic and antibacterial activities Water purification Long-term reusability

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Hollow Metal-Organic Framework/MXene/Nanocellulose Composite Films for Giga/Terahertz Electromagnetic Shielding and Photothermal Conversion

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Nano-Micro Letters 2024年第9期16卷 161-179页

作者： Tian Mai Lei Chen Pei‑Lin Wang Qi Liu Ming‑Guo Ma research center of biomass Clean Utilization MOE Engineering Research Center of Forestry Biomass Materials and BioenergyBeijing Key Laboratory of Lignocellulosic ChemistryCollege of Materials Science and TechnologyBeijing Forestry UniversityBeijing 100083People’s Republic of China State Silica-based Materials Laboratory of Anhui Province Bengbu 233000People’s Republic of China

With the continuous advancement of communication technology,the escalating demand for electromagnetic shielding interference(EMI)materials with multifunctional and wideband EMI performance has become *** the electrical and magnetic components and designing the EMI material structure have attracted extensive interest,but remain a huge ***,we reported the alternating electromagnetic structure composite films composed of hollow metal-organic frameworks/layered MXene/nanocellulose(HMN)by alternating vacuum-assisted filtration *** HMN composite films exhibit excellent EMI shielding effectiveness performance in the GHz frequency(66.8 dB at Kaband)and THz frequency(114.6 dB at 0.1-4.0 THz).Besides,the HMN composite films also exhibit a high reflection loss of 39.7 dB at 0.7 THz with an effective absorption bandwidth up to 2.1 ***,HMN composite films show remarkable photothermal conversion performance,which can reach 104.6℃under 2.0 Sun and 235.4℃under 0.8 W cm^(−2),*** unique micro-and macrostructural design structures will absorb more incident electromagnetic waves via interfacial polarization/multiple scattering and produce more heat energy via the local surface plasmon resonance *** features make the HMN composite film a promising candidate for advanced EMI devices for future 6G communication and the protection of electronic equipment in cold environments.

关键词： Metal-organic frameworks MXene Nanocellulose Electromagnetic shielding Photothermal conversion

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Bridging molecular photosensitizer and catalyst on carbon nanotubes toward enhanced selectivity and durability for CO_(2)photoreduction

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Journal of Environmental Sciences 2024年第6期140卷 157-164页

作者： Xiaofeng Cui Xueting Wang Lijun Zhao Jixin Wang Tingting Kong Yujie Xiong Anhui Engineering research center of Carbon Neutrality The Key Laboratory of Functional Molecular SolidsMinistry of EducationAnhui Laboratory of Molecular-Based MaterialsCollege of Chemistry and Materials ScienceAnhui Normal UniversityWuhu 241002China School of chemistry and Chemical Engineering Anqing Normal UniversityAnqing 246011China School of chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China

Homogenous molecular photocatalysts for CO_(2)reduction,especially metal complex-based photosensitizer-catalyst assemblages,have been attracting extensive research interests due to their efficiency and ***,their low durability and recyclability limit practical *** this work,we immobilized the catalysts of metal terpyridyl complexes and the photosensitizer of[Ru(bpy)3]Cl2onto the surface of carbon nanotubes through covalent bonds and electrostatic interactions,respectively,transforming the homogeneous system into a heterogeneous *** characterizations prove that these metal complexes are well dispersed on CNTs with a high loading(ca.12 wt.%).Photocatalytic measurements reveal that catalytic activity is remarkably enhanced when the molecular catalysts are anchored,which is three times higher than that of homogeneous molecular ***,when the photosensitizer of[Ru(bpy)3]Cl2is immobilized,the side reaction of hydrogen evolution is completely suppressed and the selectivity for CO production reaches 100%,with its durability also significantly *** work provides an effective pathway for constructing heterogeneous photocatalysts based on rational assembly of efficient molecular photosensitizers and catalysts.

关键词： durability selectivity catalyst

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Road map for, and technical challenges of, carbon-nanotube integrated circuit technology

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National Science Review 2024年第3期11卷 14-16页

作者： Jia Si Panpan Zhang Zhiyong Zhang Key Laboratory for the Physics and chemistry of Nanodevices and center for Carbon-based Electronics School of Electronics Peking University State Key Laboratory of Information Photonics and Optical Communications Beijing University of Posts and Telecommunications

The past decade has witnessed an explosion of research on carbon-nanotube(CNT) electronics due to their outstanding properties, including an ultrathin body, a high carrier mobility and a high saturation velocity.

