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New sustainable polymers with on-demand depolymerization property

Science China chemistry 2024年第9期67卷 2803-2841页

作者： Yangyang Sun Zesheng An Yanshan Gao Rongrong Hu Ye Liu Hua Lu Xiao-Bing Lu Xuan Pang Anjun Qin Yong Shen Youhua Tao Yu-Zhong Wang Junpeng Wang Gang Wu Guang-Peng Wu Tie-Qi Xu Xing-Hong Zhang Yuetao Zhang Zhenbiao Zhang Jian-Bo Zhu Miao Hong Zhibo Li State Key laboratory of Organometallic chemistry Shanghai Institute of Organic Chemistry Chinese Academy of Sciences State Key laboratory of Supramolecular Structure and Materials College of Chemistry Jilin University State Key laboratory of Luminescent Materials and Devices Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates South China University of Technology State Key laboratory of Fine Chemicals Frontiers Science Center for Smart Materials Dalian University of Technology Beijing National laboratory for Molecular Sciences Center for Soft Matter Science and Engineering Key Laboratory of Polymer Chemistry and Physics of Ministry of Education College of Chemistry and Molecular Engineering Peking University Key laboratory of Polymer Ecomaterials Changchun Institute of Applied Chemistry Chinese Academy of Sciences State Key laboratory Base of Eco-Chemical Engineering College of Chemical Engineering Qingdao University of Science and Technology The Collaborative Innovation Center for Eco-Friendly and Fire-Safety Polymeric Materials (Mo 5 National Engineering Laboratory of Eco-Friendly Polymeric Materials (Sichuan) College of Chemistry State Key Laboratory of Polymer Materials Engineering Sichuan University School of Polymer Science and Polymer Engineering the University of Akron MOE Key laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and Engineering Zhejiang University State and Local Joint Engineering laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis College of ChemistryChemical Engineering and Materials Science Soochow University

To combat the crisis of today's synthetic polymers arising from unsustainable production and disposal, it is essential for the synthetic polymer community to reshape the current polymer industry with sustainable polymers. As an emerging class of sustainable polymers, the development of chemically depolymerizable polymers(CDPs), which can undergo closed-loop depolymerization/repolymerization cycles to reproduce virgin polymers without the loss of properties from recovered monomers, offers an ideal solution to preserve finite natural resources, provides a feasible solution to the end-of-life issue of polymer waste, and thereby establishes a circular materials economy. However, two grand key challenges have been encountered in the establishment of practically useful CDPs: how to balance polymerization and depolymerization ability and how to unify conflicted depolymerizability and physical properties. Accordingly, this critical review article presents our vision for summarizing feasible strategies to overcome the above two significant challenges and the design principles for constructing an ideal CDP by highlighting selected major progress made in this rapidly expanding field.

关键词： chemically depolymerizable polymers sustainable polymers depolymerization monomer recovery degradation plastics

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SOX17-mediated immune evasion in early colorectal cancer:From pre-malignant adaptation to tumor progression

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Acta Pharmaceutica Sinica B 2024年第8期14卷 3780-3782页

作者： Yanfeng Gao Yanping Wang Jinsong Zhao Yujun Song School of Medical Imaging Wannan Medical CollegeWuhu 241002China College of Engineering and applied Sciences State Key Laboratory of Analytical Chemistry for Life ScienceNanjing UniversityNanjing 210023China

One of the hallmarks of cancer is its inherently immunosuppressive microenvironment,which strategically manipulates surrounding immune cells,signaling molecules,and structural components to shield cancer cells from immune attacks and foster tumor *** tumor microenvironment is characterized by the presence of immunosuppressive entities such as tumor-associated macrophages,T cells,tumor-associated neutrophils,and myeloid-derived suppressor cells(MDSCs),as well as metabolic alterations like hypoxia2 and elevated lactate levels3.

关键词： Immune escape Tumor microenvironment Immunotherapy Immunosuppressive tumor microenvironment Transcription factor CD8^(+)T cell infiltration AKP organoids CRISPReCas9 genome editing

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Design of new chemicals for advanced electrolytes

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Science China chemistry 2024年第5期67卷 1378-1380页

作者： Haoran Cheng Zheng Ma Qian Li Jun Ming State Key laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China University of Science and Technology of China Hefei 230026China

This highlight is inspired by a recent article in Nature Energy in which Liu and co-workers [1] from Tsinghua University designed a new asymmetric lithium salt (i.e., lithium 1,1,1-trifluoro-N-[2-[2-(2-methoxy ethoxy)ethoxy]ethyl] methanesulfonamide (Li FEA)) and applied it as a new lithium-salt additive in the conventional carbonate-based electrolyte,overcoming the incompatibility issue of carbonate electrolytes with lithium metal in lithium metal batteries (LMBs),even achieving a fast-charging feature.

