4.7 Article

[Pd(NHC)(PR3)] (NHC = N-heterocyclic carbene) catalysed alcohol oxidation using molecular oxygen

期刊

DALTON TRANSACTIONS
卷 41, 期 40, 页码 12619-12623

出版社

ROYAL SOC CHEMISTRY
DOI: 10.1039/c2dt30133d

关键词

-

资金

  1. EPSRC
  2. Royal Society (University Research Fellowship)
  3. EaStCHEM School of Chemistry

向作者/读者索取更多资源

A series of [Pd(NHC)(PR3)] complexes quantitatively form [Pd(eta(2)-O-2)(NHC)(PR3)] products when submitted to an dioxygen atmosphere. Synthetic details and structural features of these Pd-peroxo complexes are described. The palladium compounds were found to be efficient catalysts in the oxidation of alcohols into corresponding carbonyl compounds using O-2 or air as oxidant. Reactions proceed at low catalyst loadings with a wide range of alcohols.

作者

我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。

评论

主要评分

4.7
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

Article Crystallography

Crystal structure of ethyl 1-(2-hydroxyethyl)-4-((4-methoxyphenyl)amino)-5-oxo-2,5-dihydro-1H-pyrrole-3-carboxylate, C16H20N2O5

Fatin Nur Ain Abdul Rashid, Muhamad Zulfaqar Bacho, Alexandra M. Z. Slawin, Mohd Abdul Fatah Abdul Manan, Saiful Azmi Johari, Mohd Fazli Mohammat

Summary: The substance is triclinic with space group P (1) over bar (no. 2). The cell parameters are a = 7.9179(7) angstrom, b = 10.1982(9) angstrom, c = 10.4144(8) angstrom, alpha = 76.184(7) degrees, beta = 87.090 (7) degrees, gamma = 73.500(8) degrees. The volume of the unit cell is 782.86(12) angstrom(3), and there are 2 molecules in the lattice. The R-gt(F) value is 0.0458, and the wR(ref)(F-2) value is 0.1333. The temperature is 93 K.

ZEITSCHRIFT FUR KRISTALLOGRAPHIE-NEW CRYSTAL STRUCTURES (2023)

Article Crystallography

Solid State Structure and Hydrogen Bonding of Some Cyclic NH Carboximides

R. Alan Aitken, Alexander J. B. Nelson, Alexandra M. Z. Slawin, Dheirya K. Sonecha

Summary: Thirteen new crystal structures of cyclic NH carboximides have been determined and compared based on their intermolecular hydrogen bonding patterns. The structures include a new cyclobutane-fused succinimide, seven new simple bi- and tricyclic succinimides derived from Diels-Alder reactions, three methylated glutarimides, a morpholinedione and adipimide, and the first seven-membered ring NH carboximide to be characterized. The compounds were found to adopt ribbon structures, centrosymmetric dimers, and bonding between NH and a remote bridging ether oxygen. Halogen bonding was also observed in one case.

CRYSTALS (2023)

Article Chemistry, Inorganic & Nuclear

Enhanced Photoluminescence and Reduced Dimensionality via Vacancy Ordering in a 10H Halide Perovskite

Hang Liu, Hassan Hafeez, David B. Cordes, Alexandra M. Z. Slawin, Gavin Peters, Stephen L. Lee, Ifor D. W. Samuel, Finlay D. Morrison

Summary: In this work, a novel inorganic halide Cs10MnSb6Cl30 with a distinctive 10H perovskite polytype structure is reported. The Cs10MnSb6Cl30 has 30% B-site vacancies ordered at both corner-and face-sharing sites, resulting in a reduction of octahedral connectivity to 1D and enhanced photoluminescence. This study demonstrates the existence of the 10H perovskite structure in halides and the potential of vacancy rearrangements to tune the optical properties of perovskite polytypes.

