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The future of sustainable chemistry and process: Convergence of artificial intelligence, data and hardware

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能源与人工智能(英文) 2020年第2期2卷 167-174页

作者： Xin Yee Tai Hao Zhang Zhiqiang Niu Steven D.R.Christie Jin Xuan Department of Chemical Engineering Loughborough UniversityLoughborough LE113TUUnited Kingdom School of Engineering The University of EdinburghEdinburgh EH93FBUnited Kingdom Department of chemistry Loughborough UniversityLoughborough LE113TUUnited Kingdom

sustainable chemistry for renewable energy generation and green synthesis is a timely research topic with the vision to provide present needs without compromising future *** the era of Industry 4.0,sustainable chemistry and process are undergoing a drastic transformation from continuous flow system toward the next level of operations,such as cooperating and coordinating machine,self-decision-making system,autonomous and automatic problem solver by integrating artificial intelligence,data and hardware in the cyber-physical *** to the lack of convergence between the physical and cyber spaces,the open-loop systems are facing challenges such as data isolation,slow cycle time,and insufficient resources *** researches have been devoted to accelerating these cycles,reducing the time between multistep processes and real-time characterization via additive manufacturing,in-/on-line monitoring,and artificial *** final goal is to concurrently propose process recipes,flow synthesis,and molecules characterization in sustainable chemical processes,with each step transmitting and receiving data *** process is known as‘closing the loop’,which will potentially create a future lab with highly integrated systems,and generate a service-orientated platform for end-to-end synchronization and self-evolving,inverse molecular design,and automatic science *** perspective provides a methodical approach for understanding cyber and physical systems individually,enabled by artificial intelligence and additive manufacturing,respectively,in combination with in-/on-line ***,the future perspective and key challenges for the development of the closed-loop system in sustainable chemistry and process are discussed.

关键词： Artificial intelligence In-/on-line monitoring Additive manufacturing

Gold-catalyzed addition reaction between creatinine and isatin:A sustainable and green chemistry approach for the diastereoselective synthesis of 3-substituted-3-hydroxyisatins

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Chinese Journal of Catalysis 2017年第5期38卷 775-783页

作者： K. Parthasarathy T. Ponpandian C. Praveen Department of chemistry Siddha Central Research Institute Central Council for Research in Siddha (CCRS) Arumbakkam Chennai‐600106 Tamil NaduIndia Inogent Laboratories Private Limited Industrial Development Area Nacharam Hyderabad‐500076 Telangana India Functional Materials Division Council of Scientific and Industrial Research‐Central Electrochemical Research Institute (CSIR‐CECRI) Karaikudi‐600006Tamil Nadu India

The aldolization of various isatins with creatinine under gold catalysis in water has been *** reaction is operationally simple as the products can be isolated by simple filtration without requiring tedious solvent extraction and column chromatographic *** generality of this methodology is showcased through the reactions of a wide range of isatin derivatives with creatinine to afford the respective aldol products in excellent yields with complete syn‐*** scope of this chemistry is further extended to a tandem reaction involving isatins,creatinine and malononitrile to afford multicomponent products in excellent yields with complete anti‐*** antioxidant potency of the synthesized compound was assessed by a spectrophotometric method,which revealed that three compounds containing halogen atoms(2c,2d and2e)were the most active compared with the standard.

关键词： Creatinine Gold catalysis Green chemistry Diastereoselectivity Antioxidant

Surface-neutralization engineered NiCo-LDH/phosphate hetero-sheets toward robust oxygen evolution reaction

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Green Energy & Environment 2024年第7期9卷 1151-1158页

作者： Shunfa Zhou Yuxuan Liu Jing Li Zhao Liu Jiawei Shi Liyuan Fan Weiwei Cai sustainable Energy Laboratory Faculty of Materials Science and Chemistry China University of Geosciences College of Science and Engineering James Cook University

Developing highly active oxygen evolution reaction（OER） electrocatalysts with robust durability is essential in producing high-purity hydrogen through water electrolysis. Layered double hydroxide（LDH） based catalysts have demonstrated efficient catalytic performance toward the relatively sluggish OER. By considering the promotion effect of phosphate（Pi） on proton transfer, herein, a facile phosphate acid（PA）surface-neutralization strategy is developed to in-situ construct NiCo-LDH/NiCoPi hetero-sheets toward OER catalysis. OER activity of NiCoLDH is significantly boosted due to the proton promotion effect and the electronic modulation effect of NiCoPi. As a result, the facilely prepared NiCo-LDH/NiCoPi catalyst displays superior OER catalytic activity with a low overpotential of 300 mV to deliver 100 mA cm-2OER and a Tafel slope of 73 mV dec-1. Furthermore, no visible activity decay is detected after a 200-h continuous OER operation. The present work,therefore, provides a promising strategy to exploit robust OER electrocatalysts for commercial water electrolysers.