关键词： lithium carbonate electrolyte

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Catalysis by subsurface metal atoms in Al(001) through electron transfer

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National Science Review 2024年第4期11卷 12-13页

作者： Bo Sun Ding Ma Beijing National laboratory for Molecular Science New Cornerstone Science Laboratory College of Chemistry and Molecular Engineering Peking University

Heterogeneous catalysis plays a crucial role in the chemical industry, which has evolved from the investigation of chemisorption to an electronic structure[1]. Diverse strategies, such as alloying,doping, and confining, have been applied to enhance the catalytic properties of active sites through electronic modulation. The electron transfer between active sites and substrates profoundly influences catalytic activity [2].

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Time-resolved ultra-small-angle X-ray scattering beamline(BL10U1)at SSRF

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Nuclear Science and Techniques 2024年第2期35卷 6-19页

作者： Wen-Qiang Hua Chun-Ming Yang Ping Zhou Feng Tian Jin-You Lin Yu-Zhu Wang Xiao-Yun Li Xia-Ran Miao Chun-Xia Hong Qiu-Shi Huang Xin-Tong Zhao Yong-Feng Men Jie Wang Xing-Yu Gao Xiu-Hong Li Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China Key laboratory of Advanced Micro Structural Materials MOEInstitute of Precision Optical EngineeringSchool of Physics Science and EngineeringTongji UniversityShanghai 200092China State Key laboratory of Polymer Physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The construction of a new beamline,BL10U1,was completed at the Shanghai synchrotron radiation facility in *** multipurpose beamline was designed to provide X-ray scattering techniques such as ultra-small-angle X-ray scattering(USAXS),small-angle X-ray scattering(SAXS),wide-angle X-ray scattering,and microfocus SAXS(μSAXS)for a broad user *** realize fast time-resolved USAXS experiments,the beamline adopted an in-vacuum undulator with a total length of 1.6 m as the photon *** in-house cryogenic-cooled double multilayer monochromator was installed to deliver a photon flux of approximately 10^(13) photons/s at a photon energy of 10 *** three-year successful operation of this beamline demonstrated that the monochromator operated smoothly,as ***10U1 has three end stations in succession:USAXS end station,μSAXS end station,and end station for industrial *** minimum scattering vector q~0.0042 nm^(-1) at 10 keV can be achieved at the USAXS end station equipped with a 28 m-long and 1.8 m-diameter vacuum flight *** theμSAXS end station,a beam spot of less than 10×8μm was achieved for micro-SAXS *** contrast,in situ experimental instruments up to 5 m high and 8 m wide can be mounted at the industrial application end station,which offers industrial scientists the opportunity to use their large industrial ***10U1 opens up a new capability to investigate phenomena such as non-equilibrium and dynamic processes of materials with a wide length scale from angstroms to micrometers with millisecond time *** this paper,we also report beamline design considerations and commissioning results.

关键词： Synchrotron radiation Ultra-small-angle X-ray scattering Micro small-angle X-ray scattering USAXS Time resolved μSAXS

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Modulating redox transition kinetics by anion regulation in Ni-Fe-X(X=O,S,Se,N,and P)electrocatalyst for efficient water oxidation

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Nano Research 2024年第6期17卷 4720-4728页

作者： Liting Wei Kaini Zhang Rui Zhao Lei Zhang Yan Zhang Suyi Yang Jinzhan Su International Research Center for Renewable Energy&State Key laboratory of Multiphase Flow in Power Engineering Xi’an Jiaotong UniversityXi’an 710049China Department of applied chemistry Yuncheng UniversityYuncheng 044000China

