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Plasmonic CsPbBr_(3)–Au nanocomposite for excitation wavelength dependent photocatalytic CO_(2) reduction

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Journal of Energy chemistry 2021年第2期30卷 309-315,I0011页

作者： Jin-Feng Liao Ya-Ting Cai Jun-Yan Li Yong Jiang Xu-Dong Wang Hong-Yan Chea Dai-Bin Kuang MOE Key Laboratory of Bioinorganic and synthetic chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen UniversityGuangzhou 510217GuangdongChina

The optoelectronic performance of CsPbBr_3 nanocrystal(NC) has been dramatically limited by the severe charge carrier recombination and its narrow light absorption range,which are anticipated to be resolved via coupling with plasmonic Au nanoparticle(NP).In view of this,CsPbBr_3-Au nanocomposite is fabricated and further employed as a concept model to study the electronic interaction between perovskite NC and Au NP for the first *** has been found that the excitation-wavelength dependent carrier transfer behavior exists in CsPbBr_3-Au *** illumination with visible light(λ>420 nm),photo-generated electrons in CsPbBr_3 can inject into Au with an electron injection rate and efficiency of 2.84×10~9 s^(-1) and 78%,*** boosted charge separation is further translated into a 3.2-fold enhancement in CO_2 photocatalytic reduction activity compared with pristine CsPbBr_*** the other hand,when solely exciting Au NP with longer wavelength light(λ>580 nm),the localized surface plasmon resonance(LSPR) induced hot electrons in Au NPs can transfer to CsPbBr_3 NC and further participate in photocatalytic reaction towards CO_2 *** present study provides new insights into preparing plasmonic nanostructure to enhance the performance of perovskite based optoelectronic devices.

关键词： Perovskite Gold nanoparticle Photocatalysis Localized surface plasmon resonance

Chirality and chiral functional composites of bicontinuous cubic nanostructured cubosomes

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Chinese Chemical Letters 2022年第3期33卷 1488-1492页

作者： Deyin Wang Hongkai Liu Wei Wang center for synthetic Soft Materials Key Laboratory of Functional Polymer Materials of Ministry of Education and Institute of Polymer ChemistryCollege of ChemistryNankai UniversityTianjin 300071China

Molecular self-assembly is the most important strategy for the development of chiral aggregates and chiral functional materials. In this study, we rationally designed and synthesized chiral fluorescent heteroclusters that were self-assembled into microscale cubosomes with a three-dimensional(3D) bicontinuous cubic phase nanostructure. The cubosomes exhibited chirality, indicating that chirality is transferred from the molecules to the 3D nanostructure. Therefore, we confirmed the formation of a chiral bicontinuous cubic phase nanostructure for the first time. We also showed that this chirality originates from the continuous change in the saddle-splay distortion of the molecules within the curved bilayer. At the same time, transparent films of chiral composites were prepared by mixing the chiral cubosomes with an epoxy resin and then curing the mixture. Therefore, we demonstrated an effective method for preparing chiral composites.

关键词： Chirality Self-assembly Nanostructure Composite

Deciphering life sciences with“live”chemistry——The 2022 Nobel Prize in chemistry

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Science China chemistry 2023年第1期66卷 7-9页

作者： Xinyuan Fan Peng R.Chen synthetic and functional biomolecules center Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationBeijing National Laboratory for Molecular SciencesCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Peking-Tsinghua center for Life Sciences Peking UniversityBejing 100871China

The 2022 Nobel Prize in chemistry was awarded to Carolyn ***,Morten Meldal *** Sharpless for their development of click reaction and bioorthogonal *** understanding of life sciences has been fundamentally accelerated by such novel chemistries,and to some extent,revolutionized by the emergence of new chemical tools benefited from these cutting-edge interdisciplinary *** turn,the high demands of more powerful chemical tools for the sophisticated living systems have further promoted the development of new chemistry with newfunctionalities and applications.

关键词： Nobel life promoted

Dual-functional photocatalysis boosted by electrostatic assembly of porphyrinic metal-organic framework heterojunction composites with CdS quantum dots

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中国化学快报:英文版 2023年第9期34卷 165-170页

作者： Zhiyao Chen Sihong Li Qijie Mo Li Zhang Cheng-Yong Su MOE Laboratory of Bioinorganic and synthetic chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen UniversityGuangzhou 510006China

