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Photoinduced transposed Paternò-Büchi reaction for effective synthesis of high-performance jet fuel

Chinese Journal of chemical engineering 2024年第3期67卷 39-48页

作者： Jinxiu Hu Xianlong Liu Yi Liu Kang Xue Chengxiang Shi Xiangwen Zhang Li Wang Ji-Jun Zou Lun Pan Key Laboratory for Green Chemical Technology of the Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China Zhejiang Institute of Tianjin University Ningbo 315201China Collaborative Innovative Center of Chemical Science and Engineering(Tianjin) Tianjin 300072China

High-energy-density fuels are important for volume-limited aerospace vehicles,but the increase in fuel energy density always leads to poor cryogenic ***,we investigated the transposed Paternò-Büchi reaction of biomass cyclic ketone and cyclic alkene to synthesize a new kind of alkyl-substituted polycyclic hydrocarbon fuel with high energy density and good cryogenic *** triplet-energy-quenching results and phosphorescent emission spectra reveal the sensitization mechanism of the reaction,including photosensitizer excitation,triplettriplet energy transfer,cyclization,and relaxation,and the possible reaction path was revealed by the density functional theory(DFT)*** reaction conditions of photosensitizer type and addition,molar ratio of substrates,reaction temperature,and incident light intensity were optimized,with the target product yield achieving 65.5%.Moreover,the reaction dynamics of the reaction rate versus the light intensity are *** the hydrogenation-deoxygenation reaction,three fuels with a high density of 0.864-0.938 g·ml^(-1) and a low freezing point of<-55℃ are *** work provides a benign and effective approach to synthesize high-performance fuels.

关键词： High-energy-density fuel Transposed Patern-oeBüchi reaction Kinetics Bioenergy Photochemistry

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Cross-upgrading of biomass hydrothermal carbonization and pyrolysis for high quality blast furnace injection fuel production:Physicochemical characteristics and gasification kinetics analysis

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International Journal of Minerals,Metallurgy and Materials 2024年第2期31卷 268-281页

作者： Han Dang Runsheng Xu Jianliang Zhang Mingyong Wang Jinhua Li State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China School of Chemical Engineering The University of QueenslandQueensland 4072Australia

The paper proposes a biomass cross-upgrading process that combines hydrothermal carbonization and pyrolysis to produce high-quality blast furnace injection *** results showed that after upgrading,the volatile content of biochar ranged from 16.19%to 45.35%,and the alkali metal content,ash content,and specific surface area were significantly *** optimal route for biochar pro-duction is hydrothermal carbonization-pyrolysis(P-HC),resulting in biochar with a higher calorific value,C=C structure,and increased graphitization *** apparent activation energy(E)of the sample ranges from 199.1 to 324.8 kJ/mol,with P-HC having an E of 277.8 kJ/mol,lower than that of raw biomass,primary biochar,and *** makes P-HC more suitable for blast furnace injection ***,the paper proposes a path for P-HC injection in blast furnaces and calculates potential environmental benefits.P-HC of-fers the highest potential for carbon emission reduction,capable of reducing emissions by 96.04 kg/t when replacing 40wt%coal injec-tion.

关键词： blast furnace injection biomass cross-upgrading hydrothermal carbonization pyrolysis physicochemical properties gasific-ation properties

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Oxygen-deficient tungsten oxide nanoflowers for dynamically tunable near-infrared light transmittance of smart windows

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Nano Research 2023年第10期16卷 12165-12172页

作者： Ya Huang Baoshun Wang Pei Lyu Siming Zhao Xueke Wu Shiliang Zhang Run Li Qinyuan Jiang Fei Wang Yanlong Zhao Rufan Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

