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Nickel-catalyzed enantioselective reductive amination of benzylic ketones in alcohols

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Science China Chemistry 2024年第8期67卷 2566-2570页

作者： Xiuhua Wang Jianrong Steve Zhou state key laboratory of chemical Oncogenomics School of Chemical Biology and BiotechnologyPeking University Shenzhen Graduate SchoolShenzhen 518055China

Asymmetric reductive amination directly converts ketones and amines to alkylamines, which are important motifs in *** report that cationic nickel complexes of chiral diphosphines promote enantioselective reductive amination of benzylic ketones with both arylamines and benzhydrazide. Isopropanol was used as a safe and cheap source of hydrogen instead of formic acid. The reaction can be readily applied to a concise synthesis of diarylethylamines, a class of neuroactive substances.

关键词： transfer hydrogenation nickel catalysis chiral alkylamine reductive amination synthetic method

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Optimization of biofuel supply chain integrated with petroleum refineries under carbon trade policy

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Frontiers of chemical Science and engineering 2024年第3期18卷 113-122页

作者： Wenhui Zhang Yiqing Luo Xigang Yuan chemical engineering Research Center School of Chemical Engineering and TechnologyTianjin UniversityTianjin300350China state key laboratory of chemical engineering Tianjin UniversityTianjin300350China

The use of fossil fuels results in significant carbon dioxide *** have been increasingly adopted as sustainable alternatives to fossil fuel to address this environmental *** petroleum refineries into biofuel supply chains is an effective approach to mitigating greenhouse gas emissions and improving environmental *** this study,an integrated supply chain optimization framework was established,considering the carbon trade *** addition,a mixed-integer nonlinear programming model was developed to optimize the selection of biomass suppliers,construction of pretreatment plants and biorefineries,integration of petroleum refineries,and selection of transportation routes with the objective of minimizing the total annual *** example is presented to illustrate the applicability of the *** optimization results show that integrating petroleum refineries into biofuel supply chains effectively mitigates carbon *** trade policies can have a direct impact on the total annual cost and carbon emissions of the supply chain.

关键词： renewable energy biofuel supply chain carbon trade policy

Amorphous hybrid tungsten oxide–nickel hydroxide nanosheets used as a highly efficient electrocatalyst for hydrogen evolution reaction

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Nano Research 2024年第4期17卷 2499-2508页

作者： Chao Lyu Chenghai Dai Yiwei Tan state key laboratory of Materials-Oriented chemical engineering School of Chemistry and Chemical EngineeringNanjing Tech UniversityNanjing 211816China

There are more challenges for alkaline hydrogen evolution reaction(HER)via simultaneously expediting the electron-coupled water dissociation process(Volmer step)and the following electrochemical H_(2) desorption(Heyrovsky step).Hybrid amorphous electrocatalysts are highly desirable for efficient hydrogen evolution from water-alkali electrolyzers due to the bifunctionality for the different elementary steps of HER and optimal interactions with water molecules and the reactive hydrogen intermediates(Had).Herein,the synthesis of amorphous hybrid ultrathin(tungsten oxide/nickel hydroxide)hydrate(a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O)nanosheets on nickel foam(NF)for efficient alkaline HER is *** structural and composition features of a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O are characterized in *** resulting a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O/NF electrocatalyst with the synergistic effect of both hybrid components for the HER elementary steps shows greatly improved the activity and durability for the HER with a low overpotential of-41 and-163 mV at-10 and-500 mA·cm^(-2),respectively,a Tafel slope as low as-72.9 mV·dec^(-1),and long-term stability of continuous electrolysis for at least 150 h accompanying by inappreciable overpotential change in 1 M *** the hybrid a-[WO_(3)/Ni(OH)_(2)]·0.2H_(2)O,Ni(OH)_(2) and WO_(3) moieties are separately responsible for accelerating dissociative adsorption of water and weakening Had adsorption strength,which is beneficial to the improvement of the alkaline HER activity.

关键词： amorphous nanomaterial bimetallic electrocatalyst tungsten oxide ultrathin nanosheet hydrogen evolution reaction

Towards carbon neutrality of calcium carbide-based acetylene production with sustainable biomass resources

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Green Energy & Environment 2024年第6期9卷 1068-1078页

作者： Peng Jiang Guanhan Zhao Hao Zhang Tuo Ji Liwen Mu Xiaohua Lu Jiahua Zhu state key laboratory of Materials-oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing211816China

