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engineering Ru(N^N)_(3)-modified covalent organic framework for photocatalytic olefin epoxidation

Science China Chemistry 2024年第11期67卷 3719-3728页

作者： Yan-Lin Li Sheng-Li Huang Guo-Yu Yang Key Laboratory of Cluster Science(Ministry of Education) Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081China

Photocatalytic olefin oxidation using air as an oxidant is an environmentally friendly method for producing epoxides. Covalent organic frameworks(COFs) have emerged as promising photocatalysts in various organic synthesis reactions. The combination of tri-(2-pyridinal aldehyde)-containing precursor with 4,4’,4’’-(1,3,5-triazine-2,4,6-triyl)trianiline generated(N^N)-I-COF. Via imine-to-quinoline transformation and coordination anchorage of Ru(N^N)_(3)unit, Ru(N^N)_(3)@Q-COF was obtained with improved chemical stability, skeleton conjugation, and novel photochemical characteristics, and demonstrated excellent photocatalytic activity in olefin epoxidation with a wide range of substrates. The presence of H_(2)O played a crucial role in the formation of reactive oxygen species(ROSs), which in turn influenced the olefin oxidation process. The hydrophilicity of Ru(N^N)_(3) facilitated the approach of H_(2)O and O_(2) to the photogenerated charges, thereby promoting ROSs generation. The lipophilicity of Q-COF allowed for the absorption of olefin substrates, and its nano-channels increased encountering possibility between olefins and ROSs. Consequently, Ru(N^N)_(3)@Q-COF provided an intriguing platform for olefin photooxidation and could be recycled multiple times without any degradation in performance. This report revealed that the conversion of classical ROSs into less potent oxidants with rapid kinetic rates played a crucial role in achieving highly efficient and selective epoxidation of terminal olefins.

关键词： polypyridyl Ru covalent organic framework olefin epoxidation photocatalysis

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Preparation of slow-release regulated Rs-198 bilayer microcapsules and application of its lyophilized bacterial inoculant on Capsicum annuum *** salt stress

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Particuology 2023年第8期79卷 54-63页

作者： Shuangxi Zhu Yanhui He Jiawei Dong Yujia Dong Chun Li Zhansheng Wu Yimeng Lu Xi'an Key Laboratory of Textile Chemical Engineering Auxiliaries School of Environmental and Chemical EngineeringXi'an Polytechnic UniversityXi'an710048China Department of Chemical Engineering Tsinghua UniversityBeijing100084China

The survival adaptation of bacteria in saline soil is *** bilayer microcapsules were prepared by secondary embedding of monolayer sodium alginate(NaAlg)-bentonite(Bent)-sodium carboxy-methylcellulose(CMC)microcapsules wrapped with plant growth promoting rhizobacteria(PGPR)Pseudomonas putida Rs-198 by chitosan solution to promote the synergistic effect of bilayer microen-capsulation and *** characterization of the Rs-198 bilayer microcapsules showed that the amino and carboxyl groups were cross-linked and a thin layer of chitosan was formed on the outside of the *** bilayer microcapsule(Ch-d)with a chitosan concentration of 0.8 wt%and pH 6 showed a slow release of bacteria with a maximum release of 6.06 × 10^(9) cfu/g on the 7th *** viable bacteria of Ch-d increased by 4.42%after 60 days of storage compared with monolayer *** 0.9 wt%L-cysteine,10 wt%glycerinum,10 wt%trehalose and 12 wt%soluble starch were added as bacterial protective agents during the process of preparing the Ch-d lyophilized bacterial inoculant(Ch-d LBI).Pot experiments showed that Ch-d LBI exhibited better growth promotion of Capsicum annuum *** salt ***,the bilayer microcapsule as slow-release bacterial inoculant is a potential alternative for sustainable agriculture.