Electrochromic smart windows have attracted much attention in energy-saving buildings because of their ability to selectively modulate visible(VIS)and near-infrared(NIR)light *** is known,the NIR region accounts for about 50%of the total solar ***,reducing the NIR transmittance of windows will play a crucial role in reducing the energy consumption of ***,for most of the reported electrochromic materials(ECMs)-based windows,it remains a longlasting challenge about how to achieve a low NIR transmittance during the past *** this work,we synthesize oxygendeficient tungsten oxide(WO_(3−x))nanoflowers(NFs)by a simple and efficient method that is facile for their mass *** WO_(3−x)NFs exhibit low NIR transmittance of only 4.11%,0.60%,and 0.19%at 1200,1600,and 1800 nm,respectively,due to the localized surface plasmon resonance(LSPR)***,the WO_(3−x)NFs exhibit an excellent dual-band modulating ability for both VIS and NIR *** are able to operate in three distinct modes,including a bright mode,a cool mode,and a dark ***,the WO_(3−x)NFs exhibit a fast bleaching/coloring time(1.54/6.67 s),and excellent cycling stability(97.75%of capacity retention after 4000 s).

关键词： electrochromic tungsten oxide dual-band smart window infrared

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Green microfluidics in microchemical engineering for carbon neutrality

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Chinese Journal of chemical engineering 2023年第1期53卷 332-345页

作者： Qingming Ma Jianhong Xu School of Pharmacy Qingdao UniversityQingdao 266021China The State Key Laboratory of Chemical Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

The concept of“carbon neutrality”poses a huge challenge for chemical engineering and brings great opportunities for boosting the development of novel technologies to realize carbon offsetting and reduce carbon *** high-efficient,low-cost,energy-efficient and eco-friendly microfluidicbased microchemical engineering is of great *** kind of“green microfluidics”can reduce carbon emissions from the source of raw materials and facilitate controllable and intensified microchemical engineering processes,which represents the new power for the transformation and upgrading of chemical engineering ***,a brief review of green microfluidics for achieving carbon neutral microchemical engineering is presented,with specific discussions about the characteristics and feasibility of applying green microfluidics in realizing carbon *** of green microfluidic systems are categorized and reviewed,including the construction of microfluidic devices by bio-based substrate materials and by low carbon fabrication methods,and the use of more biocompatible and nondestructive fluidic systems such as aqueous two-phase systems(ATPSs).Moreover,low carbon applications benefit from green microfluidics are summarized,ranging from separation and purification of biomolecules,high-throughput screening of chemicals and drugs,rapid and cost-effective detections,to synthesis of fine chemicals and novel ***,challenges and perspectives for further advancing green microfluidics in microchemical engineering for carbon neutrality are proposed and discussed.

关键词： Microchemical engineering Carbon neutrality Microfluidics Aqueous two-phase systems(ATPSs) Environment chemical processes

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Multistep continuous flow synthesis of Erlotinib

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Chinese chemical Letters 2024年第4期35卷 371-375页

作者： Hui Jin Qin Cai Peiwen Liu Yan Chen Derong Wang Weiping Zhu Yufang Xu Xuhong Qian State Key Laboratory of Bioreactor Engineering Shanghai Key Laboratory of Chemical BiologySchool of PharmacyEast China University of Science and TechnologyShanghai 200237China

Erlotinib is an orally administered, highly effective, specific epidermal growth factor receptor tyrosine kinase inhibitor, used to treat non-small cell lung cancer and pancreatic cancer. The traditional synthetic methods for Erlotinib exhibit long reaction time and safety concern. Herein, we describe a novel five-step route for the synthesis of Erlotinib in flow. These five steps comprise etherification, nitration, reduction,addition and cyclization reactions. All steps were optimized and converted to continuous flow process,which drastically reduces the reaction time and considerably improves the process safety as well as the total yield. Enabled by five continuous flow units, Erlotinib is efficiently afforded with an E-factor of 38,an overall yield of 83%, and a total residence time of 25.1 min. Majority steps in this process have been optimized for quantitative conversion, which offers the possibility of telescoping the entire process.

