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Visible-Light-Mediated C(sp^3)-H Thiocarbonylation for Thiolactam Preparation with Potassium Sulfide

Chinese Journal of Chemistry 2019年第12期37卷 1234-1238页

作者： Wei Tan Cuihong Wang Xuefeng Jianga Shanghai Key Laboratory of Green Chemistry and Chemical Process School of Chemistry and Molecular EngineeringEast China Normal University3663 North Zhongshan RoadShanghai 200062China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of Sciences345 Lingling RoadShanghai 200032China

Summary of main observation and conclusion We report herein a protocol for thiolactam preparation with potassium sulfide via visible-light-mediated C(sp3)-H thiocarbonylation,in which polysulfide dianions and radical anions generated from potassium sulfide were the key active species.A variety of thiolactams were straightforward established under mild ***,it was successfully applied to structural modification of tetrahydroberberine.

关键词： conditions. sulfide potassium

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Electron trap-induced charge accumulation and surface reaction kinetics synergistically enhance overall nitrogen photofixation

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Chinese Chemical Letters 2025年第8期36卷

作者： Longjian Li Ping Zhang Yongchong Yu Reyila Tuerhong Xiaoping Su Lijuan Han Enzhou Liu Jizhou Jiang Key Laboratory of Environment-Friendly Composite Materials of the State Ethnic Affairs Commission Gansu Province Engineering Research Center for Biomass Functional Composite Materials Key Laboratory for the Utilization of Environment Friendly Composite Materials and Biomass in Universities of Gansu Province Gansu Province Research Center for Basic Sciences of Surface and Interface Chemistry College of Chemical Engineering Northwest Minzu University Lanzhou 730030 China Gansu Natural Energy Research Institute Gansu Academy of Science Lanzhou 730046 China School of Chemical Engineering Xi'an Key Laboratory of Special Energy Materials Northwest University Xi'an 710069 China School of Materials Science and Engineering Key Laboratory of Green Chemical Engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education Wuhan Institute of Technology Wuhan 430205 China

Available online Further oxidation of NH 3 produced via photocatalytic N 2 fixation represents a promising strategy to enhance the economic value of N 2 fixation. This work employs first-principles density functional theory (DFT) calculations to demonstrate that incorporating Co into NiO improves both N 2 adsorption and activation as well as M-N electron exchange intensity. Guided by these predictions, a novel Co single-atom photocatalyst supported by nanoconfined NiO@C nanosheets was synthesized using a direct metal atomization method, achieving high HNO 3 production (60.54 %). NH 4 + and NO 3 − production rates during N 2 photofixation reached 67.97 µmol g cat −1  h −1 and 104.28 µmol g cat −1  h −1 , respectively. The overall N 2  → NH 3  → HNO 3 photofixation pathway was validated through in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and 15 N isotopic labeling. Mechanistic studies reveal that Co single-atom introduction serves as an electron trap, enhancing photogenerated electron accumulation with a five-fold increase in carrier density compared to NiO@C, as observed via in-situ X-ray photoelectron spectroscopy (XPS). This synergistic effect between electron traps and N 2 adsorption/activation sites at Co single-atom centers supports rapid N 2 reduction kinetics. Additionally, nanoconfined ink-bottle pores in the carbon layer impede NH 3 desorption, further boosting NO 3 − production. This work offers a comprehensive approach to optimizing N 2 photofixation through electron regulation and surface reaction kinetics.

关键词： Co single-atom Electron trap N2 photofixation Nanoconfined NiO@C NO3− production

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Revealing global reaction mechanisms of polypropylene pyrolysis by reactive molecular dynamic simulation and reaction class prediction

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Polymer Degradation and Stability 2025年 239卷

作者： Li, Wenyao Zheng, Mo Li, Jiangang Ren, Chunxing Li, Xiaoxia College of New Materials and Chemical Engineering Beijing Institute of Petrochemical Technology Beijing 102617 China State Key Laboratory of Mesoscience and Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China Innovation Academy for Green Manufacture Chinese Academy of Sciences Beijing100190 China University of Chinese Academy of Sciences Beijing100049 China

