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Ultra-small UiO-66-NH_(2)nanoparticles immobilized on g-C_(3)N_(4)nanosheets for enhanced catalytic activity

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Green Energy & Environment 2022年第3期7卷 512-518页

作者： Zhuizhui Su Bingxing Zhang Xiuyan Cheng Fanyu Zhang Qiang Wan Lifei Liu Xiuniang Tan Dongxing Tan Lirong Zheng Jianling Zhang Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing100190China School of Chemical Sciences University of Chinese Academy of SciencesPhysical Science LaboratoryHuairou National ComprehensiveScience CenterBeijing100190China Beijing Synchrotron Radiation Facility(BSRF) Institute of High Energy PhysicsChinese Academy of SciencesBeijing100049China

UiO-66-NH_(2),an important metal-organic framework,is usually synthesized by solvothermal method and the particle size is generally larger than 200 nm,which limits its catalytic applications in chemical reactions.It is very meaningful to produce UiO-66-NH_(2) nanoparticles with ultrasmall size,but remains challenging.Herein,we synthesized UiO-66-NH_(2) nanoparticles in size of 8-15 nm that are immobilized on g-C_(3)N_(4)nanosheets.Compared with the UiO-66-NH_(2) synthesized by the traditional solvothermal method(>200 nm),the ultra-small UiO-66-NH_(2) nanoparticles immobilized on g-C_(3)N_(4)have more unsaturated coordination positions and increased Lewis acidity.Owing to these combined advantages,the ultra-small UiO-66-NH_(2)nanoparticles exhibit greatly improved catalytic activity for Meerwein-Ponndorf-Verley reaction than larger UiO-66-NH_(2)particles.

关键词： particles catalytic meaningful

Efficient catalytic removal of COS and H_(2)S over graphitized 2D micro-meso-macroporous carbons endowed with ample nitrogen sites synthesized via mechanochemical carbonization

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Green Energy & Environment 2022年第5期7卷 983-995页

作者： Xun Kan Guanqing Zhang Yingying Luo Fujian Liu Yong Zheng Yihong Xiao Yanning Cao Chak-tong Au Shijing Liang Lilong Jiang National Engineering Research Center of Chemical Fertilizer Catalyst(NERC-CFC) School of Chemical EngineeringFuzhou UniversityFuzhou350002China

Developing a suitable catalyst for the elimination of highly toxic carbonyl sulfide(COS)and hydrogen sulfide(H_(2)S) is of great significance in terms of industrial safety and environmental protection.We demonstrate here the facile synthesis of graphitized 2D micro-meso-macroporous carbons by one-step carbonization of a mixture of urea and glucose at 700–900℃.The as-synthesized graphitized catalysts,designated as 2DNHPC-x(x=urea/glucose mass ratio),are endowed with an ultra-high concentration(12.9–20.2 wt%)of stable and versatile nitrogen sites(e.***.pyrrole and pyridine)which are anchored on the surface via stable covalent bonding.As a result,the 2D-NHPC-x are active in catalytic hydrolysis of COS on pyrrolic N to H_(2)S,and the H_(2)S can be subsequently captured on pyridinic N and converted to elemental sulfur at ambient conditions over the same materials.Among the prepared catalysts,2D-NHPC-x can catalytically hydrolysize 91%of COS to H_(2)S at 30℃,whereas the conversion ratio over the common catalysts g-C_(3)N_(4)and Fe_(2)O_(3)are below 6.0%.Furthermore,these catalysts also exhibit H_(2)S conversion and sulfur selectivity of nearly 100%at 180℃with long-time durability,which is higher than those of the most reported carbonbased catalysts.In contrast,the H_(2)S capacities of activated carbon,ordered mesoporous carbons(OMC)and N-doped OMC are 3.9,1.5 and2.39 mmol g^(-1),respectively.Both the experimental and theoretical results are disclosed that 2D-NHPC-x are superior to the nitrogen-doped porous materials ever applied in simultaneous catalytic elimination of both COS and H_(2)S.

