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MOF-templated tubular Ni_(1−x)Co_(x)S_(2)-CdS heterojunction with intensified direct Z-scheme charge transmission for highly promoted visible-light photocatalysis

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Nano Research 2024年第7期17卷 6281-6293页

作者： Chuan Jiang Yuanxin Qiu Xinxin Xin Yanyan Li Huilin Li Hui Wang Jixiang Xu Haifeng Lin Lei Wang Volodymyr Turkevych key laboratory of Eco-chemical engineering International S&T Cooperation Foundation of Eco-chemical Engineering and Green ManufactureCollege of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China Shandong Provincial key laboratory of Olefin Catalysis and Polymerization Key Laboratory of Rubber-Plastics of Ministry of EducationSchool of Polymer Science and EngineeringQingdao University of Science and TechnologyQingdao 266042China V.Bakul Institute for Superhard Materials National Academy of Sciences of UkraineKyiv 04074Ukraine

Hollow semiconductor nanostructures with direct Z-scheme heterojunction have significant advantages for photocatalytic reactions,and optimizing the interfacial charge transmission of Z-scheme heterojunction is the hinge to achieve excellent solar conversion *** this work,tubular Ni_(1−x)Co_(x)S_(2)-CdS heterostructures with reinforced Z-scheme charge transmission were constructed through an In-metal-organic framework(MOF)templated *** Z-scheme charge transfer mechanism was sufficiently confirmed by combining density functional theory(DFT)calculation,X-ray photoelectron spectroscopy(XPS),surface photovoltage spectroscopy(SPV),and radical testing ***,the use of sodium citrate complexant contributes to the formation of intimate heterointerface,and the Fermi level gap between CdS and NiS_(2)is enlarged through Co doping into NiS_(2),which enhances the built-in electric field and photo-carriers transmission driving force for Ni_(1−x)Co_(x)S_(2)-CdS heterojunction,resulting in an evidently promoted activity toward H2 evolution reaction(HER).Under visible-light(λ>400 nm)irradiation,the Ni_(1−x)Co_(x)S_(2)-CdS composite with 10 mol%Co doping and 80 wt.%CdS(NC_(0.10)S-80%CdS)achieved an outstanding HER rate up to 35.94 mmol·g^(−1)·h^(−1)(corresponding to the apparent quantum efficiency of 34.7%at 420 nm),approximately 76.4 times that of 3 wt.%Pt-loaded CdS and it is much superior to that of most CdS-based photocatalysts ever ***,the good photocatalytic durability of Ni_(1−x)Co_(x)S_(2)-CdS heterostructures was validated by cycling and long-term HER *** work could inspire the development of high-performance Z-scheme heterojunction via optimizing the morphology and interfacial charge transmission.

关键词： tubular heterostructure Z-scheme charge transmission interfacial coupling built-in electric field visible-light photocatalysis

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Controllable Ring-opening Polymerization ofδ-Valerolactone Catalyzed by Quinolinyl-Urea/MTBD Systems

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Chinese Journal of Polymer Science 2024年第8期42卷 1103-1110页

作者： Xin-Yu Liu Liang Zhu Su-Yun Jie Bo-Geng Li State key laboratory of Chemical engineering College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310058China

Due to their excellent biocompatibility and biodegradability,aliphatic polyesters are widely used in the biomedical,packaging and agricultural fields,which are usually accessed by the ring-opening polymerization(ROP)of lactones and the catalysts particularly play an important *** a series of quinolinyl-urea catalysts have been synthesized via the reaction between isocyanate and aminoquinoline with an amino group at different substitution positions and *** combination with 7-methyl-1,5,7-triazabicyclo[4,4,0]dec-5-ene(MTBD)as a cocatalyst and benzyl alcohol(BnOH)as an initiator,1-(3,5-bis(trifluoromethyl)phenyl)-3-(quinolin-3-yl)urea(3-QU)was observed to be most active for the ROP ofδ-valerolactone(δ-VL).The polymerization conditions were optimized by varying the type of organic base,catalyst concentration and reaction *** changing the ratio of[M]_0/[I],linear polyvalerolactones(PVLs)with different molecular weights and narrow molecular weight distribution were *** kinetic and chain extension experiments were carried out to prove the"living"/controllable *** the NMR experiments were used to support the proposal of possible mechanism.

关键词： Quinolinyl-urea Ring-opening polymerization PVL

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A FRET-Based Ratiometric H_(2)S Sensor for Sensitive Optical molecular Imaging in Second Near-Infrared Window

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Research 2024年第3期2023卷 671-684页

作者： Shan Lei Kejia Jiang Chenqing Zhang Wei Sun Yuantao Pan Dong Wang Peng Huang Jing Lin Marshall laboratory of Biomedical engineering International Cancer CenterShenzhen Key Laboratory of Tumor Visualization Molecular MedicineLaboratory of Evolutionary Theranostics(LET)School of Biomedical EngineeringShenzhen University Medical SchoolShenzhen UniversityShenzhen 518055China. Center for AIE Research College of Materials Science and EngineeringShenzhen UniversityShenzhen 518060China.