Acetylene is produced from the reaction between calcium carbide(CaC_(2))and water,while the production of CaC_(2) generates significant amount of carbon dioxide not only because it is an energy-intensive process but also the raw material for CaC_(2) synthesis is from ***,a comprehensive biomass-to-acetylene process was constructed that integrated several units including biomass pyrolysis,oxygen-thermal CaC_(2) fabrication and calcium *** comparison,a coal-to-acetylene process was also established by using coal as *** carbon efficiency,energy efficiency and environmental impacts of the bio-based calcium carbide acetylene(BCCA)and coal-based calcium carbide acetylene(CCCA)processes were systematically ***,the environmental impacts were further evaluated by applying thermal integration at system level and energy substitution in CaC_(2) *** though the BCCA process showed lower carbon efficiency and energy efficiency than that of the CCCA process,life cycle assessment demonstrated the BCCA(1.873 kgCO_(2eq) kg-prod^(-1))a lower carbon footprint process which is 0.366 kgCO_(2eq) kg-prod^(-1) lower compared to the CCCA *** sustainable energy(biomass power)substitution in CaC_(2) furnace,an even lower GWP value of 1.377 kgCO_(2eq) kg-prod^(-1) can be achieved in BCCA *** work performed a systematic analysis on integrating biomass into industrial acetylene production,and revealed the positive role of biomass as raw material(carbon)and energy supplier.

关键词： Biomass pyrolysis CO_(2)mitigation Calcium carbide Acetylene Calcium loop

Tungsten oxide/nitrogen-doped carbon nanotubes composite catalysts for enhanced redox kinetics in lithium-sulfur batteries

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Chinese Journal of chemical engineering 2024年第3期67卷 58-67页

作者： Deqing He Zihao Xie Qian Yang Wei Wang Chao Su School of Energy and Power Jiangsu University of Science and TechnologyZhenjiang 212100China state key laboratory of Materials-Oriented chemical engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China

The sluggish redox kinetics of polysulfides in lithium-sulfur(Li-S)batteries are a significant obstacle to their widespread adoption as energy storage ***,recent studies have shown that tungsten oxide(WO_(3))can facilitate the conversion kinetics of polysulfides in Li-S ***,we fabricated host materials for sulfur using nitrogen-doped carbon nanotubes(N-CNTs)and WO_(3).We used low-cost components and simple procedures to overcome the poor electrical conductivity that is a disadvantage of metal *** composites of WO_(3) and N-CNTs(WO_(3)/N-CNTs)create a stable framework structure,fast ion diffusion channels,and a 3D electron transport network during electrochemical reaction *** a result,the WO_(3)/N-CNT-Li2S6 cathode demonstrates high initial capacity(1162 mA·h·g^(-1) at 0.5℃),excellent rate performance(618 mA·h·g^(-1) at 5.5℃),and a low capacity decay rate(0.093%up to 600 cycles at 2℃).This work presents a novel approach for preparing tungsten oxide/carbon composite catalysts that facilitate the redox kinetics of polysulfide conversion.

关键词： Li-S batteries Composites Ion diffusion channels 3D electron transport network Redox kinetics

Recent advances in the microfluidic generation of shape-controllable hydrogel microparticles and their applications

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Green chemical engineering 2024年第1期5卷 16-30页

作者： Yingzhe Liu Zhuo Chen Jianhong Xu The state key Lab of chemical engineering Department of Chemical EngineeringTsinghua UniversityBeijing100084China

Hydrogel microparticles,generally accepted as significant green materials,have been widely used in chemical,biological,and biomedical fields owing to their excellent biocompatibility,biodegradability,and *** these,non-spherical hydrogel microparticles with diverse shape anisotropy have great potential in applications such as drug delivery,cellular interaction,micromotors,*** from their shapes,their functionalities in such fields cannot be satisfied by the typical spherical ***,microfluidics with precise control and domination of fluids at microflow sizes has emerged as a powerful method for synthesizing shape-controllable hydrogel microparticles with good monodispersity and unique *** this review,we tried to provide an overview of the production of non-spherical microparticles composed of green hydrogel materials,emphasizing the microfluidic ***,a brief introduction to their current applications is also presented.

关键词： Microfluidics Hydrogel Microparticles Non-spherical Anisotropic Green materials

Mitochondrial sensitive probe with aggregation-induced emission characteristics for early brain diagnosis of Parkinson’s disease

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Aggregate 2024年第1期5卷 216-227页

作者： Liwen Huang Yutong Zhou Di Jiao Jing Ren Yilin Qi Heping Wang Yang Shi Dan Ding Xue Xue state key laboratory of Medicinal chemical Biology College of PharmacyNankai UniversityTianjinP.R.China state key laboratory of Medicinal chemical Biology Key Laboratory of Bioactive MaterialsMinistry of Educationand College of Life SciencesNankai UniversityTianjinP.R.China

