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Chinese Chemical Letters 2024年第4期35卷 193-198页

作者： Tingting Liu Pengfei Sun Wei Zhao Yingshuang Li Lujun Cheng Jiahai Fan Xiaohui Bi Xiaoping Dong college of Chemistry and Chemical Engineering Zhejiang Sci-Tech UniversityHangzhou 310018China college of Environmental Science and Engineering Nankai UniversityTianjin 300071China Hangzhou Kaiming catalyst co. Ltd.Hangzhou 310013China

Mg-doped manganese oxide octahedral molecular sieve(Mg-OMS-2)catalysts were prepared by hydrothermal *** photothermal degradation performance of these catalysts for formaldehyde(HCHO)in batch system and continuous system was *** light absorption of OMS-2 was increased by Mg-doped,especially for near infrared light,which promoted surface temperature reach a maximum of 214.8℃ under xenon *** this temperature,the reinforced surface lattice oxygen and oxygen vacancy that formed by lattice distortion via Mg-doped were *** best HCHO elimination efficiency was achieved over Mg_(0.2)/OMS-2 catalyst with Mg^(2+)/Mn^(2+)=1/5,which could reduce HCHO from 250 ppm to 10 ppm within 20 *** in situ DRIFTS was also carried out to monitor the changes in the content of reaction intermediates and analyze the degradation paths of *** was found the HCHO was attacked by formed·OH and·O^(2-) to generate formate species and carbonate species,and finally transformed to co_(2) and H_(2)*** photothermal catalytic oxidation process exhibited a high efficiency purification of HCHO without the help of extra energy consumption.

关键词： Mg doping Photothermal catalysis OMS-2 HCHO Reaction mechanism

Development and Catalytic Cracking Performance of Ultrastable Y Zeolite Rich in Secondary Pores

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China Petroleum Processing & Petrochemical Technology 2024年第2期26卷 13-21页

作者： Li Jiaxing Wang Shengji Sha Hao Wang Juan Zhou Lingping Wang Lixia SINOPEC Research Institute of Petroleum Processing co. LtdBeijing 100083China catalyst co. Ltd.Qilu BranchSINOPECZibo 255336China

A novel ultra-stable zeolite, NSZ, rich in secondary pores was developed through the combination of gas-phase andmild hydrothermal methods. This zeolite was successfully tested in an industrial setting for the first time in the world. The porestructure characteristics of the NSZ zeolite prepared for industrial use were analyzed and characterized using BET. The resultsindicate a significant increase in the secondary pore volume of NSZ zeolite compared to the existing ultra-stable zeolite HSZ-5, which is produced through a conventional gas-phase method. The average secondary pore volume to total pore volume ratioin NSZ zeolite was found to be 58.96% higher. The catalytic cracking performance of NSZ zeolite was evaluated. The resultsshowed that the NSC-LTA catalyst, with NSZ as the active component, outperformed the HSC-LTA catalyst with HSZ-5 zeolitein terms of obtaining more high-value products (gasoline and liquefied petroleum gas) during the hydrogenated light cycle oilprocessing. Additionally, the NSC-LTA catalyst showed a significant improvement in coke selectivity.

关键词： gas-phase ultra-stable zeolite catalyst catalytic cracking

The Formation of SO_(2) and Emission Reduction Solutions in the Preparation of a Hydrogenation catalyst Support

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China Petroleum Processing & Petrochemical Technology 2024年第1期26卷 98-106页

作者： Hu Anpeng Wang Zhen Yang Qinghe Hu Dawei Gong Yu Jia Yanzi Dai Qiaoling Pu Ning SINOPEC Research Institute of Petroleum Processing Beijing 100083China Zibo Qimao catalyst co. Ltd.Zibo 255400China

The key reason for SO_(2) formation during the production of a residue hydrogenation catalyst support was identified and subsequent emission reduction solutions were then investigated and verified *** results demonstrated that carbon-containing organic materials,including sesbania powder and cellulose,did not completely decompose over the temperature range of 350−600℃during the heating stage of the calcination process,but rather underwent a condensation reaction within the same temperature range to form carbon-containing species with a lower ratio of hydrogen to carbon and a higher condensation degree,which promoted the decomposition of sulfate to form SO_(2).Systematic experimental work revealed that three different measures,i.e.,applying the staged calcination method,reducing the heating rate,and increasing the air flow rate,during the calcination process could all achieve the effect of reducing SO_(2) emissions.