Second near-infrared(NIR-II)window optical molecular imaging kicks off a new revolution in high-quality imaging in vivo,but always suffers from the hurdles of inevitable tissue autofluorescence background and NIR-II probe ***,we prepare a Förster resonance energy transfer-based ratiometric NIR-II window hydrogen sulfide(H_(2)S)sensor through the combination of an H_(2)S-responsive NIR-II cyanine dye(acceptor,LET-1055)and an H_(2)S-inert rhodamine hybrid polymethine dye(donor,Rh930).This sensor not only exhibits high sensitivity and selectivity,but also shows rapid reaction kinetics(~20 min)and relatively low limit of detection(~96 nM)toward H_(2)S,allowing in vivo ratiometric NIR-II fluorescence imaging of orthotopic liver and colon tumors and visualization of the drug-induced hepatic H_(2)S *** findings provide the potential for advancing the feasibility of NIR-II activity-based sensing for in vivo clinical diagnosis.

关键词： H_ Infrared kinetics

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Towards wafer-scale growth of two-dimensional cerium dioxide single crystal with high dielectric performance

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Nano Research 2024年第9期17卷 8592-8599页

作者： Zhuofeng Shi Muhammad Imran Xiaohui Chen Xin Liu Yaqi Zhu Zhaoning Hu Saiyu Bu Jialin Zhang Chunhu Li Xiaodong Zhang Li Lin College of Chemistry and Chemical engineering Qingdao UniversityQingdao 266000China School of Materials Science and engineering Peking UniversityBeijing 100871China Center for Nanochemistry Beijing Science and Engineering Center for NanocarbonsBeijing National Laboratory for Molecular ScienceCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China key laboratory of Marine Chemistry Theory and Technology Ministry of EducationCollege of Chemistry and Chemical EngineeringOcean University of ChinaQingdao 266100China

Owing to the atomically thin nature,two-dimensional(2D)oxide materials have been widely reported to exhibit exciting transport and dielectric properties,such as fine gate controllability and ultrahigh carrier mobility,that outperform their bulk ***,unlike the successful synthesis of bulk oxide single crystals,reliable methods for synthesizing large-area single crystal of 2D oxide,that would suppress the negative influence from defective grain boundaries,remain unavailable,especially for nonlayered ***,we report that the lattice symmetry between the substrate and cerium dioxide(CeO_(2))would allow for the aligned nucleation and epitaxial growth of CeO_(2)on sapphire substrates,enabling the wafer-sized growth of CeO_(2)single *** careful tuning of the growth temperature and oxygen flow rate contributed to the harvesting of CeO_(2)wafer with reduced thickness and enhanced growth *** removal of grain boundaries improved the dielectric performance in terms of high dielectric strength(E_(bd)≈8.8 MV·cm^(-1)),suppressed leakage current,along with high dielectric constants(ε_(r)≈24).Our work demonstrates that with fine dielectric performance and ease of synthesizing wafer-sized single crystals,CeO_(2)can function as potential candidate as gate insulator for 2D-materials based nanoelectronics,and we believe the reported protocol of aligned nucleation can be extended to other 2D oxides.

关键词： dielectric materials two-dimensional materials chemical vapor deposition cerium dioxide

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Significant enhancement in local thermal conductivity of erythritol at interface with nanoparticles due to their interaction

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Nano Research 2024年第8期17卷 7726-7736页

作者： Ning Cao Yanhui Feng Kening Yan Zihan Liu Jiawei Wan Lin Qiu School of Energy and Environmental engineering University of Science and Technology BeijingBeijing 100083China State key laboratory of Biochemical engineering Key Laboratory of Biopharmaceutical Preparation and DeliveryInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China

When nano-fillers are used to enhance the thermal conductivity of organic phase change materials(PCMs),the naturally formed interface is considered to hinder thermal transport of the composite ***,the effect of the interface on the thermal properties of surrounding PCM has not been fully *** this paper,three composite PCMs(Ery@SiC,Ery@SiO_(2) and Ery@Si_(3)N_(4))were prepared by melt-blending *** local thermal conductivity and reduced Young’s modulus(E^(*))of the erythritol at the interface and far away from the interface in the composite PCMs were simultaneously measured by scanning thermal microscopy(SThM).The results revealed significant enhancement in local thermal conductivity of erythritol at the interface and its obvious positive correlation with E^(*).For different composite PCMs,molecular dynamics(MD)simulations suggested that the increase in intrinsic thermal conductivity and E^(*)of erythritol is attributed to the increase in interaction energy between erythritol and nanoparticles,as more erythritol phonon vibrations transform from localized mode to delocalized mode and erythritol has a higher density at the *** findings will provide new ideas for the design of PCM for energy storage.