Photocatalytic dual-functional reaction under visible light irradiation represents a sustainable development *** detail,H2production coupled with benzylamine oxidation can remarkably lower the cost by replacing sacrificial *** this work,Cd S quantum dots(Cd S QDs)were successfully loaded onto the surface of a porphyrinic metal-organic framework(Pd-PCN-222)by the electrostatic selfassembly at room *** consequent Pd-PCN-222/CdS heterojunction composites displayed superb photocatalytic activity under visible light irradiation,achieving a H2production and benzylamine oxidation rate of 5069 and 3717μmol g^(-1)h^(-1)with>99%selectivity in 3 *** is no noticeable loss of catalytic capability during three successive *** studies by in situ electron spin resonance and X-ray photoelectron spectroscopy disclosed that CdS QDs injected photoexcited electrons to Pd-PCN-222 and then Zr6clusters under visible-light irradiation,and thus Cd S QDs and Zr6clusters behave as the photocatalytic oxidation and reduction centers,respectively.

关键词： Metal-organic framework composites Electrostatic self-assembly Dual-functional photocatalysis CdS quantum dots Metalloporphyrin

Beyond cotton and polyester: An evaluation of emerging feedstocks and conversion methods for the future of fashion industry

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Journal of Bioresources and Bioproducts 2024年第2期9卷 130-159页

作者： Ryen M.Frazier Keren A.Vivas Ivana Azuaje Ramon Vera Alonzo Pifano Naycari Forfora Hasan Jameel Ericka Ford Joel J.Pawlak Richard Venditti Ronalds Gonzalez Department of Forest Biomaterials North Carolina State UniversityRaleighNC 27695USA Department of Textile Engineering Chemistry and ScienceThe Nonwovens InstituteNorth Carolina State UniversityRaleighNC 27695USA

As the global population grows,the demand for textiles is increasing ***,this puts immense pressure on manufacturers to produce more *** synthetic fibers can be pro-duced cheaply,they have a negative impact on the *** the other hand,fibers from wool,sisal,fique,wood pulp(viscose),and man-made cellulose fibers(MMCFs)from cotton can-not alone meet the growing fiber demand without major stresses on land,water,and existing markets using these *** a greater emphasis on transparency and circular economy practices,there is a need to consider natural non-wood alternative sources for MMCFs to supple-ment other fiber ***,introducing new feedstocks with different compositions may require different biomass conversion ***,based on existing work,this review ad-dresses the technical feasibility of various alternative feedstocks for conversion to textile-grade ***,alternative feedstocks are introduced,and then conventional(dissolving pulp)and emerging(fibrillated cellulose and recycled material)conversion technologies are evaluated to help select the most suitable and promising processes for these emerging alternative sources of *** is important to note that for alternative feedstocks to be adopted on a meaningful scale,high biomass availability and proximity of conversion facilities are critical *** North America,soybean,wheat,rice,sorghum,and sugarcane residues are widely available and most suitable for conventional conversion through various dissolving pulp production methods(pre-hydrolysis kraft,acid sulfite,soda,SO2-ethanol-water,and potassium hydroxide)or by emerging cellulose fibrillation *** dissolving pulp conversion is well-established,fibrillated cel-lulose methods could be beneficial from cost,efficiency,and environmental ***,the authors strongly encourage more work in this growing research ***,conducting thorough cost and sustainability assessment

关键词： Non-wood Residue Regenerated cellulose Dissolving pulp Man-made cellulose fiber Apparel textile

A Single-Fluorophore Multicolor Molecular Sensor That Visually Identifies Organic Anions Including Phosphates

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CCS chemistry 2024年第3期6卷 774-782页

作者： Zezhou Zong Qi Zhang Da-Hui Qu Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research center School of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237

Developing fluorescent sensors for small-molecule phosphates offers opportunities in optically detecting biorelevant reactions and ***,it remains elusive how to identify phosphates from other anions,such as carboxylates and sulfates,because current synthetic phosphate receptors lack *** we report the construction of a multicolor fluorescent sensor that can identify phosphates from other analogous *** key design principle is to take advantage of the highly sensitive conformation-dependent emissive wavelength of diphenyl-9,14-dihydrodibenzo[a,c]phenazine fluorophores to sense the minor structural differences between phosphates and other anions,for example,sulfates and *** effect of structural factors such as spacer length and urea versus thiourea has been investigated by comparing the optical properties and binding affinities with the phosphate *** strategy provides a simple and robust fluorescent sensing solution to optically analyze small-molecule phosphates with antiinterference performance.

