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NiCo/Al_(2)O_(3)nanocatalysts for the synthesis of 5-amino-1-pentanol and 1,5-pentanediol from biomass-derived 2-hydroxytetrahydropyran

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Green Chemical Engineering 2024年第1期5卷 119-131页

作者： Jian Yang Jia Zhang Enrico Benassi Xuemei Li Hailong Liu Weiguo Fang Junying Tian Chungu Xia Zhiwei Huang State Key Laboratory for Oxo synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou730000China School of Petrochemical Engineering Lanzhou University of TechnologyLanzhou730050China Novosibirsk State University Novosibirsk630090Russia University of Chinese Academy of Sciences Beijing100049China

Al_(2)O_(3)-supported monometallic Ni,Co,and bimetallic Ni-Co nanocatalysts originated from layered double hydroxide precursors were synthesized by co-precipitation method,and used for the synthesis of useful 5-amino-1-pentanol(5-AP)and 1,5-pentanediol(1,5-PD)by reductive amination(RA)or direct hydrogenation of biofurfuralderived 2-hydroxytetrahydropyran(2-HTHP),*** both reactions,the yield of the target products decreased monotonously with the increasing amounts of Co in the NiCo/Al_(2)O_(3)catalysts,owing probably to the replacement of highly reactive Ni by Co component with inferior hydrogenation activity at the low reaction temperature of 60℃.However,the incorporation of Co could improve the reducibility of the NiCo/Al_(2)O_(3)bimetallic catalysts and promote the reaction stability of the catalysts,especially for Ni_(2)Co1/Al_(2)O_(3),in both reactions with over 180 h *** of the catalysts before and after the reaction showed that the incorporating Co could inhibit the sintering of metal particles and hinder the surface oxidation of the more reactive Ni0species,thanks to the formation of Ni-Co alloy in the bimetallic ***-based modeling of the reaction mechanisms is also performed,supporting the reaction pathway proposed previously and also the much higher activity of Ni in the RA of 2-HTHP as compared with Co.

关键词： NiCo bimetallic catalysts Layered double hydroxide Reductive amination Amino alcohol Quantum chemical calculations

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Recent applications of macrocycles in supramolecular catalysis

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Chinese Chemical Letters 2024年第4期35卷 132-141页

作者： Conghui Wang Lei Xu Zhenhua Jia Teck-Peng Loh College of Advanced Interdisciplinary Science and Technology Henan University of TechnologyZhengzhou 450001China Division of Chemistry and Biological Chemistry School of Chemistry Chemical Engineeringand BiotechnologyNanyang Technological UniversitySingapore 637371Singapore institute of Advanced synthesis School of Chemistry and Molecular Engineering Nanjing Tech UniversityNanjing 211816China

Numerous supramolecular macrocycles have been utilized for developing catalysts by exploiting their specific molecular recognition and ability to form inclusion complexes through noncovalent interactions. The cyclic structure and modified functional groups of these macrocycles can influence substrate and transition state stability, as well as reaction selectivity. The inner cavities of these macrocycles are particularly beneficial, as they enable substrates to adopt preorganized arrangements and serve as versatile platforms for highly efficient supramolecular catalytic systems. This minireview provides an overview of recent advancements in supramolecular catalysis using various macrocycles, such as crown ethers, cyclodextrins,calixarenes, pillararenes, cucurbiturils, and other novel macrocycles.