关键词： TRANSISTORS

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Regioselective C-C bond cleavage/aminocarbonylation cascade under copper catalysis

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Science China chemistry 2024年第11期67卷 3798-3806页

作者： Qi-Chao Shan Yan Zhao Yong Wu Hong-Fei Liu Xin-Hua Duan Li-Na Guo Department of chemistry School of Chemistry Energy Research Center of Energy Storage Materials and Devices Ministry of EducationXi'an Jiaotong University State Key Laboratory of Applied Organic chemistry Lanzhou University

A regioselective C-C bond cleavage/aminocarbonylation cascade is presented. In recent years, tremendous progress has been made in the alkoxyl radical-mediated C-C bond cleavage of unstrained monocarbocycles. In contrast, the deconstruction and functionalization of bicyclic skeletons has been less developed and has mainly focused on the ring expansion process. Inspired by the aromatization-driven C-C bond cleavage, here we demonstrate a ring-opening/aminocarbonylation cascade under copper catalysis, in which the formation of a stable γ-lactam or succinimide skeleton reverses the selectivity of C-C cleavage. Remarkably, the photo and thermal assistance is not required when the succinimide skeleton is formed during the ring opening process. DFT calculations revealed that this unexpected ring-opening process is thermodynamically and kinetically favourable.

关键词： C-C bond cleavage controllable regioselectivity aminocarbonylation bicyclic alkoxy radical

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STING agonist-conjugated metal-organic framework induces artificial leukocytoid structures and immune hotspots for systemic antitumor responses

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National Science Review 2024年第7期11卷 189-204页

作者： Taokun Luo Xiaomin Jiang Yingjie Fan Eric Yuan Jinhong Li Langston Tillman Wenbin Lin Department of chemistry University of Chicago Department of Radiation and Cellular Oncology and the Ludwig center for Metastasis research University of Chicago

Radiotherapy is widely used for cancer treatment, but its clinical utility is limited by radioresistance and its inability to target metastases. Nanoscale metal-organic frameworks(MOFs) have shown promise as high-Z nanoradiosensitizers to enhance radiotherapy and induce immunostimulatory regulation of the tumor microenvironment. We hypothesized that MOFs could deliver small-molecule therapeutics to synergize with radiotherapy for enhanced antitumor efficacy. Herein, we develop a robust nanoradiosensitizer,GA-MOF, by conjugating a STING agonist, 2,3-cyclic guanosine monophosphate–adenosine monophosphate(GA), on MOFs for synergistic radiosensitization and STING activation. GA-MOF demonstrated strong anticancer efficacy by forming immune-cell-rich nodules(artificial leukocytoid structures) and transforming them into immunostimulatory hotspots with radiotherapy. Further combination with an immune checkpoint blockade suppressed distant tumors through systemic immune activation. Our work not only demonstrates the potent radiosensitization of GA-MOF, but also provides detailed mechanisms regarding MOF distribution, immune regulatory pathways and long-term immune effects.

关键词： metal-organic framework radiosensitization STING agonist artificial leukocytoid structures immune hotspots immunotherapy nanomedicine

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Hydrogen bond-bridged phosphorene flexible film for photodynamic inhibiting Staphylococcus aureus

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Nano research 2024年第6期17卷 5461-5468页

作者： Ziyu Wei Wenting Li Zhifang Liu Yongfa Zhu Huaqiang Cao Department of chemistry Engineering Research Center of Advanced Rare Earth MaterialsTsinghua UniversityBeijing 100084China

Antibiotics are a widely used and effective treatment for bacterial ***,bacteria can gradually evolve during infection,leading to developing resistance to antibiotics,which renders previously effective treatments *** a useful and convenient manner to treat bacterial infections is a great ***,we report a flexible hydrogen-bond-bridged phosphorene film with photodynamic antibacterial properties and excellent mechanical properties,fabricated from electrochemical exfoliation of black phosphorus(BP).When illuminated under 700 nm light,the hydrogen bond-bridged phosphorene flexible film is capable of converting ground-state triplet oxygen(O_(2))into excited-state singlet oxygen(^(1)O_(2)),destroying the structure of the membrane of Staphylococcus aureus,and eventually leading to bacterial death,via breaking the C=C of unsaturated fatty acids within the bacterial cell membrane after the reaction between^(1)O_(2)and unsaturated fatty acids,thus realizing a highly efficient antibacterial approach,which is supported by gas chromatography-mass spectrometry(GC-MS)*** work establishes an effective phototherapy platform for treating bacterial traumatic infections.

关键词： hydrogen bond-bridged phosphorene flexible film photodynamic Staphylococcus aureus

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