关键词： carbons catalytic endowed

Recent advances in catalytic enantioselective direct C–H bond functionalization of electrondeficient N-containing heteroarenes

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Organic Chemistry Frontiers 2022年第1期9卷 265-280页

作者： Xiao-Lan Liu Luo-Bin Jiang Mu-Peng Luo Zhi Ren Shou-Guo Wang Shenzhen Institutes of Advanced Technology Chinese Academy of Sciences1068 Xueyuan AvenueShenzhenChina College of Pharmacy Shenzhen Technology University3002 Lantian RoadShenzhenChina School of Medical Imaging Xuzhou Medical UniversityXuzhouChina

catalytic enantioselective direct C–H bond functionalization of electron-deficient N-containing heteroarenes represents one of the most straightforward and powerful protocols to construct diverse enantioenriched highly functionalized N-heteroarene products.Efficient catalytic systems and a variety of strategies for highly chemo-and stereoselective C–H functionalization of electron-deficient N-containing heteroarenes have been developed over the past few decades.This review summarized the rapid progress in the catalytic asymmetric C–H functionalization of N-containing heteroarenes and discussed the challenges and potential of the field in the current stage.

关键词： deficient catalytic enantioselective

Asymmetric catalytic Polymerization: Advances and Challenges

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高分子科学：英文版 2023年第1期41卷 1-2页

作者： Xiao-Bing Lu State Key Laboratory of Fine Chemicals Frontiers Science Center for Smart MaterialsDalian University of Technology

Most naturally occurring biomacromolecules are optically active owing to their unique chiral structural units and/or helical conformations.Some of them show specific functionalities,such as supersensitive responses to external stimuli,highly selective recognition abilities,superior mechanical properties,and excellent catalytic activity under extremely mild conditions.These functionalities result from the unique chiral structural units and orderly arrangement of building blocks in the main-chain backbones of these biological macromolecules,such as enzymes,genes,and proteins.Indeed,the sequence and stereochemistry of the repeating units in a polymeric chain also have significant influence on their material performance.Therefore,construction of functional polymers with precise control of chirality and sequence,similar to those in living systems,is of great significance.

关键词： precise catalytic bones

Preface to special column on catalytic conversion of CO_(2)

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Chinese Journal of Catalysis 2022年第7期43卷 1545-1546页

作者： Yanqiang Huang Da-Gang Yu Guoxiong Wang CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Key Laboratory of Green Chemistry&Technology of Ministry of Education College of ChemistrySichuan University State Key Laboratory of Catalysis CAS Center for Excellence in NanoscienceDalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of Sciences

With the increasing awareness of sustainable chemistry and green chemistry,catalytic conversion of carbon dioxide(CO_(2))into high value‐added and bulk chemicals is a promising tech‐nology that can utilize CO_(2) as an ideal C1 source while simulta‐neously storing renewable energy.Despite being frustrated with its thermodynamic stability and kinetic inertness,CO_(2) has been tamed for triggering catalytic constructions of highly‐valued entities like important hydrocarbon fuels and fine chemicals,mainly aiding by two scenarios:CO_(2) reduction and CO_(2)‐involved organic synthesis.Accordingly,science,industry and govern‐ment agencies have been devoted to leverage these synthetic tools in targeting the catalytic conversion of CO_(2).Therefore,it motivates us to organize the special column of“catalytic Con‐version of CO_(2)”.The column contains 14 papers,including 4 reviews,4 communications and 6 articles,which cover the frontiers and most of the research aspects of catalytic con‐version of CO_(2).

关键词： catalytic utilize valued

Degree-of-isolation shapes the catalytic performance of single-site alloy catalysts

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中国科学:化学英文版 2023年第9期66卷 2443-2444页

作者： Qiaoqiao Guan Junling Lu Key Laboratory of Precision and Intelligent Chemistry Department of Chemical PhysicsKey Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education InstitutesCollaborative Innovation Center of Chemistry for Energy Materials(iChEM)University of Science and Technology of ChinaHefei 230026China

Metal nanocatalysts have attracted widespread attention in heterogeneous catalysis for their remarkable catalytic performance.The electronic properties of metal nanoparticles govern the orbital hybridization and charge transfer between active metals and reactants;meanwhile,the local geometries of metal nanoparticles could also have a substantial impact on chemical bond breaking and bond making.