关键词： Supramolecular catalysis Macrocycle Host-guest interactions Confinement Selectivity

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MOF‐derived 1D/3D N‐doped porous carbon for spatially confined electrochemical CO2 reduction to adjustable syngas

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Carbon Energy 2024年第8期6卷 1-13页

作者： Wei Zhang Hui Li Daming Feng Chenglin Wu Chenghua Sun Baohua Jia Xue Liu Tianyi Ma Key Laboratory for Green synthesis and Preparative Chemistry of Advanced Materials Institute of Clean Energy ChemistryCollege of ChemistryLiaoning UniversityShenyangLiaoningChina School of Science RMIT UniversityMelbourneVictoriaAustralia School of Pharmaceutical and Chemical Engineering Taizhou UniversityTaizhouZhejiangChina Department of Chemistry and Biotechnology Swinburne University of TechnologyHawthornVictoriaAustralia

Electrochemical reduction of CO_(2)to syngas(CO and H_(2))offers an efficient way to mitigate carbon emissions and store intermittent renewable energy in ***,the hierarchical one‐dimensional/three‐dimensional nitrogen‐doped porous carbon(1D/3D NPC)is prepared by carbonizing the composite of Zn‐MOF‐74 crystals in situ grown on a commercial melamine sponge(MS),for electrochemical CO_(2)reduction reaction(CO_(2)RR).The 1D/3D NPC exhibits a high CO/H_(2)ratio(5.06)and CO yield(31 mmol g^(−1)h^(−1))at−0.55 V,which are 13.7 times and 21.4 times those of 1D porous carbon(derived from Zn‐MOF‐74)and N‐doped carbon(carbonized by MS),*** is attributed to the unique spatial environment of 1D/3D NPC,which increases the adsorption capacity of CO_(2)and promotes electron transfer from the 3D N‐doped carbon framework to 1D carbon,improving the reaction kinetics of CO_(2)*** results and charge density difference plots indicate that the active site of CO_(2)RR is the positively charged carbon atom adjacent to graphitic N on 1D carbon and the active site of HER is the pyridinic N on 1D *** presence of pyridinic N and pyrrolic N reduces the number of electron transfer,decreasing the reaction kinetics and the activity of CO_(2)*** CO/H_(2)ratio is related to the distribution of N species and the specific surface area,which are determined by the degree of spatial confinement *** CO/H_(2)ratios can be regulated by adjusting the carbonization temperature to adjust the degree of spatial confinement *** the low cost of feedstock and easy strategy,1D/3D NPC catalysts have great potential for industrial application.

关键词： electrochemical CO_(2)reduction reaction melamine sponge metal‐organic frameworks porous carbon syngas

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Synthetic Strategies of Carbon Nanobelts and Beyond

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Chemical Research in Chinese Universities 2024年第4期40卷 627-631页

作者： LI Yanbang SHANG Wansong REN Yu ZHANG Xi-Sha LI Cheng ZHANG Guanxin ZHANG Deqing Beijing National Laboratory for Molecular Science CAS Key Laboratory for Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing100190P.R.China University of Chinese Academy of Sciences Beijing100049P.R.China

Carbon nanobelts(CNBs)with aesthetically appealing molecular structures and outstanding physical properties have attracted more and more attentions from the scientific community due to their potential applications in synthetic materials,host-guest chemistry,optoelectronics,and so *** synthesis of CNBs at different stages was overviewed and some representative breakthroughs and advances in synthetic strategies were highlighted and *** key issue for the synthesis of CNBs is how to construct curved structures with high strain *** not only proposed a few unconventional CNBs as the promising target molecules,but also pointed out the bottom-up synthesis of conjugated tubular segments of carbon nanotubes sharing similar properties as carbon nanotubes is the next focus in this emerging area.

关键词： Carbon nanobelt Strain energy Carbon nanoring Single-walled carbon nanotube Bottom-up synthesis

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Dynamic steric confinement effect expands the frontier of Cu-catalyzed asymmetric propargylic aminations

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Science China Chemistry 2024年第10期67卷 3181-3183页

作者： Peng Chen Mao-Mao Zhang Wen-Jing Xiao Liang-Qiu Lu Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction Ministry of EducationCollege of ChemistryCentral China Normal UniversityWuhan 430079China Wuhan institute of Photochemistry and Technology Wuhan 430082China State Key Laboratory for Oxo synthesis and Selective Oxidation Lanzhou Institute of Chemical Physics(LICP)Chinese Academy of SciencesLanzhou 730000China School of Chemistry and Chemical Engineering Henan Normal UniversityXinxiang 453007China

Chiralα-tertiary amines and related azacycles are commonly found in many natural products,pharmaceuticals and agrochemicals[1].Copper-catalyzed asymmetric propargylic amination(APA)reactions have been established as a reliable method to access enantio-enriched propargylic amines,largely due to the seminal contribution of Nishibayashi et al.[2]and van Maarseveen et al.[3]in 2008.