Polypropylene (PP) pyrolysis offers a promising solution for transforming waste plastics into high-value chemicals. This work presents a combination approach of large-scale reactive molecular dynamic simulation (ReaxFF MD) and automatic reaction class prediction with machine learning method for investigating PP pyrolysis reaction mechanism. The reasonableness of the global reaction understanding on PP pyrolysis is supported by both the consistent representative pyrolyzate detections between experiments and simulation, as well as the same yield ranking of C3H6>C2H4>CH4>C2H6 at the initial decomposition dominant stage between experiments and simulations. The comprehension of the dynamic product profiles and their relevant reaction classes in polypropylene pyrolysis was revealed, which indicates that the major species distribution in PP pyrolysis detectable experimentally become explainable by the major reaction classes with the aid of automatic reaction classification approach of SRG-Reax, The dominant homolysis and β-scission reaction classes accounting for 30 %∼50 % in the initial PP pyrolysis corresponds to the rapid increasing yields of C2H4 and C3H6. The increasing reaction classes of ring opening & recombination and chain cyclization as well as of intra-molecular H-shift, H detachment and inter-molecular H-abstraction should be responsible for the increasing ring formation of 5-membered, 6-membered, 7-membered rings, particularly for formation of aryl rings and naphthalene with temperature. The formation pathways of benzene, naphthalene and anthracene were unraveled. The mechanism understanding of PP pyrolysis demonstrate the potential of the combined simulation strategy of large-scale simulation and reaction class prediction in deepening understanding polymer degradation mechanism. © 2025

关键词： Ring opening polymerization

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Efficient Capture and Low Energy Release of NH3by Azophenol Decorated Photoresponsive Covalent Organic Frameworks

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Angewandte Chemie 2024年第34期136卷

作者： Xiaoxin Tian Xiao Zhao Zhenzhen Wang Yunlei Shi Zhiyong Li Jikuan Qiu Huiyong Wang Suojiang Zhang Jianji Wang Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals Key Laboratory of Green Chemical Media and Reactions Ministry of Education (China) School of Chemistry and Chemical Engineering Henan Normal University Xinxiang Henan 453007 P. R. China School of Chemistry and Materials Engineering Xinxiang University Xinxiang Henan 453003 P. R. China Beijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 P. R. China College of Chemistry and Molecular Sciences Longzihu New Energy Laboratory Henan University Zhengzhou Henan 450000 P. R. China

In NH 3 capture technologies, the desorption process is usually driven by high temperature and low pressure (such as 150–200 °C under vacuum), which accounts for intensive energy consumption and CO 2 emission. Developing light responsive adsorbent is promising in this regard but remains a great challenge. Here, we for the first time designed and synthesized a light responsive azophenol-containing covalent organic framework (COF), COF-HNU38, to address this challenge. We found that at 25 °C and 1.0 bar, the cis -COF exhibited a NH 3 uptake capacity of 7.7 mmol g −1 and a NH 3 /N 2 selectivity of 158. In the adsorbed NH 3 , about 29.0 % could be removed by vis-light irradiated cis-trans isomerization at 25 °C, and the remaining NH 3 might be released at 25 °C under vacuum. Almost no decrease in adsorption capacity was observed after eight adsorption-desorption cycles. As such, an efficient NH 3 capture and low energy release strategy was established thanks to the multiple hydrogen bond interactions (which are strong in total but weak in individuals) between NH 3 and the smart COF, as well as the increased polarity and number of hydrogen bond sites after the trans-cis isomerization.

关键词： ammonia capture Covalent Organic Framework (COF) photo switching azophenol

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Machine learning advancements in organic synthesis: A focused exploration of artificial intelligence applications in chemistry

Artificial Intelligence Chemistry

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Artificial Intelligence Chemistry 2024年第1期2卷

作者： Rizvi Syed Aal E Ali Jiaolong Meng Muhammad Ehtisham Ibraheem Khan Xuefeng Jiang State Key Laboratory of Molecular & Process Engineering School of Chemistry and Molecular Engineering East China Normal University 3663 North Zhongshan Road Shanghai 200062 China Green Chemistry Group School of Sciences and Technology Chemistry Division University of Camerino ChIP Research Center Via Madonna delle Carceri 62032 Camerino MC Italy State Key Laboratory of Estuarine and Coastal Research East China Normal University Shanghai 200241 China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic Chemistry Chinese Academy of Sciences Shanghai 200032 China

Artificial intelligence (AI) is driving a revolution in chemistry, reshaping the landscape of molecular design. This review explores AI’s pivotal roles in the field of organic synthesis applications. AI accurately predicts reaction outcomes, controls chemical selectivity, simplifies synthesis planning, accelerates catalyst discovery, and fuels material innovation and so on. It seamlessly integrates data-driven algorithms with chemical intuition to redefine molecular design. As AI chemistry advances, it promises accelerated research, sustainability, and innovative solutions to chemistry’s pressing challenges. The fusion of AI and chemistry is poised to shape the field’s future profoundly, offering new horizons in precision and efficiency. This review encapsulates the transformation of AI in chemistry, marking a pivotal moment where algorithms and data converge to revolutionize the world of molecules.