关键词： alumina sesbania powder cellulose sulfur dioxide

Facile synthesis of hierarchical NaX zeolite from natural kaolinite for efficient Knoevenagel condensation

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Chinese Journal of Chemical Engineering 2024年第1期65卷 75-84页

作者： Wen Xiao Peng Dong Chan Wang Jingdong Xu Tiesen Li Haibo Zhu Tinghai Wang Renwei Xu Yuanyuan Yue National Engineering Research Center of Chemical Fertilizer catalyst College of Chemical EngineeringFuzhou UniversityFuzhou 350108China Qingyuan Innovation Laboratory Quanzhou 362801China Sinochem Quanzhou Energy Technology co. Ltd.Quanzhou 362000China

Zeolite catalysts have found extensive applications in the synthesis of various fine ***,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic ***,we explore an economic and environmentally friendly method for synthesizing hierarchical NaX zeolite that exhibits improved catalytic performance in the Knoevenagel condensation reaction for producing the useful fine chemical *** synthesis was achieved via a low-temperature activation of kaolinite and subsequent in-situ transformation strategy without any template or *** characterizations reveal that the synthesized NaX zeolite has both intercrystalline and intra-crystalline mesopores,smaller crystal size,and larger external specific surface area compared to commercial NaX *** mechanism investigations show that the inter-crystalline mesopores are generated by stacking smaller crystals formed from in-situ crystallization of the depolymerized kaolinite,and the intra-crystalline mesopores are inherited from the pores in the depolymerized *** synthesis strategy provides an energy-saving and effective way to construct hierarchical zeolites,which may gain wide applications in fine chemical manufacturing.

关键词： Hierarchical NaX zeolite Template-free synthesis Natural kaolinite Knoevenagel condensation

Electrochemical conversion of organic compounds and inorganic small molecules

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Science China Chemistry 2024年第10期67卷 3223-3246页

作者： Weimei Zeng Youai Qiu Department of Chemistry Nankai UniversityTianjin 300071China

Electrochemical synthesis presents a facile and sustainable strategy to produce valuable *** review summarizes the most recent advances in electrosynthesizing value-added compounds with inorganic small ***“small molecules”refers to a broad spectrum of chemicals,we mainly focus on the electrochemical conversion of co_(2),H_(2)O/D_(2)O,NH_(3)and SO_(2)until March *** review intends to compare the results and display general trends throughout the field,with an emphasis on the substrate scope and mechanical ***,we propose several techniques and protocols that can enable a more fundamental understanding of the electrochemical reaction involving inorganic small molecules and help drive this methodology toward commercialization.

关键词： electrochemical synthesis inorganic small molecule organic synthesis carbon dioxide water

Density-Functional Theories for Polyelectrolyte Systems

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Chinese Journal of Polymer Science 2024年第9期42卷 1302-1312,I0006页

作者： Jia-Wei Zhang Yu-Hang Zhang Bao-Hui Li Qiang Wang School of Physics Nankai UniversityTianjin90001China Department of Chemical and Biological Engineering Colorado State University1370 Campus DeliveryFort CollinsCO80523-1370USA

Polymer density-functional theories(PDFTs)have distinct advantages in the study of polyelectrolyte(PE)systems over experiments and molecular *** we give an introductory review of some PDFTs recently developed for PE *** start with a general formalism of PDFTs and its relation to the widely used polymer self-consistent field theory(SCFT),then explain the various correlations that are neglected in SCFT but can be accounted for in PDFTs,including those due to the excluded-volume interaction and chain connectivity of uncharged polymers,the electrostatic correlations of small ions,and the chain correlations in *** also list some applications of PDFTs for PE systems,and finally give some perspectives on future *** hope that our review can attract more researchers to apply and further develop PDFTs as a promising class of theoretical and computational tools.

关键词： Polymer density-functional theories Polyelectrolytes correlations

Highly efficient photocatalytic conversion of co_(2) into CH_(4) over Cu single atom promoted heterojunction:The effect of uplifted d-band center

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Chinese Chemical Letters 2024年第2期35卷 484-488页

作者： Hao Zhang Qian Liu Zhurui Shen School of Materials Science and Engineering Nankai UniversityTianjin 300350China

Photoreduction of co_(2) to solar fuels has caused great interest,but suffers from low catalytic efficiency and poor ***,we designed a S-scheme heterojunction(Cu-TiO_(2)/WO_(3))with Cu single atom to significantly boost the photoreduction of co_(2).Notably,the developed Cu-TiO_(2)/WO_(3) achieved the solardriven conversion of co_(2) to CH_(4) with an evolution rate of 98.69μmol g^(−1) h^(−1),and the electron selectivity of CH_(4) reached 88.5%.The yield was much higher than those of pristine WO_(3),TiO_(2)/WO_(3) and Cu-TiO_(2) *** and theoretical analysis suggested that the S-scheme heterojunction accelerated charge migration and inhibited the recombination of electron-hole ***,the charge separation effect of the heterojunction meliorated the position of the *** uplifted d-band centers of Cu and Ti on Cu-TiO_(2)/WO_(3) not only improved the electron interaction between Cu single atoms and substrate-TiO_(2),accelerated the adsorption and activation of co_(2) on the active sites of Cu single atom,but also optimized the Gibbs free energies of CH 4 formation pathway,leading to excellent selectivity toward CH_(4).This work provides new insights into the design of photocatalyst systems with high photocatalytic performance.

