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Selective synthesis of the b_(11)H_(14)^(-) and b_(12)H_(12)^(2-) borane derivatives and the general mechanisms of the b-H bond condensation

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science China chemistry 2024年第3期67卷 876-881页

作者： Yi Jing Xinghua Wang Hui Han Xin-Ran Liu Xing-Chao Yu Xi-Meng Chen Donghui Wei Lai-Sheng Wang Xuenian Chen College of chemistry Green Catalysis CenterZhengzhou UniversityZhengzhou 450001China school of chemistry and Chemical Engineering Henan Key Laboratory of Boron Chemistry and Advanced Energy MaterialsHenan Normal UniversityXinxiang 453007China Department of chemistry Brown UniversityProvidenceRI 02912USA

Polyhedral boranes are a class of well-known boron molecular clusters with unique physical and chemical properties,and great efforts have been made in the past decades to find more effective synthetic ***,the established synthetic methods suffer from low efficiency and low selectivity because the mechanism of the b-H bond condensation reaction,critical for the synthesis of the polyhedral boranes,is not well *** we report highly selective and efficient synthetic methods of the salts of the tetradecahydridoundecaborate(1-)(b_(11)H^(-)_(14)) and dodecahydrido-dodecaborates(2-)(b_(12)H_(12)^(2-)) anions by employing commercially available and inexpensive starting *** theoretical and experimental investigations are carried out to elucidate the reaction *** have found that the nature of the b-H bond condensation is the dihydrogen bonding interaction in which the positively charged hydrogens(bridged hydrogens) play a crucial *** current study has not only led to more effective and selective synthetic methods for b_(11)H^(-)_(14) and b_(12)H_(12)^(2-) but also unveiled the nature of the b-H bond condensation and the general formation mechanisms of polyhedral *** finding will facilitate the development of more effective synthetic methods for polyhedral boranes and spur their wide application.

关键词： boranes polyhedral boranes dihydrogen bond nucleophilicity

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Highly Red Emissive Conjugated Homopolymers based on Double b←N bridged bipyridine Unit

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Chinese Journal of Polymer science 2024年第8期42卷 1029-1037页

作者： Yu-Yue Gao Kai-Yuan Zhang Shu-Meng Wang Hui Tong Jun Liu State Key Laboratory of Polymer Physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China school of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China

Conjugated homopolymers based on six-member rings,e.g.,polyfluorene,always exhibit blue emission and conjugated homopolymers based on five-member rings,e.g.,polythiophene,can give red emission with low *** this work,we report a series of new conjugated homopolymers based on six-member rings with high-efficiency deep-red *** repeating units of the red light emitting homopolymers are double b←N bridged bipyridine(bNbP)with the boron atoms functionalized with diphenyl,borafluorene,and 2,7-di-tert-butyl-borafluorene groups,*** relationship between the chemical structures and the opto-electronic properties of the monomers and the homopolymers has been systematically *** three polymers emit pure red light(λ_(max)=656 nm)or deep red light(λ_(max)=693 nm)with fluorescence quantum efficiency in solution higher than 60%.The polymers can be used as the emitters in solution-processed organic light-emitting diodes with red emission and decent device *** work indicates a new strategy to design highly efficient light emitting conjugated polymers.

关键词： Conjugated homopolymers Double b←N bridged bipyridine(bNbP) Deep-red emission High fluorescent efficiency

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Rational modulation of electronic structure in PtAuCuNi alloys boosts efficient electrocatalytic ethanol oxidation assisted with energy-saving hydrogen evolution

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Journal of Energy chemistry 2024年第6期93卷 557-567,I0014页

作者： Hu Yao Yinan Zheng Xin Yu Songjie Hu baolian Su Xiaohui Guo Key Lab of Synthetic and Natural Functional Molecule chemistry of Ministry of Education The College of Chemistry and Materials ScienceNorthwest UniversityXi’an 710069ShaanxiChina Department of Inorganic chemistry University of NamurBruxellesB-5000 NamurBelgium