关键词： Pseudomonas putida Rs-198 Bilayer microcapsules Chitosan solution Lyophilized bacterial inoculant

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NH_(4)^(+)-Modulated Cathodic Interfacial Spatial Charge Redistribution for High-Performance Dual-Ion Capacitors

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Nano-Micro Letters 2025年第5期17卷 391-406页

作者： Yumin Chen Ziyang Song Yaokang Lv Lihua Gan Mingxian Liu Shanghai Key Lab of Chemical Assessment and Sustainability School of Chemical Science and EngineeringTongji UniversityShanghai 200092People’s Republic of China College of Chemical Engineering Zhejiang University of TechnologyHangzhou 310014People’s Republic of China

Compared with Zn^(2+),the current mainly reported charge carrier for zinc hybrid capacitors,small-hydrated-sized and light-weight NH_(4)^(+)is expected as a better one to mediate cathodic interfacial electrochemical behaviors,yet has not been *** we propose an NH_(4)^(+)-modulated cationic solvation strategy to optimize cathodic spatial charge distribution and achieve dynamic Zn^(2+)/NH_(4)^(+)co-storage for boosting Zinc hybrid *** to the hierarchical cationic solvated structure in hybrid Zn(CF_(3)SO_(3))_(2)–NH_4CF_(3)SO_(3)electrolyte,high-reactive Zn^(2+)and small-hydrate-sized NH_4(H_(2)O))(4)^(+)induce cathodic interfacial Helmholtz plane reconfiguration,thus effectively enhancing the spatial charge density to activate 20%capacity ***,cathodic interfacial adsorbed hydrated NH_(4)^(+)ions afford high-kinetics and ultrastable C···H(NH_(4)^(+))charge storage process due to a much lower desolvation energy barrier compared with heavy and rigid Zn(H_(2)O)_6^(2+)(5.81 vs.14.90 eV).Consequently,physical uptake and multielectron redox of Zn^(2+)/NH_(4)^(+)in carbon cathode enable the zinc capacitor to deliver high capacity(240 mAh g^(-1)at 0.5 A g^(-1)),large-current tolerance(130 mAh g^(-1)at 50 A g^(-1))and ultralong lifespan(400,000cycles).This study gives new insights into the design of cathode–electrolyte interfaces toward advanced zinc-based energy storage.

关键词： NH_(4)^(+)-modulated cathodic interface Spatial charge redistribution Zn^(2+)/NH_(4)^(+) co-storage Dual-ion capacitor

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Hydrophobic modification of polysaccharides and the construction and properties of their micelles:a review of applications in the field of biomedicine

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Science China Chemistry 2024年第6期67卷 1881-1903页

作者： Dayang Wang Xiaohua Li Huanchen Yao Xin Liu Yan Gao Hailin Cong Bing Yu Youqing Shen College of Chemistry and Chemical Engineering College of Life SciencesCollege of Materials Science and EngineeringInstitute of Biomedical Materials and EngineeringQingdao UniversityQingdao266071China State Key Laboratory of Bio-Fibers and Eco-Textiles Qingdao UniversityQingdao266071China School of Materials Science and Engineering Shandong University of TechnologyZibo255000China Key Laboratory of Biomass Chemical Engineering of Ministry of Education Center for Bionanoengineeringand Department of Chemical and Biological EngineeringZhejiang UniversityHangzhou310027China

Nanomedicine delivery technology plays an important role in modern medicine and has shown good therapeutic effects in scientific *** have the characteristics of wide sources,excellent biocompatibility,and *** addition,there are multifunctional groups on the main chain of polysaccharides,which can be surface-modified or functionalized to have targeting ability through specific sugar *** polysaccharide micelles with good biocompatibility,degradability,high safety,easy structural modification,and special core-shell structure are regarded as ideal carriers for ***,this review is focused on the hydrophobic modification designs of polysaccharides,the preparation methods and characteristics of micelles,and the applications of amphiphilic polysaccharide micelles in the field of *** is expected to provide some ideas and inspiration for the design of polysaccharide drug carriers.

关键词： polysaccharide hydrophobic modification micelle drug delivery biomedicine

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MXene-based materials for separator modification of lithium-sulfur batteries

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Chinese Journal of Structural Chemistry 2024年第7期43卷 54-64页

作者： Fangling Cui Zongjie Hu Jiayu Huang Xiaoju Li Ruihu Wang Hebei Key Laboratory of Functional Polymer School of Chemical Engineering and TechnologyHebei University of TechnologyTianjin300130China

Lithium-sulfur(Li-S)batteries are one of the promising energy storage ***,rapid capacity attenuation caused by shuttle effect of soluble polysulfides is a major challenge in practical *** separator modification is one complementary countermeasure besides the construction of sulfur host materials in *** is one type of outstanding candidates for promoting redox kinetics of sulfur ***,recent advances of MXene-based materials as separator modifiers are *** importance of high conductivity and catalytic effects in promoting catalytic conversion of polysulfides and suppressing shuttle effect of polysulfides has been highlighted,and the superiority of MXene for improving reversible capacity and cycling stability has been *** strategies for the design of MXene-based separator modifiers are proposed to improve energy density and *** review provides new perspectives for future development of high-performance Li-S batteries.