关键词： Cu single atom Heterojunction co_(2)photoreduction d-band center DFT

5S-Heudelotinone alleviates experimental colitis by shaping the immune system and enhancing the intestinal barrier in a gut microbiota-dependent manner

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Acta Pharmaceutica Sinica B 2024年第5期14卷 2153-2176页

作者： Qing Meng Jianshuang Guo Ke Lv Yang Liu Jin Zhang Mingyue Li Xirui Cheng Shenghua Chen Xiaoguang Huo Quan Zhang Yue Chen Jing Li State Key Laboratory of Medicinal Chemical Biology College of PharmacyNankai UniversityTianjin 300353China college of Chemistry and Frontiers Science Center for New Organic Matter Haihe Laboratory of Sustainable Chemical TransformationsNankai UniversityTianjin 300071China Accendatech company Ltd.Tianjin 300193China

Aberrant changes in the gut microbiota are implicated in many diseases,including inflammatory bowel disease(IBD).Gut microbes produce diverse metabolites that can shape the immune system and impact the intestinal barrier integrity,indicating that microbe-mediated modulation may be a promising strategy for preventing and treating *** fecal microbiota transplantation and probiotic supplementation are well-established IBD therapies,novel chemical agents that are safe and exert strong effects on the gut microbiota are urgently ***,we report the total synthesis of heudelotinone and the discovery of 5S-heudelotinone(an enantiomer)as a potent agent against experimental colitis that acts by modulating the gut microbiota.5S-Heudelotinone alters the diversity and composition of the gut microbiota and increases the concentration of short-chain fatty acids(SCFAs);thus,it regulates the intestinal immune system by reducing proinflammatory immune cell numbers,and maintains intestinal mucosal integrity by modulating tight junctions(TJs).Moreover,5S-heudelotinone(2)ameliorates colitis-associated colorectal cancer(CAC)in an azoxymethane(AOM)/dextran sulfate sodium(DSS)-induced in situ carcinoma ***,these findings reveal the potential of a novel natural product,namely,5S-heudelotinone,to control intestinal inflammation and highlight that this product is a safe and effective candidate for the treatment of IBD and CAC.

关键词： 5S-heudelotinone Total synthesis Inflammatory bowel disease Gut microbiota Short-chain fatty acids Immune system Intestinal barrier Drug discovery

How Does the Government Facilitate the co-Production of Digital Public Safety Services?——Based on Empirical Evidence from Shenzhen

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Social Sciences in China 2024年第2期45卷 113-134页

作者： Wu Xiaolin Zhou Enlai School of Government Nankai University

The application of big data technology provides support for the co-production of public safety *** research often focuses on how technology influences co-production,but lacks attention to the key actors that drive co-production and the mechanisms that facilitate *** study examines the role of government in the digital co-production of public safety services,using the practice of Shenzhen as a case *** has built 125 information systems based on over 100 billion pieces of big data,forming a model of digital safety service *** study reveals three types of digital co-production,characterized by"government-business joint planning,passive participation of businesses and the public,and active cooperation among government,businesses,and the public"in the"design-production-application"*** study shows that the government is not only a co-producer but also a proactive actor in activating the willingness of non-governmental entities to *** governments mobilize non-governmental participation through three mechanisms:empowerment,profit enhancement,and value ***"power-interest-value"paradigm is applicable for analyzing the co-production of public services and helps to explain the transformation mechanisms of co-production behavior.

关键词： public safety co-production smart emergency response digital public safety

Kinetic Resolution of Racemic 4-Substituted Chroman-2-ones Through Asymmetric Lactone Hydrogenation

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CCS Chemistry 2024年第10期6卷 2560-2576页

作者： Xiong Wu Hai-Tao Yue Xiao-Dong Zuo Xiao-Hui Yang Pu-Cha Yan Jian-Hua Xie Qi-Lin Zhou State Key Laboratory and Institute of Elemento-Organic Chemistry College of ChemistryFrontiers Science Center for New Organic MatterNankai UniversityTianjin 300071 Zhejiang Jiuzhou Pharmaceutical co. Ltd.TaizhouZhejiang 318000

Esters are abundant in natural and synthetic products and their conversion into primary alcohols holds great importance in fine chemical ***,achieving asymmetric hydrogenation(AH)of racemic esters with remote stereocenters via kinetic resolution(KR)remains a formidable challenge due to the difficulties associated with discerning spatially distant *** address this issue,we have designed a hydroxy-assisted strategy that introduces a hydroxy group into racemicβ-aryl esters to facilitate hydrogenation and enhance chiral discrimination through a lactone *** employing chiral Ir-SpiroPAP catalysts,we achieved exceptional AH of racemic 4-substituted chroman-2-ones,lactone form of ortho-hydroxylatedβ-aryl esters,via KR,resulting in impressive selectivity factor(s)values of up to *** approach exhibited significant efficacy for racemic chroman-2-ones containingβ-aryl,alkenyl,alkynyl,and alkyl groups,enabling the synthesis of chiralγ-aryl primary alcohols and the recovery of chiralβ-aryl esters or chroman-2-ones,typically difficult to access using existing *** scalability and broad synthetic applications of this method were exemplified by successfully synthesizing chiral drugs(R)-fesoterodine and enrasentan,alongside various chiral intermediates essential for producing chiral drugs and natural *** promising results highlight the potential of this approach as a powerful tool for synthesizing valuable chiral compounds.

关键词： asymmetric hydrogenation chiralγ-aryl primary alcohols hydrogenation of esters iridium catalysts kinetic resolution