关键词： Artificial intelligence Chemical selectivity Retrosynthesis prediction Catalyst design Material design

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Correction to “Study on the Hydrocyclonic Separation of Natural Gas Hydrate Slurries Combined with the Solution of Particles’ Settling Equation”

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Industrial & engineering Chemistry Research 2023年第47期62卷 20470页

作者： Yuchen Qian Faqi Zhou Jun Xu Huixin Yuan Chong Peng School of Mechanical Engineering Changzhou University Changzhou 213164 Jiangsu China Jiangsu Key Laboratory of Green Process Equipment Changzhou 213164 Jiangsu China Sinopec Shanghai Research Institute of Petrochemical Technology Shanghai 201208 China State Key Laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology Dalian116024 China

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Vacuum-Assisted Confined Growth of MOF@COF Composite Membranes with Enhanced Hydrogen Permselectivity

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Angewandte Chemie 2024年第7期137卷

作者： Siqi Li Zheng Wan Chunxin Jin Jinlin Hao Dr. Yanhong Li Dr. Xiaofang Chen Prof. Dr. Jürgen Caro Prof. Dr. Aisheng Huang State Key Laboratory of Molecular & Process Engineering Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular Engineering East China Normal University 500 Dongchuan Road Shanghai 200241 China Institute of Physical Chemistry and Electrochemistry Leibniz University Hanover Callinstrasse 3A 30167 Hanover Germany Institute of Eco-Chongming 20 Cuiniao Road Chongming District Shanghai 202162 China

With ordered and periodic network structures, adjustable pore sizes and high chemical stability, covalent organic frameworks (COFs) have drawn much attention for the fabrication of superior separation membranes. However, it is challenging to prepare COF membranes with a molecular sieving property for gas separation due to their relatively large pore size. In this work, we develop the MOF-in-COF concept for vacuum-assisted synthesis of metal–organic framework (MOF) ZIF-8 inside the pores of TB-COF formed from trihydroxy-benzene-tricarbaldehyde (T) and diamino-biphenyl-disulfonic acid (B), thus constructing a novel ZIF-8@TB-COF membrane. Attributing to the formation of a well-defined one-dimensional (1D) nanoscale transport channel, the ZIF-8@TB-COF membrane displays a high hydrogen permselectivity. At 100 °C and 200 kPa, the mixture separation factors of H 2 /CO 2 , H 2 /CH 4 and H 2 /C 3 H 8 are 21.9, 63.1 and 134.4, respectively, which are much higher than those of the pristine TB-COF membrane due to the precise size sieving channels brought about by the incorporated MOF. The synthesis of ZIF-67@TB-COF membrane demonstrates the versatility of the synthesis strategy.

关键词： Molecular sieve membranes Covalent organic framework membranes Metal–organic framework membranes Confined growth MOF@COF composite

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Fluorinated solvent coupled anions-derived hybrid interphase enabled highly reversible and cryogenic silicon anode

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Journal of Colloid and Interface Science 2025年

作者： Chengxin Peng Xuhao Yang Wenjing Tang Suting Weng Liang Wang Zhou Zhang Bo Deng Ting Yi Weimin Zhao Jinchen Fan Huixin Chen Xuefeng Wang Shixue Dou Wei Tang School of Materials and Chemistry University of Shanghai for Science and Technology Shanghai 200093 China Tianjin Key Laboratory of Chemical Process Safety Hebei Provincial Key Laboratory of Green Chemical Technology and High Efficient Energy Saving School of Chemical Engineering and Technology Hebei University of Technology Tianjin 300130 China Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 China College of Automotive Engineering Yancheng Institute of Technology Yancheng Jiangsu 224051 China College of Chemical Engineering and Safety Shandong University of Astronautics Binzhou 256600 China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 Fujian China Shaanxi Key Laboratory of Energy Chemical Process Intensification School of Chemical Engineering and Technology Xi’an Jiaotong University Xi’an Shaanxi 710049 China

Silicon (Si) has emerged as a prominent candidate for high-energy batteries due to its exceptionally high theoretical capacity and favorable lithiation potential. However, its electrochemical performance at subzero temperatures is significantly hampered by slow ion transport and sluggish ion diffusion processes. Here, we present a weakly solvation electrolyte formulated with 1 M lithium bis(fluorosulfonyl)imide (LiFSI) in a mixture of fluoroethylene carbonate (FEC) / methyl trifluoroacetate (MTFA). This electrolyte is elaborated to enhances the ion desolvation process and facilitate the formation of an anion-coupled fluorinated solvent-derived hybrid solid electrolyte interphase (SEI) on Si anodes, thereby significantly improving the electrochemical performance. Comprehensive characterizations paired with molecular dynamics (MD) calculations reveal that the hybrid SEI consists of an organic outer layer and a lithium fluoride (LiF) and sulfurized species-rich inner layer, which maintain the structural integrity of the electrode while promoting rapid Li + diffusion even at cryogenic temperatures. As anticipated, the Si electrode demonstrates exceptional delivery capacities of approximately 3100–2600 mAh g −1 at subzero temperatures ranging from 0 °C to −20 °C, and a reversible specific capacity of around 2100 mAh g −1 even at −30 °C.