关键词： Erlotinib Continuous flow synthesis Microchannel flow reactor Process optimization Continuous nitration Continuous hydrogenation

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Study on trifluoromethanesulfonic acid-promoted synthesis of daidzein: Process optimization and reaction mechanism

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Chinese Journal of chemical engineering 2024年第7期71卷 132-139页

作者： Hai Cao Haibin Yang Yanxiong Fang Yuandi Zeng Xiaolan Cai Jingjing Ma School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006China Jieyang Branch of Chemistry and Chemical Engineering Guangdong Laboratory(Rongjiang Laboratory) Jieyang 515200China

Daidzein has been widely used in pharmaceuticals,nutraceuticals,cosmetics,feed additives,*** preparation process and related reaction mechanism need to be further investigated.A cost-effective process for synthesizing daidzein was developed in this *** this article,a two-step synthesis of daidzein(Friedel–Crafts acylation and[5+1]cyclization)was developed via the employment of trifluoromethanesulfonic acid(TfOH)as an effective promoting *** effect of reaction conditions such as solvent,the amount of TfOH,reaction temperature,and reactant ratio on the conversion rate and the yield of the reaction,respectively,was systematically investigated,and daidzein was obtained in 74.0%isolated yield under optimal *** to the facilitating effect of TfOH,the Friedel–Crafts acylation was completed within 10 min at 90℃ and the[5+1]cyclization was completed within 180 min at 25℃.In addition,a possible reaction mechanism for this process was *** results of the study may provide useful guidance for industrial production of daidzein on a large scale.

关键词： Synthesis Optimal design chemical processes Reaction mechanism

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An integrated technology for the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3)in a high-gravity environment

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Chinese Journal of chemical engineering 2024年第8期72卷 117-125页

作者： Kangrui Nie Ruize Shang Fuming Miao Liuxiang Wang Youzhi Liu Weizhou Jiao Shanxi Province Key Laboratory of Chemical Process Intensification and School of Chemistry and Chemical Engineering North University of ChinaTaiyuan 030051China

In this study,an integrated technology is proposed for the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3)in a high-gravity *** effects of absorbent type,high-gravity factor,gas/liquid ratio,and initial BaCl2concentration on the absorption rate and amount of CO_(2)and the preparation of BaCO_(3)are *** results reveal that the absorption rate and amount of CO_(2)follow the order of ethyl alkanolamine(MEA)>diethanol amine(DEA)>N-methyldiethanolamine(MDEA),and thus MEA is the most effective absorbent for CO_(2)*** absorption rate and amount of CO_(2)under high gravity are higher than that under normal ***,the absorption rate at 75 min under high gravity is approximately 2 times that under normal *** is because the centrifugal force resulting from the high-speed rotation of the packing can greatly increase gas-liquid mass transfer and *** particle size of BaCO_(3)prepared in the rotating packed bed is in the range of 57.2—89 nm,which is much smaller than that prepared in the bubbling reactor(>100.3 nm),and it also has higher purity(99.6%)and larger specific surface area(14.119 m^(2)·g^(-1)).It is concluded that the high-gravity technology has the potential to increase the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3).This study provides new insights into carbon emissions reduction and carbon utilization.

关键词： High-gravity technology Wet absorption CO_(2)capture Enhanced mass transfer CO_(2)utilization Barium carbonate

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Facile formation of hierarchical magnesium silicate hydrate microspheres as an adsorbent for the textile dyes

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Particuology 2024年第10期93卷 99-110页

作者： Tin Kyawoo Naveed Karim Chao Jiang Saeed Ahmed Weiliang Tian Huiyu Li Yongjun Feng State Key Laboratory of Chemical Resource Engineering Beijing Engineering Center for Hierarchical CatalystsBeijing University of Chemical TechnologyBeijing100029China Department of Chemistry The University of ChakwalChakwal48800Pakistan College of Chemistry and Chemical Engineering Tarim UniversityAlar843300China

Hierarchical porous magnesium silicate hydrate (MSH) microspheres composed of sheets are successfully developed under facile conditions using a hard template. The role of hexadecyltrimethylammonium bromide (CTAB) on the formation and adsorption behavior was also observed for the methyl orange and methylene blue. The formed MSH possesses a surface area of 453.24 m^(2)/g, an average pore size of 6.38 nm, and a pore volume of 0.75 cm^(3)/g without CTAB. Based on the role of CTAB and the change in the ratio of Mg/Si, the MSH retained its sphere-like structure with a variation in pore parameters. The formed MSH was used as an adsorbent to remove methylene blue and methyl orange. The pseudo-second-order kinetic and Langmuir Isotherm models are well-fitted, with a 256.4 mg/g removal capacity and 84.2 mg/g for methylene blue and methyl orange, respectively. The modified MSH with CTAB played a positive role for the methyl orange and a negative role for the methylene blue regarding removal performance.