关键词： MXene Lithium-sulfur batteries Separators Shuttle effects Catalysis

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Structure engineering of Layered Double Hydroxides(LDHs)for Heterogeneous Catalysis

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chemical Research in Chinese Universities 2024年第4期40卷 590-610页

作者： GAO Zhexi MA Haoran WANG Qian LI Dianqing FENG Junting DUAN Xue State Key Laboratory of Chemical Resource Engineering Beijing Engineering Center for Hierarchical CatalystsBeijing University of Chemical TechnologyBeijing100029P.R.China Quzhou Institute for Innovation in Resource Chemical Engineering Quzhou324000P.R.China

Layered double hydroxide(LDH)is regarded as an advanced platform material in catalysis and attracts vast attrition *** a kind of two-dimensional layered material,it exhibits great advantages including cation-tunability in layer,lattice limitation,topological transformation,ion exchange and intercalation *** also can be used as building blocks for composite catalytic *** 100 years,a large number of works have been accomplished and researchers made great progress on investigating the LDH-based catalytic *** this review,we summarize representative achievements and significant progress in recent years,which mainly include constructing high entropy catalytic material,high dispersion/stability and interfacial supported catalytic material,composite catalytic materials and nano-reactor based on ***,through collecting the excellent works,we conclude the future development potential of LDH and provide a perspective.

关键词： Layered double hydroxide(LDH)material Heterogeneous catalysis Structure engineering

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Beyond two-dimension: One-and zero-dimensional halide perovskites as new-generation passivators for high-performance perovskite solar cells

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Journal of Energy Chemistry 2023年第8期83卷 189-208,I0007页

作者： Yuanyuan Zhao Huimin Xiang Ran Ran Wei Zhou Wei Wang Zongping Shao State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 210009JiangsuChina WA School of Mines:Minerals Energy and Chemical EngineeringCurtin UniversityPerthWA 6845Australia

Perovskite solar cells(PSCs) as a rising star in the photovoltaic field have received rapidly increasing attention recently due to the boosting power conversion efficiencies(PCEs) from 3.8% to 25.7% in the last13 years. Nevertheless, the conventional PSCs with three-dimensional(3D) halide perovskites as light absorbers suffer from inferior PCEs and poor durability under sunlight, high-temperature and humid conditions due to the high defect amount and structural instability of 3D perovskites, respectively. To tackle these crucial issues, lower-dimensional halide perovskites including zero-dimensional(0D), onedimensional(1D), and two-dimensional(2D) perovskites have been employed as efficient passivators to boost the PCEs and durability of 3D-PSCs due to the high structural stability and superior resistance against moisture, heat and sunlight. Therefore, in order to achieve better understanding about the advantages and superiorities of combining low-dimensional perovskites with their 3D counterparts in improving the PCEs and durability of 3D-PSCs, the recent advances in the development and fabrication of mixeddimensional PSCs with 1D/0D perovskites as passivators are summarized and discussed in the *** superiority of 1D/0D perovskites as passivators over 2D counterparts, the passivation mechanism and the methods of 1D/0D perovskites are also presented and discussed. Furthermore, the rules to choose1D/0D perovskites or relevant spacer cations are also emphasized. On this basis, several specific strategies to design and fabricate mixed-dimensional PSCs with 1D/0D perovskites are presented and ***, the crucial challenges and future research directions of mixed-dimensional PSCs with 1D/0D perovskites as passivators are also proposed and discussed. This review will provide some useful insights for the future development of high-efficiency and durable mixed-dimensional PSCs.

关键词： Perovskite solar cells Mixed-dimensional Passivators Stability Power conversion efficiency

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An orderly arranged dual-role MIL-53(Al)nanorods array rooted on carbon nanotube film for long-life and stable lithium-sulfur batteries

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Nano Research 2023年第2期16卷 2409-2420页

作者： Feichao Wu Quanqing Li Gaofeng Jin Yuhong Luo Xiaohang Du Jingde Li Zisheng Zhang Hebei Provincial Key Laboratory of Green Chemical Technology and High Efficient Energy Saving Tianjin Key Laboratory of Chemical Process SafetySchool of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300130China Department of Chemical and Biological Engineering University of OttawaOttawaON K1N 6N5Canada