关键词：

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Aging amorphous/crystalline heterophase PdCu nanosheets for catalytic reactions

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National Science Review 2019年第5期6卷 955-961页

作者： Hongfei Cheng Nailiang Yang Xiaozhi Liu Qinbai Yun Min Hao Goh Bo Chen Xiaoying Qi Qipeng Lu Xiaoping Chen Wen Liu Lin Gu Hua Zhang Center for Programmable Materials School of Materials Science and EngineeringNanyang Technological University State Key Laboratory of Biochemical Engineering Institute of Process Engineering Chinese Academy of Sciences Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences School of Physical Sciences University of Chinese Academy of Sciences Singapore Institute of Manufacturing Technology A*STAR School of Materials Science and Engineering University of Science and Technology Beijing School of Chemical and Biomedical Engineering Nanyang Technological University Songshan Lake Materials Laboratory Department of Chemistry City University of Hong Kong

Phase engineering is arising as an attractive strategy to tune the properties and functionalities of *** particular, amorphous/crystalline heterophase nanostructures have exhibited some intriguing ***, the one-pot wet-chemical synthesis of two types of amorphous/crystalline heterophase Pd Cu nanosheets is reported, in which one is amorphous phase-dominant and the other one is crystalline *** the aging process of the synthesized Pd Cu nanosheets is studied, during which their crystallinity increases, accompanied by changes in some physicochemical *** a proof-of-concept application, their aging effect on catalytic hydrogenation of 4-nitrostyrene is *** a result, the amorphous phase-dominant nanosheets initially show excellent *** aging for 14 days, their catalytic activity is higher than that of crystalline phase-dominant *** work demonstrates the intriguing properties of heterophase nanostructures, providing a new platform for future studies on the regulation of functionalities and applications of nanomaterials by phase engineering.

关键词： amorphous/crystalline heterophase nanosheets aging selective hydrogenation catalysis

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A slippery liquid-infused porous surface with self-cleaning and liquid-repellent properties, long-term corrosion resistance, and high mechanical stability

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Colloids and Surfaces A: Physicochemical and engineering Aspects 2025年 723卷

作者： Ying Wang Ningbo Hu Yan Zhang Renguo Song Lin Liu Xiaobing Zhao Guanggui Cheng Ningyi Yuan Jianning Ding School of Materials Science and Engineering Jiangsu Collaborative Innovation Center for Photovoltic Science and Engineering Jiangsu Province Cultivation Base for State Key Laboratory of Photovoltaic Science and Technology Changzhou University Changzhou 213164 China Jiangsu Key Laboratory of Materials Surface Science and Technology Changzhou University Changzhou 213164 China School of Mechanical Engineering and Rail Transit Green Process Equipment Key Laboratory of Jiangsu Provincial Universities Changzhou University Changzhou 213164 China Micro/Nano Science and Technology Center Jiangsu University Zhenjiang 212013 China Institute of Technology for Carbon Neutralization Yangzhou University Yangzhou 225127 China

In this study, a simple and environmentally friendly micro-arc oxidation technology was used to prepare a slippery liquid-infused porous surface (SLIPS) on the surface of Ti alloy. The micro-arc oxidation treatment could effectively form micro-nano rough and porous morphology on the surface of Ti alloy. After Octadecyltrimethoxysilane treatment and dimethylsilicone oil injection, a SLIPS was successfully formed. The prepared SLIPS was hydrophobic, forming a uniform and smooth coating. Due to its excellent repulsion to the liquid medium, the SLIPS exhibited excellent self-cleaning and corrosion resistance. The corrosion current density of SLIPS was 5 orders of magnitude lower than that of Ti alloy, the corrosion potential was positively shifted by 1.194 V, and the impedance in the low frequency region was increased by 4 orders of magnitude. Furthermore, after immersion in 3.5 wt% NaCl solution for 4 weeks, impacting in simulated seawater for 7 days, and rubbing with sandpaper for 50 times, respectively, the SLIPS could still have good corrosion resistance, showing excellent long-term anti-corrosion properties and mechanical stability. The constructed interlocking structure and the lubricity of dimethylsilicone oil endowed it with high mechanical stability. It could be expected that the prepared slippery liquid-infused porous surface could be used to expand the practical application of traditional Ti alloy materials.

关键词： Oxidation resistance

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