关键词： Adsorption Hierarchical microspheres Magnesium silicate Methyl orange Methylene blue Surfacemodification

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Impact of Annealing on the Melt Recrystallization of a-PDLA/α-PLLA Double-layered Films

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Chinese Journal of Polymer Science 2024年第2期42卷 230-238,I0009页

作者： Yun-Peng Li Hao-Ran Shen Shao-Juan Wang Hao Zhang Jian Hu Rui Xin Xiao-Li Sun Shou-Ke Yan Key Laboratory of Rubber-Plastics Ministry of Education/Shandong Provincial Key Laboratory of Rubber-plasticsQingdao University of Science&TechnologyQingdao266042China State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing100029China

Poly(lactic acid)(PLA) as a bio-based polymer with biodegradability and biocompatibility has attracted much attention. To manipulate its properties for different applications, regulation of crystal structure and crystalline morphology becomes an attractive research topic. In this work, the structure evolution of layered samples containing an amorphous poly(D-lactide)(PDLA) layer and a crystalline poly(L-lactide)(PLLA)layer with highly oriented edge-on α lamellar crystals after annealing at 150 ℃ or/and after melt-recrystallization has been studied by AFM, FTIR,and TEM combined with electron diffraction. The results demonstrate that melt recrystallization of the as-prepared sample leads to the formation of abundant randomly oriented PLA stereo-complex(PLA SC) crystals. Annealing at 150 ℃ results in the formation of a small amount of oriented PLA SC crystals at the interface. These PLA SC crystals show great impact on the recrystallization behavior of sample after melting at 190 ℃ and then crystallizing at 90 ℃. First, they impede the mutual diffusion of the overlying PDLA and underlying PLLA, and thus reduce their stereocomplexation ability as manifested by the decreased amount of PLA SC crystals. Second, they act as substrate to initiate the epitaxial crystallization of the overlying PDLA and underlying PLLA, which ensures the production of a highly oriented structure of PDLA and PLLA after melt recrystallization again.

关键词： Poly(L-lactide) Poly(D-lactide) Double layer Stereocomplex

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Preparation and properties of poly(ethylene glycol)-bpoly( 3-acrylamidophenylboronic acid) glucose responsive particles and their hyaluronic acid-based microneedle patches

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Journal of Zhejiang University-Science A(Applied Physics & engineering) 2024年第5期25卷 395-410页

作者： Yichuan HONG Haojie YU Li WANG Xiang CHEN Di SHEN Yu WANG Shuning REN Yudi HUANG Jian YANG State Key Laboratory of Chemical Engineering College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310058China Zhejiang-Russia Joint Laboratory of Photo-Electro-Magnetic Functional Materials College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310058China

To overcome the pain and risk of hypoglycemia in insulin administration,glucose-responsive microneedles have been developed by researchers,which could release insulin according to the blood glucose *** designed a kind of particles by a reversible addition-fragmentation chain transfer(RAFT)method containing a phenylboronic acid group as the sensor of glucose and carrier of ***(ethylene glycol)(PEG)-2-(dodecylthio(thiocarbonyl)thio)-2-methylpropionic acid(DDMAT)was synthesized as a macromolecular RAFT agent,which was then reacted with 3-acrylamidophenylboronic acid(AAPBA)to synthesize the block copolymer ***-responsive particles loaded with insulin were prepared by self-assembly based on hydrophilic-hydrophobic *** patches loaded with glucose-responsive particles were prepared using hyaluronic acid as the *** insulin release behavior of the particles in glucose solutions of 0,100,and 400 mg/dL showed significant glucose responsiveness and good *** results of blood glucose control experiments in rats indicate that a single microneedle patch can effectively maintain normal blood glucose for over 7 h.

关键词： Diabetes Hyaluronic acid Phenylboronic acid(PBA) Glucose responsive hydrogel Microneedles

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