The early diagnosis of Parkinson’s disease(PD)provides opportunities for early intervention to slow the progression of neurological degeneration in patients,particularly as the aging population increases in our *** a series of pathological features of PD,mitochondria abnormalities have been identified as central event that occurs at the early stage of ***,the method for detecting mitochondrial abnormalities-associated early PD has not been fully *** herein report a specifically mitochondrial targeting probe(named TPA-BT-SCP)that is able to characterize mitochondria abnormalities for early diagnosis of PD and monitor PD neurodegenerative *** probe is an aggregation-induced emission(AIE)probe with a strong positive charge,a 3D distorted molecular structure,and a separated HOMO-LUMO distribution,designed with unique molecular design *** research demonstrated that TPA-BT-SCP could emit stable and strong fluorescence,and rapidly accumulate in mitochondria due to the negative *** intranasal administration of 1-methy-4-phenyl-1,2,3,6-tetrahydropyridine(MPTP)-induced PD mice,TPA-BT-SCP successfully bypassed the blood−brain barrier to light up the brain,allowing the grading of PD severity based on its high *** together,this work develops a novel AIE probe that exhibits dramatically high sensitivity to mitochondrial changes and enables noninvasive diagnosis of early PD in the brain.

关键词： aggregation-induced emission early diagnosis Parkinson’s disease

Flower-like tin oxide membranes with robust three-dimensional channels for efficient removal of iron ions from hydrogen peroxide

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Chinese Journal of chemical engineering 2024年第1期65卷 1-7页

作者： Risheng Shen Shilong Li Yuqing Sun Yuan Bai Jian Lu Wenheng Jing state key laboratory of Materials-Oriented chemical engineering Nanjing Tech UniversityNanjing 210009China National Energy Group Science and Technology Research Institute Co. Ltd.Nanjing 210023China

Membrane technology has become the mainstream process for the production of electronic grade hydrogen peroxide(H_(2)O_(2)).But due to the oxidation degradation of the organic membranes(***)by the strong oxidative radicals(e.g.OH)generated via the activation of H_(2)O_(2)by iron ions(Fe^(3+)),the short effective lifetime of membranes remains a *** nano tin oxide(SnO_(2))has great potential for the removal of Fe^(3+)in strongly oxidative H_(2)O_(2)because of its ability to stabilize H2O_(2)and preferentially adsorb Fe^(3+).Herein,we have designed for the first time a flower-like robust SnO_(2)membrane on the ceramic support by in situ template-free one-step hydrothermal *** three-dimensional loose pore structure in the membrane built by interlacing SnO_(2)nanosheets endows the SnO_(2)membrane with a high specific surface area and abundant adsorption sites(AOH).Based on the coordination complexation and electrostatic attraction between the SnO_(2)surface and Fe^(3+),the membrane shows a high Fe3+removal efficiency(83%)and permeability(24 L·m^(-2)·h^(-1)·MPa^(-1))in H_(2)O_(2).This study provides an innovative and simple approach to designing robust SnO_(2)membranes for highly efficient removal of Fe^(3+)in harsh environments,such as strong oxidation conditions.

关键词： Hydrogen peroxide SnO_(2)membrane Adsorption Hydrothermal

Dendrimer-induced synthesis of porous organosilica capsules for enzyme encapsulation

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Frontiers of chemical Science and engineering 2024年第4期18卷 41-48页

作者： Ziyi Chu Boyu Zhang Zhenhua Wu Jiaxu Zhang Yiran Cheng Xueying Wang Jiafu Shi Zhongyi Jiang School of Environmental Science&engineering Tianjin UniversityTianjin 300072China Collaborative Innovation Center of chemical Science and engineering Tianjin 300072China state key laboratory of Biochemical engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China key laboratory for Green chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Organic matter-induced mineralization is a green and versatile method for synthesizing hybrid nanostructured materials,where the material properties are mainly influenced by the species of natural biomolecules,linear synthetic polymer,or small molecules,limiting their ***,we adopted dendrimer poly(amidoamine)(PAMAM)as the inducer to synthesize organosilica-PAMAM network(OSPN)capsules for mannose isomerase(MIase)encapsulation based on a hard-templating *** structure of OSPN capsules can be precisely regulated by adjusting the molecular weight and concentration of PAMAM,thereby demonstrating a substantial impact on the kinetic behavior of the MIase@OSPN *** MIase@OSPN system was used for catalytic production of mannose from Dfructose.A mannose yield of 22.24% was obtained,which is higher than that of MIase in organosilica network capsules and similar to that of the free *** overall catalytic efficiency(kcat/Km)of the MIase@OSPN system for the substrate D-fructose was up to 0.556 s^(-1)·mmol^(-1)·***,the MIase@OSPN system showed excellent stability and recyclability,maintaining more than 50% of the yield even after 12 cycles.

关键词： enzyme immobilization enzyme catalysis organosilica networks capsules sugar biosynthesis