NiFe-based electrocatalysts will experience dynamical surface reconstruction during oxygen evolution reaction(OER)process,and the derived metal(oxy)hydroxide hybrids on the surface have been considered as the actual active species for *** efforts have been dedicated to understanding the surface reconstruction,but there is rare research on recognizing the origin of improved performance derived from anion species of ***,the OER electrocatalytic characteristics were tuned with different anions in NiFe-based catalyst,using NiFe-based oxides/nitride/sulfide/selenides/phosphides(NiFeX,X=O,N,S,Se,and P)as the model *** combination of X-ray photoelectronic spectroscopy,electrochemical tests,operando spectroscopic characterizations,and density functional theory(DFT)calculations,reveals that anion with lower electronegativity in NiFe-based catalyst leads to higher conductivity and delayed valence transition of Ni sites,as well as optimized adsorption behavior towards oxygen intermediates,contributing to enhanced OER ***,NiFeP electrocatalyst demonstrates an ultralow overpotential of 265 mV at 20 mA·cm−2 for OER,as well as long-term *** work not only offers further insights into the effect of anionic electronegativity on the intrinsic OER electrocatalytic properties of NiFe-based electrocatalyst but also provides guide to design efficient non-noble metal-based electrocatalysts for water oxidation.

关键词： oxygen evolution reaction(OER) anion species electronegativity valence transition

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Rational design of ZnCdS/TpPa-1-COF heterostructure photocatalyst by strengthening the interface connection in solar hydrogen production reactions

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Nano Research 2024年第3期17卷 1027-1034页

作者： Di Yang Zhi-Gang Li Xinghao Zhang Zenghuan Ren Weihan Lu Haining Liu Xiaomeng Guo Jijie Zhang Xian-He Bu Tianjin Key laboratory of Metal and Molecule-Based Material chemistry School of Materials Science and EngineeringNankai UniversityTianjin 300350China College of chemistry and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuang 050018China State Key laboratory of Elemento-Organic chemistry College of ChemistryNankai UniversityTianjin 300071China

ZnCdS quantum dots(QDs)are highly coveted in photocatalysis research for their exceptional visible-light responses and high light-absorption ***,their practical application is hindered by their tendency to aggregate,due to having high surface *** address this issue,herein,a heterostructure is synthesized by growing ZnCdS QDs with a size of approximately 5 nm onto the surface of a two-dimensional(2D)covalent organic framework(COF),*** approach suppresses the aggregation of the QDs and improves their *** ZnCdS/TpPa-1-COF composite exhibited a peak hydrogen evolution rate of 6244.16μmol·g^(-1)·h^(-1),which was 2.89 and 4.18 times greater than that of ZnCdS and TpPa-1-COF,*** zero-dimensional/two-dimensional(0D/2D)heterojunction formed by ZnCdS and TpPa-1-COF generates a strong interfacial force,which is attributed to the intimate contact between the *** connections accelerate charge separation,improve the utilisation of reduced electrons,and reduce the extent of agglomeration of the ZnCdS QDs,thereby resulting in high hydrogen production activity of the ***,the photocatalytic mechanism is studied using Kelvin probe force microscopy and theoretical *** study offers a novel approach for creating sulfide photocatalysts and is crucial for investigating the potential practical applications of the related photocatalysts.

关键词： covalent organic frameworks quantum dots photocatalysis hydrogen generation heterojunction

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S-scheme heterojunction in photocatalytic hydrogen production

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Journal of Materials Science & Technology 2024年第2期169卷 82-104页

作者： Teng Li Noritatsu Tsubaki Zhiliang Jin School of chemistry and Chemical Engineering North Minzu UniversityYinchuan 750021China Department of applied chemistry Graduate School of EngineeringUniversity of ToyamaGofuku 3190Toyama 930-8555Japan

As an ideal secondary energy source,hydrogen has the title of clean energy and the product of its complete combustion is only water,which is not polluting to the *** hydrogen production technology is an environmentally friendly,safe,and low-cost strategy that requires only an inexhaustible amount of solar energy and water as *** paper provides a detailed and detailed review of S-scheme heterojunction photocatalysts for photocatalytic hydrogen production,mainly including TiO_(2)-based,Perovskite-based,CdS-based,Graphitic phase carbon nitride-based,COF-based graphdiyne-based,ZnO-based,and ZnIn_(2)S_(4)-based S-scheme heterojunction *** classification of S-scheme heterojunctions is ***’s more,various characterizations for direct verification of the charge migration mechanism of S-scheme heterojunctions are *** on the present study,the future potential challenges and future research trends for S-scheme heterojunctions in photocatalytic hydrogen evolution technology are pointed out,which provides feasible strategies for the development and design of S-scheme heterojunction photocatalysts in the field of photocatalytic hydrogen evolution.