It is of great value to synchronously resolve the critical issues of the polysulfide shuttle and dendrite growth in lithium-sulfur(Li-S)***,a bifunctional Al-based Material of Institute Lavoisier-53(MIL-53(Al))/carbon nanotube(MIL-53/CNT)composite is reported for this matter,which was constructed by growing an ordered MIL-53(Al)nanorods array on the CNT *** the sulfur cathode,the proposed structure serves as a multifunctional interlayer to block polysulfides and accelerate their catalytic conversion,thus efficaciously inhibiting the shuttle ***,when applied as the anode host material(Li@MIL-53/CNT),the flexible CNT film serves as a self-standing framework to accommodate Li metal and alleviate the volume expansion,while the uniform ion channels built by the MIL-53(Al)nanorods array along with the abundant oxygen groups can homogenize Li ion diffusion,enabling a steady Li plating/stripping behavior and limiting the dendrite *** surprisingly,Li-S full battery with MIL-53/CNT interlayer and Li@MIL-53/CNT anode delivers an appreciable specific capacity of 735 mAh·g^(–1)and excellent cycle durability at 5 C,presenting a limited capacity decay of 0.03%per cycle in 500 ***,an impressive cycle stability and rate capability are also achieved at high-sulfur loading and lean electrolyte conditions.

关键词： lithium-sulfur batteries nanorods array MIL-53(AL) interlayer anode host material

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Application and progress of techno-economic analysis and life cycle assessment in biomanufacturing of fuels and chemicals

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Green chemical engineering 2023年第2期4卷 189-198页

作者： Rongzhan Fu Lixia Kang Chenyue Zhang Qiang Fei Shaanxi Key Laboratory of Degradable Biomedical Materials School of Chemical EngineeringNorthwest UniversityXi'an710069China Shaanxi Key Laboratory of Energy Chemical Process Intensification School of Chemical Engineering and TechnologyXi'an Jiaotong UniversityXi'an710049China

To reduce the dependency on petroleum-based products and emission of greenhouse gas,renewable biofuels and chemicals play an important role to meet the unmatched energy demands of the rapidly growing ***,most biofuel and chemical products do not reach the commercialization stage,mainly hindered by incomparable economics to ***-economic assessment(TEA)is a useful tool to estimate eco-nomic performance,and identify bottlenecks for the development of biofuel and chemical production technology,meanwhile,life cycle assessment(LCA)is applied to assess sustainability by reducing the environmental impact of biofuel and chemical *** present review covers TEA and LCA research progress in the manufacturing of biofuels and biochemical,and discusses the impacts of TEA and LCA results on the development and optimi-zation of biofuel and chemical *** addition,challenges associated with TEA and LCA of biofuel and biochemical production were briefly overviewed,and potential approaches that may overcome such challenges were discussed enabling viable and sustainable biomanufacturing of fuels and *** integrated TEA and LCA studies could significantly promote the economic and sustainable development of the biomanufacturing process.

关键词： Techno-economic assessment Life cycle assessment Biomanufacturing Fuels chemicals Bioethanol Biodiesel

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MOF-assisted Synthesis of Dual-atom Palladium Catalysts for Acetylene Semi-hydrogenation

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China Petroleum Processing & Petrochemical technology 2024年第3期26卷 42-52页

作者： Chen Jie Xu Yuebing Qi Jian Liu Bing Liu Xiaohao Department of Chemical Engineering School of Chemical and Material EngineeringJiangnan UniversityWuxi 214122China State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

The selective removal of trace acetylene in ethylene feed gas is of great significance in the petrochemicalindustry;however, there are still challenges in designing and developing high-performance catalysts. Here, a MOFassistedencapsulation strategy was adopted for the precise synthesis of diatomic Pd2 sites on a ZnO support. When usedfor the acetylene semi-hydrogenation reaction, the dual-atom Pd2-ZnO catalyst exhibited improved catalytic performance,achieving complete conversion of acetylene at 125 °C with an 89% selectivity to ethene, as compared to Pd single-atom andnanoparticles. This enhancement was mainly attributed to the catalyst’s ability to dissociate H2 and facilitate the desorptionof intermediate C2H4. Moreover, the strong interaction between the support and the diatomic Pd sites was responsible for thecatalyst’s excellent stability during the long-term reaction.

关键词： dual-atom palladium acetylene semi-hydrogenation MOFs hydrogen dissociation intermediate

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