INORGANIC CHEMISTRY (2023)

Article Crystallography

The X-ray Structures of 2-and 3-Sulfolene and Two Halogenated Derivatives

R. Alan Aitken, Alexandra M. Z. Slawin, Dheirya K. Sonecha

Summary: This paper reports the crystal structures of 2,5-dihydrothiophene 1,1-dioxide and 2,3-dihydrothiophene 1,1-dioxide, which show perfectly planar rings with expected bond lengths and angles. In contrast, the halogenated derivatives 3,3,4,4-tetrachlorotetrahydrothiophene 1,1-dioxide and 2,3-dibromotetrahydrothiophene 1,1-dioxide exhibit twisted conformations. The degree of planarity is compared with similar 5-membered ring cyclic sulfones, and the C-H...O hydrogen bonding patterns are discussed.

JOURNAL OF CHEMICAL CRYSTALLOGRAPHY (2023)

Article Chemistry, Organic

Probing Regio- and Enantioselectivity in the Formal [2+2] Cycloaddition of C(1)-Alkyl Ammonium Enolates with β- and α,β-Substituted Trifluoromethylenones

Yihong Wang, Claire M. M. Young, David B. B. Cordes, Alexandra M. Z. Slawin, Andrew D. D. Smith

Summary: The isothiourea-catalyzed formal [2+ 2] cycloaddition of C(1)-alkyl and C(1)-unsubstituted ammonium enolates with beta- and alpha,beta-substituted trifluoromethylenones has been developed. The reaction exhibited preferential [2 + 2]-cycloaddition over the alternative [4 + 2]-cycloaddition, resulting in beta-lactones with excellent diastereo- and enantioselectivity. The regioselectivity of the reaction was determined by the substituents on both reactants.

JOURNAL OF ORGANIC CHEMISTRY (2023)

Article Chemistry, Physical

Catalytic and anticancer activity of two new Ni(II) complexes with a pyrazole based heterocyclic Schiff-base ligand: Synthesis, spectroscopy and X-ray crystallography

Suman Mandal, Mitali Sarkar, Shanku Denrah, Arka Bagchi, Arunima Biswas, David B. Cordes, Alexandra M. Z. Slawin, Nitis Chandra Saha

Summary: A new pyrazole Schiff-base ligand and its two Ni(II) complexes have been synthesized and characterized. The complexes show promising catalytic and anticancer activities.

JOURNAL OF MOLECULAR STRUCTURE (2023)

Article Chemistry, Multidisciplinary

Thermally activated delayed fluorescence and high-contrast mechanochromism of anthrone-based donor-acceptor systems

Pagidi Sudhakar, Alexandra Slawin, Eli Zysman-Colman

Summary: This article reports the synthesis and optoelectronic characterization of several luminescent materials, and explains the changes in their luminescent properties in polymer films, revealing that some of these materials exhibit delayed fluorescence and reversible photoluminescent response.

FRONTIERS IN CHEMISTRY (2023)

Article Chemistry, Organic

The (2S,2'S,4R,5S,5'R)-2,2'-Di-tert-butyl-4-hydroxy-5,5'-dimethyl-4,5'-bi(1,3-dioxolanyl)-4'-one

R. Alan Aitken, Lynn A. Power, Alexandra M. Z. Slawin

Summary: X-ray diffraction analysis confirmed that the product formed by base-induced dimerization matches the described compound structure, rather than the previously proposed isomeric structure. Additionally, a similar compound derived from a different substrate was obtained and characterized.

MOLBANK (2023)

Article Chemistry, Multidisciplinary

An air-stable [Cu(NHC)(OR)] (R = C(H)(CF3)2) complex for C-H, N-H and S-H bond activation

Sylwia Ostrowska, Pierre Arnaut, David J. Liptrot, Catherine S. J. Cazin, Steven P. Nolan

Summary: The synthesis, isolation, and full characterization of a new copper complex [Cu(IPr)(OC(H)(CF3)(2))] (IPr = 1,3-bis(2,6-diisopropylphenyl)imidazol-2-ylidene) are reported. This copper(I) complex is a versatile synthon capable of activating various X-H bonds including C-H, N-H, and S-H bonds. [Cu(IPr)(OC(H)(CF3)(2))] was investigated as a pre-catalyst in several catalytic reactions.