Compared to conventional electrocatalytic water splitting,electrocatalytic ethanol oxidation reaction(EOR)along with hydrogen production is considered a more energy-efficient ***,we prepared a type of novel quaternary alloy catalyst(PtAuCuNi@NF)that exhibits excellent activity for EOR(0.215 V at 10 mA cm^(-2))and hydrogen evolution reaction(HER)(7 mV at 10 mA cm^(-2)).Experimental results demonstrated that both Cu and Ni modulated the electronic environment around Pt and *** electron-rich active center facilitates the rapid adsorption and dissociation of reactants and intermediates for both EOR and ***,in the ethanol-assisted overall water splitting(E-OWS),a current density of 10 mA cm^(-2)was achieved at 0.28 ***,an advanced acid-base self-powered system(A-bsps)that can achieve a self-powered voltage of 0.59 V was ***,the self-driven hydrogen production with zero external power supply was realized by integrating A-bsps with the E-OWS *** interesting results can provide a feasible strategy for designing and developing advanced nanoalloy-based materials for clean energy integration and use in various fields.

关键词： Pt-based alloy Electronic structure Ethanol oxidation Self-powered system Overall water splitting

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A Golden Touch in the Design of Multifunctional Porphyrin Metallacages:Host-Guest chemistry for Drug-Target Interactions

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CCS chemistry 2024年第7期6卷 1662-1671页

作者： Tamara Rodríguez-Prieto Darren Wragg Nicole Heiduk Mihyun Park Nicole Strittmatter Roland A.Fischer Angela Casini Guillermo Moreno-Alcántar Chair of Medicinal and bioinorganic chemistry Department of ChemistrySchool of Natural SciencesTechnical University of Munich85748 Garching b.München Professorship for Analytical chemistry Department of ChemistrySchool of Natural SciencesTechnical University of Munich85748 Garching b.München Chair of Inorganic and MetalOrganic chemistry Department of ChemistrySchool of Natural SciencesTechnical University of Munich85748 Garching b.München Munich Data science Institute(MDSI) Technical University of Munich85748 Garching b.München

The use of three-dimensional self-assembled metallacages(MCgs)as multimodal drug platforms holds great ***,the synthesis of MCgs with increased complexity and functionality is a great challenge since understanding of the interaction of MCgs with biological targets is still *** this context,this work reports on the integration of a gold(III)porphyrin scaffold into a prismatic MCg structure and explores its application for multimodal therapy of cancer in vitro,namely enabling both photodynamic therapy and *** experimental approaches with a state-of-the-art metadynamics theoretical study,we discovered that the gold cage shows unprecedented host-guest interaction-driven selective stabilization of guanine-quadruplex(G4)structures-validated anticancer drug targets-disclosing a new mechanism to pursue in the design of supramolecular drugs.

关键词： gold metallacages porphyrins G4stabili-zation host-guestchemistry anticanceragents

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Orientation bias of Self-Assembled Alkanes and Their Derivatives Under Dynamic Lateral Nanoconfinement Conditions

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CCS chemistry 2024年第4期6卷 1024-1033页

作者： Conditions Lihua Yu Yuanzhi Xia Tianze Hu brent Daelemans Steven De Feyter Department of chemistry Division of Molecular Imaging and PhotonicsKU LeuvenB-3001 Leuven

Self-assembled molecular networks(SAMNs)formed on crystalline solid substrates result from the spontaneous arrangement of individual molecules into structured *** interaction between molecules and the substrate leads to a nonrandom orientation of SAMNs with respect to the substrate’s *** the case of graphite,the sixfold rotational symmetry of the substrate results in an equivalent rotational degeneracy in the orientation of *** this study,we explored how nanoconfinement,that is,the restriction of SAMN formation to nanometersized areas,known as nanocorrals,could impact and potentially alleviate the orientational degeneracy of SAMNs,with emphasis on the influence of molecule symmetry,size,and intermolecular *** this end,we investigated the orientation distribution of n-alkanes and functionalized alkanes within nanocorrals,which were fabricated using scanning tunneling microscopy lithography(nanoshaving).We observed lifting of orientational degeneracy for long alkanes,contrary to shorter alkanes,which did not exhibit this orientation ***,functionalized alkanes with hydrogen bonding groups demonstrated preferential alignment regardless of length,highlighting the significance of stabilizing intermolecular interactions in the alignment *** study discussed the underlying principles of the molecular packing process and shed light on the complexity of molecular self-assembly in nanoconfined spaces.