关键词： catalytic performance breaking

catalytic dechlorination of chlorobenzene in water by Pd/Fe bimetallic system

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Journal of Environmental Sciences 2003年第5期15卷 647-651页

作者： ZHOU Hong yi XU Xin hua WANG Da hui Department of Environmental Engineering Zhejiang UniversityHangzhou 310027China. College of Biological&Environmental Engineering Zhejiang University of TechnologyHangzhou 310032China

catalytic reductive dechlorination of monochlorobenzene(MCB) was carried out in the palladium/iron system. With low Pd loading(0 005%), 45% dechlorination efficiency was achieved within 5 h. Pd as catalyst accelerated the reductive dechlorination reaction. Dechlorination mechanism and kinetics were discussed. The reaction took place on the bimetal surface in a pseudo first order reaction, with the rate constant being 0 0071 min -1 ( K SA =8 0×10 -3 L/(m 2·h). The reduction product for MCB was benzene.

关键词： reductive dechlorination catalytic palladium/iron chlorobenzene

SERS monitoring of photoinduced-enhanced oxidative stress amplifier on Au@carbon dots for tumor catalytic therapy

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Light(Science & Applications) 2022年第10期11卷 2492-2502页

作者： Linjia Li Jin Yang Jiahui Wei Chunhuan Jiang Zhuo Liu Bai Yang Bing Zhao Wei Song State Key Laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012China Department of Vascular Surgery of China-Japan Union Hospital Jilin UniversityChangchun 130031China College of Basic Medical Sciences Jilin UniversityChangchun 130021China Department of Laboratory Animals College of Animal SciencesJilin UniversityChangchun 130062China State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Currently,artificial enzymes-based photodynamic therapy(PDT)is attractive due to its efficient capacity to change the immunosuppressive tumor microenvironment(TME).It is of great significance to study the therapeutic mechanism of novel artificial enzymes in TME through a monitoring strategy and improve the therapeutic effect.In this study,Au@carbon dots(Au@CDs)nanohybrids with a core-shell structure are synthesized,which not only exhibit tunable enzyme-mimicking activity under near-infrared(NIR)light,but also excellent surface-enhanced Raman scattering(SERS)properties.Therefore,Au@CDs show a good capability for monitoring NIR-photoinduced peroxidase-like catalytic processes via a SERS strategy in tumor.Moreover,the Au@CDs deplete glutathione with the cascade catalyzed reactions,thus elevating intratumor oxidative stress amplifying the reactive oxygen species damage based on the NIR-photoinduced enhanced peroxidase and glutathione oxidase-like activities,showing excellent and fast PDT therapeutic effect promoted by photothermal property in 3 min,finally leading to apoptosis in cancer cells.Through SERS monitoring,it is further found that after removing the NIR light source for 33 min,the reactive oxygen species(ROS)activity of the TME is counteracted and eliminated due to the presence of glutathione.This work presents a guidance to rationally design of artificial enzyme for ROS-involved therapeutic strategies and a new spectroscopic tool to evaluate the tumor catalytic therapy.

关键词： catalytic oxidative artificial

catalytic Enantioselective Formal Synthesis of MDM2 Antagonist RG7388 and Its Analogues

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Chinese Journal of Chemistry 2020年第5期38卷 435-438页

作者： Xue-Jie Zou Wu-Lin Yang Jing-Yan Zhu Wei-Ping Deng Shanghai Key Laboratory of New Drug Design and School of Pharmacy East China University of Science and Technology130 Meilong RoadShanghai 200237China

The catalytic asymmetric 1,3-dipolar[3+2]cycloaddition of azomethine ylides with stilbenes has been established,affording structurally diverse pyrrolidines bearing four contiguous stereocenters with stereo-diversity in generally high yields and good to excellent stereoselectivities(up to 98%yield,99:1 dr,>99%ee).Meanwhile,this strategy allowed the formal synthesis of antitumor drug RG7388(PhaseⅢclinical study)and its analogues in high efficiency.

关键词： stereo catalytic allowed