关键词： Oxygen evolution reaction Phosphate Layered double hydroxide Hetero-sheets Stability

Photoredox catalytic alkylarylation of alkynes with arylsulfonylacetate as bifunctional reagent

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Science China chemistry 2024年第6期67卷 2022-2028页

作者： Chonglong He Min Wang Yulong Wang Lirong Zhao Youkang Zhou Keyuan Zhang Shenyu Shen Yaqiong Su Xin-Hua Duan Le Liu School of chemistry Engineering Research Center of Energy Storage Materials and DevicesMinistry of EducationXi’an Key Laboratory of Sustainable Energy Material ChemistryXi’an Jiaotong UniversityXi’an710049China

Difunctionalization of alkynes represents a powerful and straightforward approach to the synthesis of complex ***,the radical difunctionalization of alkynes mediated by bifunctional reagents remains challenging and underexplored,despite significant progress having been made in alkene ***,we report a novel arylsulfonylacetate skeleton in which aryl rings are attached to acetates through SO_(2),serving as a powerful bifunctional reagent for the alkylarylation of alkynes via vinyl-radical intermediate under photoredox *** modular bifunctional reagent enables the simultaneous incorporation of a wide range of functional groups,including(hetero)aryl ring and alkyl carboxylate into alkynes,resulting in synthetically valuable all-carbon tetrasubstituted alkene *** transformation is distinguished by its redox-neutral nature,readily accessible starting materials,compatibility with diverse functional groups and its capacity to facilitate convergent *** utility of this approach was further demonstrated by the late-stage functionalization of complex molecules and the preparation of fluorescent molecules and anti-cancer drugs.

关键词： bifunctional reagent photoredox catalysis Smiles rearrangement alkylarylation tetrasubstituted acyclic all-carbon olefins

MXenes for Bioinspired Soft Actuators:Advancements in Angle-Independent Structural Colors and Beyond

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Nano-Micro Letters 2024年第8期16卷 18-34页

作者： Siavash Iravani Rajender S.Varma Independent Researcher W Nazar STBoostan AveIsfahanIran Centre of Excellence for Research in sustainable chemistry Department of ChemistryFederal University of São CarlosSão CarlosSP 13565‑905Brazil

Soft actuators have garnered substantial attention in current years in view of their potential appliances in diverse domains like robotics,biomedical devices,and biomimetic *** actuators mimic the natural movements of living organisms,aiming to attain enhanced flexibility,adaptability,and *** the other hand,angle-independent structural color has been achieved through innovative design strategies and engineering *** carefully controlling the size,shape,and arrangement of nanostructures,researchers have been able to create materials exhibiting consistent colors regardless of the viewing *** promising class of materials that holds great potential for bioinspired soft actuators is MXenes in view of their exceptional mechanical,electrical,and optical *** integration of MXenes for bioinspired soft actuators with angle-independent structural color offers exciting *** material compatibility issues,improving color reproducibility,scalability,durability,power supply efficiency,and cost-effectiveness will play vital roles in advancing these *** perspective appraises the development of bioinspired MXene-centered soft actuators with angleindependent structural color in soft robotics.

关键词： MXenes MXene-based composites Bioinspired soft robotics Angle-independent structural color

Nickel-catalyzed carbonylative four-component 1,4-dicarbofunctionalization of 1,3-enynes

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Science China chemistry 2024年第6期67卷 2029-2038页

作者： Yan Zhao Qi-Chao Shan Hong Xin Pin Gao Xu Yang Xin-Hua Duan Li-Na Guo Department of chemistry School of ChemistryXi’an Key Laboratory of Sustainable Energy Material Chemistry and Engineering Research Center of Energy StorageMaterials and DevicesMinistry of EducationXi’an Jiaotong UniversityXi’an710049China School of Electrical Engineering Xi’an Jiaotong UniversityXi’an710049China

An efficient Ni-catalyzed four-component 1,4-carbocarbonylation of 1,3-enynes with activated alkyl halides and arylboronic acids under atmospheric pressure of CO is *** tuning the electronic and steric effects of alkyl radicals,both electronrich and electron-deficient 1,3-enynes were compatible with this *** protocol features mild conditions,broad substrate scope,excellent functional group compatibility and facile gram-scale synthesis,providing a practical approach to the quaternary carbon center-containing allenyl *** study revealed that the acyl-NiIIspecies plays an important role in both the coupling and the alkyl radical generation processes.