CHEMICAL COMMUNICATIONS (2023)

Article Chemistry, Multidisciplinary

Enantioselective isothiourea-catalysed reversible Michael addition of aryl esters to 2-benzylidene malononitriles

Alastair J. Nimmo, Jacqueline Bitai, Claire M. Young, Calum McLaughlin, Alexandra M. Z. Slawin, David B. Cordes, Andrew D. Smith

Summary: This study demonstrates an unusual reversible Michael addition reaction, using an isothiourea as a Lewis base catalyst, which produces stereoselective products. The basicity of the reaction conditions and the reactivity of the catalyst affect the selectivity of the products. By combining the reversible Michael addition with a crystallisation-induced diastereomer transformation, high yields and stereocontrol of the products can be achieved.

CHEMICAL SCIENCE (2023)

Article Materials Science, Multidisciplinary

Molecular geometry and the photophysics of thermally activated delayed fluorescence: the strange case of DMAC-py-TRZ

Ettore Crovini, Rama Dhali, Dianming Sun, Tomas Matulaitis, Thomas Comerford, Alexandra M. Z. Slawin, Cristina Sissa, Francesco Azzolin, Francesco Di Maiolo, Anna Painelli, Eli Zysman-Colman

Summary: We have studied the synthesis, optoelectronic properties, and theoretical analysis of DMAC-py-TRZ, a novel TADF emitter. The structural difference between DMAC-py-TRZ and DMAC-TRZ leads to significant changes in their steric interactions and photophysics. While the bent structure of DMAC-py-TRZ hinders TADF, emission can be observed from a relaxed orthogonal excited-state geometry. The presence of both conformers in amorphous matrices contributes to the efficiency of DMAC-py-TRZ devices through efficient energy transfer.

JOURNAL OF MATERIALS CHEMISTRY C (2023)

Article Materials Science, Multidisciplinary

Color tuning of multi-resonant thermally activated delayed fluorescence emitters based on fully fused polycyclic amine/carbonyl frameworks

John Marques dos Santos, Chin-Yiu Chan, Shi Tang, David Hall, Tomas Matulaitis, David B. Cordes, Alexandra M. Z. Slawin, Youichi Tsuchiya, Ludvig Edman, Chihaya Adachi, Yoann Olivier, Eli Zysman-Colman

Summary: Two novel p-extended amine/carbonyl-based multi-resonance thermally activated delayed fluorescence (MR-TADF) emitters have been designed and synthesized. The two emitters are isomeric, composed of nine fused rings and show green-yellow emission. Sym-DiDiKTa and Asym-DiDiKTa possess tert-butyl groups distributed in a symmetrical and asymmetrical fashion, respectively, which significantly impact the single-crystal packing structure. The devices with Sym-DiDiKTa and Asym-DiDiKTa displayed electroluminescence maxima of 543 and 544 nm, and maximum external quantum efficiencies (EQE(max)) of 9.8% and 10.5%, respectively. The maximum EQE was further improved to 19.9% by employing a hyperfluorescence strategy. The LEC with Sym-DiDiKTa as the emitter showed a ?(EL) at 551 nm and FWHM of 60 nm with luminance of 300 cd m(-2) and a fast turn-on time of less than 2 s to 100 cd m(-2).

JOURNAL OF MATERIALS CHEMISTRY C (2023)

Article Chemistry, Inorganic & Nuclear

Synthesis, characterization, and reactivity of [Pd(phosphine)(py)Cl2] (PEPPSI) and [Pd(phosphine)Cl2]2 complexes

Vladislav A. Voloshkin, Yaxu Liu, Marek Belis, Min Peng, Kristof Van Hecke, Catherine S. J. Cazin, Steven P. Nolan

Summary: The synthesis of novel phosphine palladium PEPPSI and dimer complexes bearing RuPhos, SPhos and XPhos phosphines is reported. The crystal structures of XPhos Pd PEPPSI with pyridine, SPhos Pd PEPPSI with 3-chloropyridine as throw-away ligands and the RuPhos palladium dimer were obtained and compared with previously reported congeners. The catalytic activity of these complexes was examined via a C-N coupling reaction, and it was found that RuPhos complex 2b showed the highest catalytic activity with 97% yield at a low catalyst loading. The addition of 3-pentanone significantly improved the yields of phosphine dimers and PEPPSI complexes when the reactions were performed in THF.