关键词： fluorescent sensors photoluminescence host-guest chemistry supramolecular chemistry noncovalent bonds

High-rate CH_(4)-to-C_(2)H_(6) photoconversion enabled by Au/ZnO porous nanosheets under oxygen-free system

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Science China chemistry 2024年第3期67卷 869-875页

作者： Kai Zheng Xiaojing Zhang Jun Hu Chengbin Xu Juncheng Zhu Jing Li Mingyu Wu Shan Zhu Li Li Shumin Wang Yumei Lv Xin He Ming Zuo Chengyuan Liu Yang Pan Junfa Zhu Yongfu Sun Yi Xie Hefei National Laboratory for Physical Sciences at Microscale National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230026China Key Laboratory of Photochemical Conversion and Optoelectronic Materials Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190China State Grid Anhui Electric Power Research institute Hefei 230601China

Photocatalytic CH_(4) coupling into high-valued C_(2)H_(6) is highly attractive,whereas the photosynthetic rate,especially under oxygen-free system,is still ***,we designed the negatively charged metal supported on metal oxide nanosheets to activate the inert C-H bond in CH_(4)and hence accelerate CH_(4) coupling *** an example,the synthetic Au/ZnO porous nanosheets exhibit the C_(2)H_(6) photosynthetic rate of 1,121.6μmol g^(-1)_(cat)h^(-1)and the CH_(4) conversion rate of 2,374.6μmol g^(-1)_(cat)h^(-1) under oxygen-free system,2 orders of magnitude higher than those of previously reported *** virtue of several in situ spectroscopic techniques,it is established that the generated Au^(δ-)and O^-species together polarized the C-H bond,while the Au^(δ-)and O^-species jointly stabilized the CH_(3) intermediates,which favored the coupling of CH_(3) intermediate to photosynthesize C_(2)H_(6) instead of overoxidation into CO_(x).Thus,the design of dual active species is beneficial for achieving high-efficient CH_(4)-to-C_(2)H_(6) photoconversion.

关键词： dual surface-active sites selective methane coupling ethane room temperature

Total synthesis of a putative yuzurimine-type Daphniphyllum alkaloid C_(14)–epi-deoxycalyciphylline H

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Chinese Chemical Letters 2024年第4期35卷 336-339页

作者： Jingping Hu Jing Xu Shenzhen Grubbs institute and Department of chemistry and Guangdong Provincial Key Laboratory of Catalysis and Shenzhen Key Laboratory of Small Molecule Drug Discovery and Synthesis Southern University of Science and TechnologyShenzhen 518055China

One of the largest subfamilies within the famous Daphniphyllum alkaloid family is made up of the yuzurimine-type(or macrodaphniphyllamine-type) alkaloids. Their complex aza-polycyclic caged structures, several contiguous stereogenic centers, and vicinal all-carbon quaternary centers make these alkaloids formidable challenge for synthetic chemists. Recently, synthesis of these alkaloids has received extensive attention from our community. Herein, we wish to report the total synthesis of C_(14)–epideoxycalyciphylline H, a putative member of yuzurimine-type alkaloid subfamily. Key transformations employed in our approach include an intramolecular Prins reaction and a Pd-catalyzed enyne cycloisomerization. In addition, synthesis of a daphnezomine L-type alkaloid, paxdaphnidine A, was also studied.

关键词： Total synthesis Daphniphyllum alkaloids Yuzurimine-type alkaloids Prins reaction Enyne cycloisomerization

Ultrathin two-dimensional porphyrinic metal-organic framework nanosheets induced by the axial aryl substituent

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Chinese Chemical Letters 2023年第7期34卷 117-121页

作者： Jurong Dong Yufei Wang Yu-Lin Lu Li Zhang MOE Laboratory of Bioinorganic and synthetic chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-Sen UniversityGuangzhou 510006China

Ultrathin two-dimensional metal-organic framework nanosheets have emerged as a promising kind of heterogeneous catalysts. Herein, we report a new kind of 2D porphyrinic metal-organic framework nanosheets of Rh2-PCN-222, which was prepared from the self-assembly of the metalloporphyrin ligand Rh(TCPP)(DCB)(TCPP = 5,10,15,20-tetrakis(4-methoxycarbonylphenyl)porphyrin;DCB = 3,4-dichlorobenzene) and ZrCl_(4) in the presence of two kinds of monocarboxylic acids as the modulating reagent. The thickness of Rh2-PCN-222 nanosheets was characterized by atomic force microscopy(AFM)and determined to be 5.4-9.6 nm. It was found that the axial aryl dichlorophenyl substituent, which controlled the anisotropic growth of MOFs, was essential for the formation of nanosheets. Catalytic results showed that Rh2-PCN-222 nanosheets were efficient for CO_(2) transformation.

关键词： Metalloporphyrin Axial aryl substituent 2D MOF nanosheets CO_(2)transformation Heterogeneous catalysis