关键词： scanning thermal microscopy phase change materials thermal conductivity reduced Young’s modulus interaction energy phonon participation ratio

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Polyphenol-mediated interfacial deposition strategy for supported manganese oxide catalysts with excellent pollutant degradation performance

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Chinese Chemical Letters 2024年第5期35卷 493-498页

作者： Dong Cheng Youyou Feng Bingxi Feng Ke Wang Guoxin Song Gen Wang Xiaoli Cheng Yonghui Deng Jing Wei The key laboratory of Biomedical Information engineering of Ministry of Education State Key Lab of Transducer TechnologySchool of Life Science and TechnologyXi’an Jiaotong UniversityXi’an 710049China School of Environmental and Municipal engineering Xi’an University of Architecture and TechnologyXi’an 710055China Department of Chemistry State Key Laboratory of Molecular Engineering of PolymersState Key Laboratory of Transducer TechnologyFudan UniversityShanghai 200433China key laboratory of Functional Inorganic Material Chemistry Ministry of EducationSchool of Chemistry and Materials ScienceHeilongjiang UniversityHarbin 150080China

In persulfate-based advanced oxidation process(PS-AOPs),fixing nanosized metal oxide on processable substrates is highly desirable to avoid the aggregation and loss of nanocatalysts during the practical ***,it is still challenging to develop a versatile strategy for the deposition of metal oxide nanocatalysts on various substrates with different physicochemical ***,polyphenols are utilized as a“molecular glue”and reductant to mediate the interfacial deposition of MnO_(2) nanocatalysts on different ***_(2) nanocatalysts were in-situ grown on macroscope mineral substrates(e.g.,airstone)via an interfacial redox strategy between tannic acid(TA)and oxidized KMnO4,and then employed as a fixed catalyst of peroxymonosulfate(PMS)activation for treating pharmaceutical and personal care products(PPCPs)in *** fixed MnO_(2) exhibited superior catalytic performance toward different PPCPS via a singlet oxygen(^(1)O_(2))-dominated nonradical oxidation *** in the secondary effluent of wastewater treatment plants could be effectively removed by a fixed-bed column of the fixed MnO_(2) with long term *** cycle of Mn^(4+)/Mn^(3+)and surface hydroxyl group of the fixed MnO_(2) was proved to be responsible for the activation of *** work provides a new avenue for developing fixed metal oxides for sustainable water treatment.

关键词： Redox strategy Manganese oxides Fixed catalyst Peroxymonosulfate PPCPs

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Structural transformation from Waugh-type to Keggin-type polyoxomolybdate-based crystalline material for photo/electrocatalysis

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Rare Metals 2024年第5期43卷 2241-2250页

作者： Pei-Sen Wang Zi-Tong Wang Ya-Ya Tan Peng Chen Xue-Cheng Zhang Lu-Nan Zhang Yong-Ge Wei Lu-Bin Ni School of Chemistry and Chemical engineering Yangzhou UniversityYangzhou 225002China key Lab of Organic Optoelectronics and molecular engineering of Ministry of Education Department of ChemistryTsinghua UniversityBeijing 100084China State key laboratory of Natural and Biomimetic Drugs Peking UniversityBeijing100191China

An inorganicDorganic hybrid crystalline material(SiMo_(12)O_(40))[Cu(2,2'-bipy)_(2)]_(2)·2H_(2)O(Complex 1,2,2'-bipy=2,2'-bipyridine)was synthesized for the first time by using 2,2'-bipy and transition metal copper to convert Waugh-type polyoxometalate[MnMo_(9)O_(3)_(2)]_(6-)into a Keggin polyoxometalate structure[SiMo_(12)O_(40)]^(4-)under hydrothermal conditions in glass *** crystal tests and a series of characterizations were carried out on Complex *** structure of Complex 1 is composed of[SiMo_(12)O_(40)]^(4-)and[Cu^(Ⅱ)(2,2'-bipy)_(2)]^(2+).The five-coordinated Cu is connected to two 2,2'-bipy through CuDN bonds,forming an approximately square ***,Complex 1 exhibited good photocatalytic performance for methylene blue degradation and electrocatalytic nitrite reduction properties simultaneously.