DALTON TRANSACTIONS (2023)

Article Chemistry, Multidisciplinary

Simply accessible platinum(ii) complexes enabling alkene hydrosilylation at ppm catalyst loadings

Benon Maliszewski, Eleonora Casillo, Perrine Lambert, Fady Nahra, Catherine Cazin, Steven Nolan

Summary: This article reports an efficient olefin hydrosilylation protocol using Pt(ii)-thioether-based pre-catalysts. These simple and readily available complexes exhibit excellent catalytic performance and offer significant advantages over existing alternatives, enabling rapid and high conversions at ppm-level catalyst loadings.

CHEMICAL COMMUNICATIONS (2023)

Article Materials Science, Multidisciplinary

Tuning the emission and exciton utilization mechanisms of pyrazine-based multi-carbazole emitters and their use in organic light-emitting diodes

Dongyang Chen, Le Zhang, Tomas Matulaitis, David B. Cordes, Alexandra M. Z. Slawin, Xiao-Hong Zhang, Ifor D. W. Samuel, Eli Zysman-Colman

Summary: By judicious molecular engineering, the efficiency of the triplet exciton harvesting mechanisms in OLEDs can be modulated, leading to improved device efficiency.

JOURNAL OF MATERIALS CHEMISTRY C (2023)

Article Chemistry, Inorganic & Nuclear

The impact of Lewis acid variation on reactions with di-tert-butyl diazo diesters

Vaibhav Bedi, Dipendu Mandal, Zahid Hussain, Shi-Ming Chen, Yile Wu, Zheng-Wang Qu, Stefan Grimme, Douglas W. Stephan

Summary: The reaction of (tBuO(2)CN)(2) with 9-BBN leads to the formation of a bicyclic heterocyclic compound, while its reactions with BF3 or [Et3Si][B(C6F5)(4)] result in the isolation of different compounds. Computational studies reveal that the steric and electronic properties of the Lewis acid are important in the formation of one of the compounds.

DALTON TRANSACTIONS (2024)

Article Chemistry, Inorganic & Nuclear

Post-synthetic molecular modifications based on Schiff base condensation reactions for designing functional paddlewheel diruthenium(ii,ii) complexes

Chisa Itoh, Haruka Yoshino, Taku Kitayama, Wataru Kosaka, Hitoshi Miyasaka

Summary: A new synthetic route for constructing functional paddlewheel diruthenium(II,II) complexes was developed, utilizing Schiff base condensation reactions. The attached Schiff base groups significantly affected the electronic states of the resulting complexes, as revealed by cyclic voltammetry and DFT calculations.

DALTON TRANSACTIONS (2024)

Article Chemistry, Inorganic & Nuclear

The pressure-stabilized polymorph of indium triiodide

Danrui Ni, Haozhe Wang, Xianghan Xu, Weiwei Xie, Robert J. Cava

Summary: A layered rhombohedral polymorph of indium(iii) triiodide is synthesized at high pressure and temperature. It has an orange color, which is different from ambient pressure InI3, which has a monoclinic molecular structure and a light-yellow color.

DALTON TRANSACTIONS (2024)

Review Chemistry, Inorganic & Nuclear

Unlocking the catalytic potential of gold(II) complexes: a comprehensive reassessment

Juan Carlos Perez-Sanchez, Raquel P. Herrera, M. Concepcion Gimeno

Summary: Gold(II) complexes have been less utilized in catalysis compared to their gold(I) and gold(III) counterparts. However, gold(II) complexes offer potential in homo-coupling and cross-coupling reactions, as they are more easily accessible through simplified oxidation and reduction processes. Gold(II) exhibits characteristics of both soft acid gold(I) and hard acid gold(III). This review explores the unique reactivity and potential applications of gold(II) species, highlighting their significance in catalytic transformations.