关键词： catalyzed asymmetric amines

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Copper-catalyzed enantioselective desymmetrizing C(sp^(2))-H functionalization of azide-ynamides via α-imino copper carbenes

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Science China Chemistry 2024年第9期67卷 2982-2988页

作者： En-He Huang Li-Gao Liu You-Wei Yin Hao-Xuan Dong Ji-Jia Zhou Xin Lu Bo Zhou Long-Wu Ye Key Laboratory for Chemical Biology of Fujian Province and State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

α-Imino metal carbenes are versatile intermediates in organic synthesis,and have broad applications in the assembly of divergent ***,the catalytic enantioselective desymmetrization based onα-imino metal carbenes has not been developed to ***,we disclose an enantioselective desymmetrizing C(sp^(2))-H functionalization of azide-ynamides viaα-imino copper carbenes,leading to the efficient assembly of divergent chiral indoloazepines in generally moderate to excellent yields with high ***,this reaction represents the first enantioselective desymmetrization based onα-imino metal *** synthetic transformations and biological tests show the potential utility of this ***,computational studies are employed to elucidate the reaction mechanism and the origin of enantioselectivity.

关键词： enantioselective desymmetrization metal carbenes copper catalysis nitrene transfer alkynes

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On-Surface synthesis of Electron-Deficient Bisanthene Tetraimide

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CCS Chemistry 2024年第3期6卷 672-681页

作者： Ye Liu Liangliang Chen Hailong Li Xi-Sha Zhang Qigang Zhong Zhengming Hao Minghui Wu Yan-Ying Huang Lina Wang Minchong Sheng Miao Xie Haiming Zhang Deqing Zhang Lifeng Chi Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices Institute of Functional Nano&Soft Materials(FUNSOM)Soochow UniversitySuzhouJiangsu 215123 CAS Key Laboratory for organic Solids Institute of ChemistryChinese Academy of SciencesBeijing 100190 institute of Applied Physics Justus Liebig University GiessenGiessen 35392

Imide-based conjugated molecules have emerged as a highly promising class of building blocks for constructing n-type semiconducting materials with lowlying lowest unoccupied molecular orbitals and exceptional *** imides,such as naphthalene diimides,perylene diimides and their lateral fused analogs,have been synthesized extensively,the design and synthesis of largerπ-extended molecules incorporating more than two imide groups are desirable but still very ***,we report the synthesis of an unprecedented electron-deficient bisanthene tetraimide(ATI)containing a bisantheneconjugated core and four five-membered imide groups,which was successfully achieved via a combined approach of solution and on-surface *** chemical structures,electronic states,formation mechanism and aromaticity of ATI were systematically investigated by scanning tunneling microscopy,noncontact atomic force microscopy,scanning tunneling spectroscopy,and density functional theory calculations.

关键词： on-surface synthesis electron-deficient bisanthene tetraimide dehydrocyclization low lowest unoccupied molecular orbital level

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Recent advances in memristors based on two-dimensional ferroelectric materials

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Frontiers of physics 2024年第1期19卷 195-218页

作者： Wenbiao Niu Guanglong Ding Ziqi Jia Xin-Qi Ma JiYu Zhao Kui Zhou Su-Ting Han Chi-Ching Kuo Ye Zhou institute for Advanced Study Shenzhen UniversityShenzhen 518060China College of Electronics and Information Engineering Shenzhen UniversityShenzhen 518060China institute of organic and Polymeric Materials Research and Development Center of Smart Textile TechnologyTaipei University of TechnologyTaipei 10608TaiwanChina