关键词： Ni catalysis four-component 1 4-carbocarbonylation 1 3-enynes

Boosting the self-trapped exciton emission in vacancy-ordered double perovskites via supramolecular assembly

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Chinese Journal of Structural chemistry 2024年第6期43卷 1-2页

作者： Xingwen Cheng Haoran Ren Jiangshan Luo Institute of Quantum and sustainable Technology(IQST) School of Chemistry and Chemical EngineeringJiangsu UniversityZhenjiang212013China

All-inorganic 3D lead-free vacancy-ordered double perovskites(DPs)in the A_(2)MX_(6)phase have garnered significant attention in the fields of photovoltaics and light-emitting diodes(LED)due to their exceptional optoelectronic properties[1].These properties encompass a high optical absorption coefficient,tunable bandgap,and long carrier diffusion dis-tance.

关键词： optoelectronic vacancy double

Iron-Catalyzed Reductive C(aryl)—Si Cross-Coupling of Diaryl Ethers with Chlorosilanes

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Chinese Journal of chemistry 2024年第6期42卷 578-584页

作者： Pei Liu Baowei Wu Xuefeng Cong Jie Kong School of chemistry and Chemical Engineering Northwestern Polytechnical UniversityXi'anShaanxi710072 China Institute of Molecular Plus Department of Chemistry and Haihe Laboratory of Sustainable Chemical TransformationsTianjin University92 Weijin RoadTianjin300072 China

The reductive cross-coupling between C(aryl)—O and Si—Cl bonds is of much importance as a valuable strategy for the construction of C(aryl)—Si bonds but has remained a great ***,we report a reductive cross-coupling of diaryl ethers and chlorosilanes via strong electrophilic C(aryl)—O and Si—Cl bonds cleavage by iron catalysis,which constitutes an efficient protocol for the synthesis of a range of functionalized *** combination of low cost FeCl2 as the precatalyst and iPrMgCl as the reductant shows high activity in the successive cleavage of unactivated C(aryl)—O bonds of diaryl ethers and strong electrophilic Si—Cl bonds of chlorosilanes,allowing their cross-coupling in a reductive *** low-valent iron species generated in situ by reduction of FeCl2 with iPrMgCl was proposed,which prefers to initially cleavage the C(aryl)—O bond of diaryl ethers with the chelation help of an o-amide auxiliary.

关键词： Cross-coupling Diaryl ethers Chlorosilanes C—O bond cleavage Iron catalyst 3d transition metals Selectivity Regioselectivity

Zeolite-encaged gold catalysts for the oxidative condensation of furfural

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Frontiers of Chemical Science and Engineering 2024年第8期18卷 67-77页

作者： Weijie Li Mingyang Gao Bin Qin Xin Deng Landong Li School of Materials Science and Engineering Nankai UniversityTianjin 300350China College of chemistry Nankai UniversityTianjin 300071China Haihe Laboratory of sustainable Chemical Transformations Tianjin 300192China

The oxidative condensation between renewable furfural and fatty alcohols is a crucial avenue for producing high-quality liquid fuels and valuable furan *** selectivity control in this reaction process remains a significant ***,we report the strategy of confining well dispersed gold species within ZSM-5 structure to construct highly active Au@ZSM-5 zeolite catalysts for the oxidative condensation of *** results and spectroscopy analyses demonstrate the efficient encapsulation of isolated and cationic Au clusters in zeolite ***@ZSM-5(K)catalyst shows remarkable performance with 69.7%furfural conversion and 90.2%furan-2-acrolein selectivity as well as good recycle *** is revealed that the microstructure of ZSM-5 zeolite can significantly promote oxidative condensation activity through confinement *** work presents an explicit example of constructing zeolite encaged noble metal catalysts toward targeted chemical transformations.

关键词： zeolite encapsulation gold oxidative condensation furfural