DALTON TRANSACTIONS (2024)

Article Chemistry, Inorganic & Nuclear

Enhancing isoprene polymerization with high activity and adjustable monomer enchainment using cyclooctyl-fused iminopyridine iron precatalysts

Nighat Yousuf, Yanping Ma, Qaiser Mahmood, Wenjuan Zhang, Yizhou Wang, Hassan Saeed, Wen-Hua Sun

Summary: In this study, a series of structurally rigid cyclooctyl-fused iminopyridine iron complexes were synthesized and used with methylaluminoxane for isoprene polymerization. The extent of steric hindrance of the ligand framework was found to significantly affect catalytic performance, with less hindrance leading to better activity and stability.

DALTON TRANSACTIONS (2024)

Article Chemistry, Inorganic & Nuclear

Improving the performance of perovskite solar cells using a dual-hole transport layer

Chenghao Song, Huiwei Du, Menglei Xu, Jie Yang, Xinyu Zhang, Jungan Wang, Yuanfang Zhang, Chengjun Gu, Rui Li, Tao Hong, Jingji Zhang, Jiangying Wang, Yongchun Ye

Summary: This study improves the performance of perovskite solar cells by using a dual-hole transport layer strategy. This strategy enhances the charge transfer efficiency of the transport layer, reduces charge recombination, and improves the quality of the perovskite film layer. Ultimately, the stability of the device is enhanced.

DALTON TRANSACTIONS (2024)

Article Chemistry, Inorganic & Nuclear

Aryl selenonium vs. aryl sulfonium counterions in polyoxometalate chemistry: the impact of Se+ cationic centers on the photocatalytic reduction of dichromate

Mahender Singh, Aakash Yadav, Ranjit Singh, Chullikkattil P. Pradeep

Summary: A new aryl selenonium polyoxometalate hybrid was developed and compared with an aryl sulfonium polyoxometalate hybrid in terms of their photocatalytic properties. It was found that the aryl selenonium hybrid exhibited better catalytic performance, which could be attributed to the larger atomic radii of selenium stabilizing the photogenerated electron-hole pair more efficiently. Additionally, the generation of elemental selenium through cleavage of C-Se bonds during catalysis was observed.

DALTON TRANSACTIONS (2024)

Article Chemistry, Inorganic & Nuclear

Construction of core-shell CoSe2/ZnIn2S4 heterostructures for efficient visible-light-driven photocatalytic hydrogen evolution

Yuhan Xie, Boyu Dong, Xuemin Wang, Siyuan Wang, Jinxi Chen, Yongbing Lou

Summary: This study successfully fabricated visible-light-responsive three-dimensional core-shell CoSe2/ZnIn2S4 heterostructures and achieved attractive activity in photocatalytic hydrogen evolution. The presence of CoSe2 improved light absorption and accelerated charge transfer kinetics. The strong interaction between CoSe2 and ZnIn2S4 reduced charge recombination, further enhancing photocatalytic activity for hydrogen evolution.

DALTON TRANSACTIONS (2024)

Article Chemistry, Inorganic & Nuclear

Promising TMDC-like optical and excitonic properties of the TiBr2 2H monolayer

Andre L. de O. Batista, Joao Marcos T. Palheta, Mauricio J. Piotrowski, Celso R. C. Rego, Diego Guedes-Sobrinho, Alexandre C. Dias

Summary: This study presents a simulation protocol that provides a solid foundation for exploring two-dimensional materials. Using the TiBr2 2H monolayer as an example, the study reveals its promising properties for optoelectronic and valleytronic applications, including its stability, spin-orbit coupling effects, and optical helicity selection rule.