关键词： S-scheme heterojunction Photocatalysis Charges migration Hydrogen evolution

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Emerging two-dimensional Mo-based materials for rechargeable metal-ion batteries:Advances and perspectives

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Journal of Energy chemistry 2024年第2期89卷 487-518,I0012页

作者： Qingqing Ruan Yuehua Qian Mengda Xue Lingyun Chen Qichun Zhang Department of applied chemistry School of Chemistry and Chemical EngineeringChongqing UniversityChongqing 401331China Department of Materials Science and Engineering City University of Hong Kong999077Hong KongChina

With the rapid development of rechargeable metal-ion batteries(MIBs)with safety,stability and high energy density,significant efforts have been devoted to exploring high-performance electrode *** recent years,two-dimensional(2D)molybdenum-based(Mo-based)materials have drawn considerable attention due to their exceptional characteristics,including low cost,unique crystal structure,high theoretical capacity and controllable chemical ***,like other transition metal compounds,Mo-based materials are facing thorny challenges to overcome,such as slow electron/ion transfer kinetics and substantial volume changes during the charge and discharge *** this review,we summarize the recent progress in developing emerging 2D Mo-based electrode materials for MIBs,encompassing oxides,sulfides,selenides,*** introducing the crystal structure and common synthesis methods,this review sheds light on the charge storage mechanism of several 2D Mo-based materials by various advanced characterization *** latest achievements in utilizing 2D Mo-based materials as electrode materials for various MIBs(including lithium-ion batteries(LIBs),sodium-ion batteries(SIBs)and zinc-ion batteries(ZIBs))are discussed in ***,the modulation strategies for enhancing the electrochemical performance of 2D Mo-based materials are highlighted,focusing on heteroatom doping,vacancies creation,composite coupling engineering and nanostructure ***,we present the existing challenges and future research directions for 2D Mo-based materials to realize high-performance energy storage systems.

关键词： Molybdenum-based materials Two-dimensional materials Lithium-ion batteries Sodium-ion batteries Zinc-ion batteries

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Highly selective and eco-friendly dihydroisoquinoline synthesis via Cu/Co synergistic catalysis in Cu NPs@MOFs catalyst under mild conditions

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Science China chemistry 2024年第5期67卷 1561-1568页

作者： Peng-Fei Guo Ze-Long Liang Yue-E Jiao Hang Xu Bin Zhao Key laboratory of Advanced Energy Material chemistry Renewable Energy Conversion and Storage CenterDepartment of ChemistryNankai UniversityTianjin 300071China

3,4-Dihydroisoquinoline(DHIQ)is an important precursor used in the production of drugs for treating cancer,HIV,Alzheimer's disease,*** studies on DHIQ synthesis show low catalytic selectivity due to the susceptible over-oxidation feedstock of1,2,3,4-tetrahydroisoquinoline(THIQ),which often requires alkali ***,it is desirable yet challenging to explore a highly selective and efficient oxydehydrogenation capacity for DHIQ synthesis under eco-friendly reaction ***,a novel framework 1 was synthesized,exhibiting 1D channels with the size of 4.6 A×9.6 A and high solvent/p H/thermal stability.A stable framework allows it to encapsulate Cu nanoparticles(NPs)to form Cu NPs@1-x(x=1,2,3,and 4)with varying loading amounts of Cu NPs at 2.0 wt%,3.0 wt%,4.0 wt%,and 6.0 wt%,*** NPs@1-3 could selectively catalyze the reaction from THIQ to DHIQ with a high selectivity of 98%and a recorded turnover frequency(TOF)of 22.1 h-1under eco-friendly mild *** corresponding catalytic activity can maintain at least five recyclings and can be further applied to gram-scale ***,the efficient preparation of DHIQ catalyzed by Cu NPs@1-3 could be realized even under air ***,the anticancer molecule precursor synthesis of 6,7-dimethoxy-3,4-dihydroisoquinoline was also selectively catalyzed by Cu NPs@*** investigations revealed that high catalytic performance can be attributed to the stable framework and the synergistic catalytic effect of the loaded Cu NPs and Co metal *** importantly,this work represents the first example of MOF catalysts for selectively thermo-catalytic DHIQ synthesis and demonstrates a simple approach to obtain efficient catalysts for selective oxydehydrogenation in the production of unsaturated compounds.

关键词： metal-organic frameworks Cu NPs@MOFs 3 4-dihydroisoquinoline selective oxydehydrogenation synergistic catalysis

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