关键词： self-assembly confinement condition nanocorral orientation bias scanning tunneling microscopy

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Direct Pointwise Comparison of FE Predictions to StereoDIC Measurements:Developments and Validation Using Double Edge-Notched Tensile Specimen

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Computer Modeling in Engineering & sciences 2024年第8期140卷 1263-1298页

作者： Troy Myers Michael A.Sutton Hubert schreier Alistair Tofts Sreehari Rajan Kattil Department of Mechanical Engineering University of South CarolinaColumbiaSC29208USA Correlated Solutions Incorporated 121 Dutchman BlvdColumbiaSC29063USA

To compare finite element analysis(FEA)predictions and stereovision digital image correlation(StereoDIC)strain measurements at the same spatial positions throughout a region of interest,a field comparison procedure is *** procedure includes(a)conversion of the finite element data into a triangular mesh,(b)selection of a common coordinate system,(c)determination of the rigid body transformation to place both measurements and FEA data in the same system and(d)interpolation of the FEA nodal information to the same spatial locations as the StereoDIC measurements using barycentric *** an aluminum Al-6061 double edge notched tensile specimen,FEA results are obtained using both the von Mises isotropic yield criterion and Hill’s quadratic anisotropic yield criterion,with the unknown Hill model parameters determined using full-field specimen strain measurements for the nominally plane stress *** Hill’s quadratic anisotropic yield criterion,the point-by-point comparison of experimentally based full-field strains and stresses to finite element predictions are shown to be in excellent agreement,confirming the effectiveness of the field comparison process.

关键词： StereoDIC spatial co-registration data transformation finite element simulations point-wise comparison of measurements and FEA predictions double edge notch specimen model validation

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Single-atom Rh catalysts for efficiently degrading Rhodamine b with high concentration

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Rare Metals 2024年第5期43卷 2331-2338页

作者： Shou-Yao Hu Jian-Ping Guan Run-Ze Ma Yu Tao Dong-Hao Liu Jia-Xin Gong Yu Xiong Department of chemistry and Chemical Engineering Central South UniversityChangsha 410083China

Highly concentrated dye wastewater has a serious effect on the quality of natural waters;thus,developing novel catalysts to degrade dyes rapidly and efficiently is of great *** the first time,this study reports an Rh single atom loaded on a nitrogen-doped carbon(SA-Rh/CN)*** catalyst exhibits an excellent processing capacity for high concentrations of Rhodamine b(Rh b),high catalytic activity(95.7% degradation of Rh b in60 min)and excellent stability(93.5% degradation efficiency after 10 stable runs).

关键词： catalyst. catalysts loaded

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Thermochemical co-conversion of biomass-plastic waste to biochar:a review

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Green Chemical Engineering 2024年第1期5卷 31-49页

作者： Adewale George Adeniyi Kingsley O.Iwuozor Ebuka Chizitere Emenike Oluwaseun J.Ajala Samuel Ogunniyi Kabir b.Muritala Department of Chemical Engineering Faculty of Engineering and TechnologyUniversity of IlorinIlorinP.M.B.1515Nigeria Department of Chemical Engineering Landmark UniversityOmu-AranKwara StateP.M.B.1001Nigeria Department of Pure and Industrial chemistry Nnamdi Azikiwe UniversityAwkaP.M.B.5025Nigeria Department of chemistry Federal University of TechnologyBosso CampusMinnaNiger StateP.M.B.65Nigeria