DALTON TRANSACTIONS (2024)

Article Chemistry, Inorganic & Nuclear

The {Cu2I2} cluster bearing metal organic frameworks: crystal structures and fluorescence detecting performances towards cysteine and explosive molecules

Jiang Jiang, Zi-Wei Li, Zhi-Zhuan Zhang, Bin Tan, Zhao-Feng Wu, Xiao-Ying Huang

Summary: In this work, two metal organic frameworks (MOFs) containing {Cu2I2} clusters, Eu-CuI-INA and Sr-K-CuI-INA, were synthesized and characterized. Both materials have a three-dimensional structure with {Cu2I2} clusters coordinated by INA(-) ligands and Eu3+ or Sr2+ ions. The Sr-K-CuI-INA material exhibited sensitive fluorescence sensing behaviors towards cysteine and nitro-bearing molecules, showing potential applications in bio and explosive molecule sensing. This work provides a good reference for designing fluorescent MOF probes containing CuI molecules.

DALTON TRANSACTIONS (2024)

Article Chemistry, Inorganic & Nuclear

Coral-like CoSe2@N-doped carbon with a high initial coulombic efficiency as advanced anode materials for Na-ion batteries

Zhiya Lin, Jiasheng Wu, Qianwen Ye, Yulong Chen, Hai Jia, Xiaohui Huang, Shaoming Ying

Summary: Na-ion batteries (NIBs) have attracted great interest as a potential technology for grid-scale energy storage due to the wide distribution, low cost, and environmental friendliness of sodium resources. However, their implementation is hindered by low rate capability and cycling stability caused by the large ionic size of Na+. In this study, a three-dimensional nanoarchitectured coral-like CoSe2@N-doped carbon (CL-CoSe2@NC) was synthesized, and it exhibited improved sodium storage properties with better electrode kinetics and a stable SEI film.

DALTON TRANSACTIONS (2024)

Article Chemistry, Inorganic & Nuclear

Mechanism of photocatalytic CO2 reduction to HCO2H by a robust multifunctional iridium complex

Ya-Qiong Zhang, Yu Zhang, Guoping Zeng, Rong-Zhen Liao, Man Li

Summary: The mechanism and selectivity of CO2 reduction under visible light were investigated using density functional calculations. The results showed that a tetradentate PNNP-type Iridium(III) complex exhibited high activity and selectivity in the reaction.

DALTON TRANSACTIONS (2024)

Article Chemistry, Inorganic & Nuclear

Enhanced thermoelectric properties of In-filled Co4Sb12 by dispersion of reduced graphene oxide

Sanyukta Ghosh, Shubhanth Jain, Soumya Ranjan Mishra, Gerda Rogl, Peter Rogl, Ernst Bauer, B. S. Murty, A. Govindaraj, Ramesh Chandra Mallik

Summary: In this study, reduced graphene oxide (rGO) was uniformly dispersed in the In0.5Co4Sb12 bulk material by ultrasonication, which effectively reduced the lattice thermal conductivity and improved the thermoelectric efficiency.

DALTON TRANSACTIONS (2024)

Article Chemistry, Inorganic & Nuclear

An effective visible-light driven fumarate production from gaseous CO2 and pyruvate by the cationic zinc porphyrin-based photocatalytic system with dual biocatalysts

Mika Takeuchi, Yutaka Amao

Summary: This study developed an effective visible-light driven system for fumaric acid production using renewable resources such as biomass derivatives, providing an alternative to the current petroleum-based synthesis methods.

DALTON TRANSACTIONS (2024)

Article Chemistry, Inorganic & Nuclear

Tin-doped NiFe2O4 nanoblocks grown on an iron foil for efficient and stable water splitting at large current densities

Juan Jian, Meiting Wang, Zhuo Wang, Jingwen Meng, Yuqin Yang, Limin Chang

Summary: Developing low-cost and self-supported bifunctional catalysts is crucial for highly efficient water splitting devices. In this study, nano-NiFe2O4 was directly grown onto iron foil surface and Sn4+ was introduced into the NiFe2O4. The resulting Sn-NiFe2O4/IF showed low overpotentials and high current densities during oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), making it a promising catalyst for large-scale hydrogen production.

DALTON TRANSACTIONS (2024)