In this big data era, the explosive growth of information puts ultra-high demands on the data storage/computing, such as high computing power, low energy consumption, and excellent stability. However, facing this challenge, the traditional von Neumann architecture-based computing system is out of its depth owing to the separated memory and data processing unit architecture. One of the most effective ways to solve this challenge is building brain inspired computing system with in-memory computing and parallel processing ability based on neuromorphic devices. Therefore, there is a research trend toward the memristors, that can be applied to build neuromorphic computing systems due to their large switching ratio, high storage density, low power consumption, and high stability. Two-dimensional (2D) ferroelectric materials, as novel types of functional materials, show great potential in the preparations of memristors because of the atomic scale thickness, high carrier mobility, mechanical flexibility, and thermal stability. 2D ferroelectric materials can realize resistive switching (RS) because of the presence of natural dipoles whose direction can be flipped with the change of the applied electric field thus producing different polarizations, therefore, making them powerful candidates for future data storage and computing. In this review article, we introduce the physical mechanisms, characterizations, and synthetic methods of 2D ferroelectric materials, and then summarize the applications of 2D ferroelectric materials in memristors for memory and synaptic devices. At last, we deliberate the advantages and future challenges of 2D ferroelectric materials in the application of memristors devices.

关键词： two-dimensional ferroelectric materials synthesis strategies memristors artificial synapses

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Copper(Ⅰ)-catalyzed interrupted click/radical relay:A four-component modular synthesis of triazole sulfones

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Chinese Chemical Letters 2024年第3期35卷 247-251页

作者： Pengfei Sun Fang Wei Chen-Ho Tung Zhenghu Xu Key Lab for Colloid and Interface Chemistry of Education Ministry Shandong UniversityJi'nan 250100China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China Functional Molecules of Zhejiang Province School of ScienceWestlake UniversityHangzhou 310024China Key Laboratory of organic Chemistry in Jiangxi Province Institute of Organic ChemistryJiangxi Science&Technology Normal UniversityNanchang 330013China

A new,four component copper(Ⅰ)-catalyzed interrupted click/radical relay cascade has been *** unprecedented interrupted click reaction provides a rapid modular synthesis of triazole sulfones,important privileged heterocyclic pharmacophores which cannot be accessed by a traditional click *** interception of cuprate-triazole,the key reaction intermediate formed in situ,is an important feature of this process.

关键词： Click reaction Triazole Sulfone Radical relay

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High-throughput experimentation and machine learning-promoted synthesis of α-phosphoryloxy ketones via Ru-catalyzed P(O)O–H insertion reactions of sulfoxonium ylides

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Science China Chemistry 2024年

作者： An Lin Jingyuan Liu Yougen Xu Haiting Wu Yating Chen Yan Zhang Lebin Su Xiaodan Zhao Kuangbiao Liao institute of organic Chemistry & MOE Key Laboratory of Bioinorganic and Synthetic Chemistry School of Chemistry Sun Yat-sen University Guangzhou National Laboratory Bioland Laboratory

Herein, we report a novel and highly efficient method for the synthesis of α-phosphoryloxy carbonyl compounds via Rucatalyzed P(O)O–H insertion reactions of sulfoxonium ylides and phosphinic acids, with the assistance of high-throughput experimentation(HTE) and machine learning(ML). A variety of P(O)O-H derivatives, including diarylphosphates, alkyl phosphates, and alkoxyphosphates, are competent candidates to react with sulfoxonium ylides in this transformation, and variousα-phosphoryloxy carbonyls and propylene phosphates are directly constructed. This approach utilizes readily available sulfoxonium ylide as a carbene precursor, and features mild conditions, operational simplicity, and broad functional groups tolerance, and could be used for late-stage functionalization of structurally complex bioactive molecules. Moreover, a conducive exploration of the reaction space is also conducted(756 reactions) and a machine learning model for reaction yield prediction has been developed and applied, showcasing the practical application of this newly workflow(HTE-ML) in the field of synthetic chemistry.

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