关键词： Polyoxometalates Inorganic-organic hybrid materials Photocatalytic Electrocatalytic

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Synergistic asymmetric diarylation of tethered alkenes via C–H functionalization of simple(hetero)arenes

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Science China Chemistry 2024年第8期67卷 2710-2718页

作者： Jian Yao Can Zhao Lili Shao Xiaohong Huo Xiaoming Wang Shanghai key laboratory for molecular engineering of Chiral Drugs Frontiers Science Center for Transformative MoleculesSchool of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China State key laboratory of Organometallic Chemistry and Shanghai Hongkong Joint laboratory in Chemical Synthesis Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of Chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China

By virtue of the atom-and step-economy, utilization of simple arenes as a supplant of pre-prepared aryl metal species or aryl halides for the synthesis of arylated chiral molecules has attracted great attention from the synthetic community. While transition-metal-catalyzed enantioselective diarylation of tethered alkenes has been employed to prepare important chiral cyclic compounds, the direct use of simple arenes as aryl precursors is still underdeveloped, probably due to the difficulties in the effective control of the reactivity, site-selectivity and/or enantioselectivity. Herein we report an asymmetric Pd/Ag dual metal catalytic system for the non-directed, site-and enantioselective domino Heck/intermolecular C–H functionalization of *** studies showed that Pd and Ag act in cooperation in the catalysis and the chiral bisphosphine ligand plays a bifunctional role, i.e., assisting the silver species in the cleavage of the aryl C–H bond, while inducing the enantioselectivity on direct complexation with palladium. This method provides an efficient approach to the corresponding chiral oxindoles with good enantiomeric excesses from a broad scope of arenes, including fluoroarenes, heteroarenes and several complex products derived from medicines or natural products.

关键词： asymmetric Pd/Ag dual metal catalytic system simple arenes C–H functionalization bifunctional role chiral oxindoles

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Understanding the cooperative effects in the catalysis of homodimeric fluoroacetate dehalogenase

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Science China Chemistry 2024年第7期67卷 2382-2391页

作者： Ke-Wei Chen Jia-Nan Chen Jun Zhang Chao Wang Tian-Yu Sun Yun-Dong Wu key laboratory of Computational Chemistry and Drug Design State Key Laboratory of Chemical OncogenomicSchool of Chemical Biology and BiotechnologyPeking University Shenzhen Graduate SchoolShenzhen 518055China Institute of Chemical Biology Shenzhen Bay LaboratoryShenzhen 518132China College of Chemistry and molecular engineering Peking UniversityBeijing 100871China Changping laboratory Beijing 102200China

Fluoroacetate dehalogenases(FAcD),a homodimeric enzyme,catalyzes the conversion of fluoroacetic acid to glycolic acid(GoA).It has been proved that the enzyme has a half-of-the-site ***,its catalytic(C)subunit converts the first substrate to a covalent intermediate;then,the non-catalytic(NC)subunit binds a second substrate and promotes the conversion of the intermediate in the C subunit into the final *** the release of the product,the C subunit becomes the NC subunit,and the previous NC subunit becomes the C *** elucidate the detailed mechanism behind this cooperative catalysis,we have conducted microsecond-scale MD simulations along the reaction *** simulations indicate that the substrate in the NC subunit induces W185 and Y141 adopting an open conformation in the C *** opening of W185(C)facilitates the entry of catalytic water,enhancing the catalytic activity for product formation,while the opening of Y141(C)creates an unfavorable environment for product binding,promoting its *** interaction network analysis reveals that the substrate in the NC subunit can induce conformational changes through a conserved water chain at the interface.

关键词： enzyme catalysis molecular dynamics cooperative effect pre-reaction state

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Rh(Ⅱ)-catalyzed intermolecular carboamination of pyridines via double Csp^(2)-H bond activations

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Science China Chemistry 2024年第1期67卷 374-382页

作者： Zhongfeng Luo Jingxing Jiang Lifang Zou Xiaoyu Zhou Junshan Liu Zhuofeng Ke Fengjuan Chen Huanfeng Jiang Wei Zeng key laboratory of Functional molecular engineering of Guangdong Province School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510641China School of Materials Science and engineering PCFM LabSun Yat-sen UniversityGuangzhou 510275China Guangdong Provincial key laboratory of Chinese Medicine Pharmaceutics School of Traditional Chinese MedicineSouthern Medical UniversityGuangzhou 510515China

We disclose the development of the Rh-catalyzed amine-directed remote 5,6-carboamination protocol of pyridines via dual Csp^(2)-H functionalizations.A variety of readily available 2-aminopyridines and 1,2,3-triazoles are allowed for coupling cyclization to access polyfunctionalized *** studies including DFT calculations unveil that relay carbenoidelectrophilic addition to pyridines and the sequential pyridyl Csp^(2)-H amination are involved in this *** postsynthetic utility of this methodology is showcased by versatile and site-selective modification of azaindoles.

关键词： Rh-catalysis azaindoles pyridyl Csp^(2)-H bond carboamination coupling-cyclization

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