biomass and plastics are two of the most common municipal solid wastes globally that have continuously placed a burden on the *** is therefore important that they are properly *** coconversion offers a valuable opportunity to recycle biomass and plastics simultaneously into biochar,which reduces the time and cost of recycling them individually while producing a material with a wide range of *** study is a review of published literature that discusses the thermochemical co-processing of biomass and plastic wastes into *** was observed that co-pyrolysis and co-hydrothermal carbonization are the most commonly utilized technologies for this *** characteristics of different biomass and plastics that have been thermochemically converted into biochar were *** properties of the resulting biochar are affected by the feedstock composition,pre-treatment and blending ratio,the reactor’s configuration,reaction temperature,and the presence of a *** studies found that treating the feedstocks separately resulted in a lower yield of biochar than processing them *** biochar created by this procedure has been used as a soil additive and as an adsorbent for water *** perspectives and suggestions,such as the necessity for some technical advancement,biochar’s economic benefits,improved government participation,and raised social awareness,were also *** factors have the potential to propel this field of study to great horizons.

关键词： biomass Co-pyrolysis Plastic Thermochemical process Valorization

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Synthesis of Unprotectedα-Tertiary Amines and 1,2-Amino Alcohols from Vinyl Azides by Light Induced Denitrogenative Alkylarylation/Dialkylation

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CCS chemistry 2024年第4期6卷 1060-1070页

作者： Sifan Li Hai-Wu Du Paul W.Davies Wei Shu Department of chemistry Shenzhen Grubbs InstituteSouthern University of Science and TechnologyShenzhen 518055Guangdong school of chemistry University of BirminghamEdgbastonBirmingham B152TT

Sterically congestedα-tertiary primary amines are ubiquitous substructures in pharmaceutical and agrochemical agents yet are challenging to ***,straightforward photoredox-catalyzed access to structurally diverseα,α,α-trisubstituted primary amines from denitrogenative alkylarylation or dialkylation of vinyl azides with N-hydroxyphthalimide(NHPI)esters and cyanoarenes or aryl aldehydes has been *** use of vinyl azide as a precursor to a primary aminewas enabled by the dual role of the Hantzsch ester to form an electron donor-acceptor complex and serve as a sacrificial *** strategy provides a modular synthesis ofα-tertiary primary amines,including unprotected 1,2-amino alcohols,from simple materials with excellent functional group *** synthetic applicability of this method was demonstrated by streamlined access to 2,2-disubstituted *** investigations support two parallel reductive photocatalytic cycles allowing for the denitrogenative alkylarylation or dialkylation of vinyl azides via decarboxylative radical addition followed by heteroradical cross-coupling betweenα-amino radicals and aryl anion radicals or ketyl anion radicals.

关键词： photocatalysis α-tertiary primary amines 1 2-amino alcohols vinyl azide electron donor-acceptor complex

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CO_(2)methanation boosted by support-size-dependent strong metal-support interaction and b-O-Ti component

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Green Energy & Environment 2024年第2期9卷 321-332页

作者： Shaoyu Yuan Yushan Yang Zhangyi Xiong Peijing Guo Sufang Sun Zejiang Li Jianlong Du Yongjun Gao College of chemistry and Environmental science Hebei UniversityNo.180Wusidong RoadBaoding071002HebeiChina

Strong metal-support interaction(SMSI)has a great impact on the activity and selectivity of heterogeneous catalysts,which was usually adjusted by changing reduction temperature or processing catalyst in different ***,few researches concentrate on modulating SMSI through regulating the structure of the ***,we show how changing the surface environment of the anatase TiO_(2)(b–TiO_(2))can be used to modulate the *** moderate TiOx overlayer makes the Ni metal highly dispersed on the high specific surface area of support,resulting in a substantially enhanced CO_(2)methanation ***,a novel phenomenon was observed that boron dopants promote the for-mation of the b–O–Ti interface site,enhancing the catalytic performance of CO_(2)*** calculations confirm that the b–O–Ti structure facilitates the activation of CO_(2)and further hydrogenation to methane.

关键词： CO_(2)Methanation b-doped TiO_(2) SMSI Size-dependent

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