Latest ArticlesSince graphene-based materials have shown great potential in many fields, it is important to explore ultrafast and high-efficient methods to synthesize reduced graphene oxide (rGO) using inexpensive reducing agents under mild conditions. Here, we reported a novel method for the ultrafast chemical reduction of graphene oxide (GO) at room temperature using sodium borohydride (NaBH4), sodium molybdate (Na2MoO4) and hydrochloric acid (HCl). The reduction was carried out within 2 min. A series of characterization results revealed that the obtained reduced graphene oxide has higher reduction degree than that synthesized by NaBH4 alone at high temperature. Moreover, rGO electrode based on the present reducing method exhibited a superior specific capacitance of 139.8 F/g at a current density of 1 A/g, indicating that it can be used as electrode materials for supercapacitors.
A Rh(Ⅰ)-catalyzed highly regio- and enantioselective allylic alkylation of Meldrum acid with racemic allylic substrates bearing alkyl groups has been developed. The applying of chiral bisoxazopinephosphine ligand is essential for the high yields and selectivities. This method provides a rapid access to various chiral β-alkyl-λ, δ-unsaturated carboxylic acids and their derivatives.
Carbon nanotubes (CNTs), as one-dimensional nanomaterials, show great potential in energy conversion and storage due to their efficient electrical conductivity and mass transfer. However, the security risks, time-consuming and high cost of the preparation process hinder its further application. Here, we develop that a negative pressure rather than a following gas environment can promote the generation of cobalt and nitrogen co-doped CNTs (Co/N-CNTs) by using cobalt zeolitic imidazolate framework (ZIF-67) as a precursor, in which the negative pressure plays a key role in adjusting the size of cobalt nanoparticles and stimulating the rearragement of carbon atoms for forming CNTs. Importantly, the obtained Co/N-CNTs, with high content of pyridinic nitrogen and abundant graphitized structure, exhibit superior catalytic activity for oxygen reduction reaction (ORR) with half-wave potential (E1/2) of 0.85 V and durability in terms of the minimum current loss (2%) after the 30, 000 s test. Our development provides a new pathway for large-scale and cost-effective preparation of metal-doped CNTs for various applications.
A rhodium-catalyzed directing group promoted selective C–H olefination reaction of indolizines at the 8-position is reported. Di-olefination at 2,8-positions also achieved with silver hexafluoroantimonate as an additive under similar reaction conditions. Weakly coordinating groups, such as ketone, aldehyde, amide and ester, were used as directing groups. The ester group can be removed under acid conditions and therefore is used as a traceless directing group.
Stimulus responsive materials can provide a variety of desirable properties in one equipment unit, such as optoelectronic devices, data communications, actuators, memories, sensors and capacitors. However, it remains a large challenge to design such stimulus responsive materials, especially functional materials having both dielectric switch and second harmonic generation (SHG). Here, a new stimuli-responsive switchable material [(CH3)3N(CH2)2Cl]2[Mn(SCN)4(H2O)2] was discovered as a potential second-harmonic generation (SHG) dielectric switch. It is worth noting that it has SHG characteristics before and after undergoing reversible high-temperature phase transitions. In this work, we successfully refined the tetramethylammonium cation to obtain a quasi-spherical cation, which is tetramethylchloroethyl-amine (TMCEM) cation. By substituting H with a halogen, the increased steric hindrance of the molecular makes energy barrier increased, resulting in the reversible high-temperature phase transition. At the same time, the interactions of quasi-spherical cations and [Mn(SCN)4(H2O)2]2- anions affect a non-centrosymmetric structure to induce the SHG effect. These findings provide a new approach to design novel functional switch materials.
The donor: acceptor (D: A) blend ratio plays a very important role in affecting the progress of charge transfer and energy transfer in bulk heterojunction (BHJ) organic solar cells (OSCs). The proper D: A blend ratio can provide maximized D/A interfacial area for exciton dissociation and appropriate domain size of the exciton diffusion length, which is beneficial to obtain high-performance OSCs. Here, we comprehensively investigated the relationship between various D: A blend ratios and the charge transfer and energy transfer mechanisms in OSCs based on PBDB-T and non-fullerene acceptor IT-M. Based on various D: A blend ratios, it was found that the ratio of components is a key factor to suppress the formation of triplet states and recombination energy losses. Rational D: A blend ratios can provide appropriate donor/accepter surface for charge transfer which has been powerfully verified by various detailed experimental results from the time-resolved fluorescence measurement and transient absorption (TA) spectroscopy. Optimized coherence length and crystallinity are verified by grazing incident wide-angle X-ray scattering (GIWAXS) measurements. The results are beneficial to comprehend the effects of various D: A blend ratios on charge transfer and energy transfer dynamics and provides constructive suggestions for rationally designing new materials and feedback for photovoltaic performance optimization in non-fullerene OSCs
Two types of palladium(Ⅱ)-based metallacalixarenes [ML]2+ and [ML2]2+ have been synthesized through coordination-driven self-assembly from a series of flexible pyridine-bridged diimidazole ligands [2,6-bis ((1H-imidazol-1-yl)methyl) pyridine (L1), 2,6-bis((1H-benzo[d]imidazol-1-yl)methyl)pyridine (L2), 2,6-bis((1H-naphtho[2,3-d]imidazol-1-yl)methyl)pyridine (L3)], with palladium(Ⅱ)-based building blocks [Pd(BF4)2(M1-BF4) and (tmeda)Pd(NO3)2 (M2-NO3) (tmeda = N, N, N', N'-tetramethyl-ethylenediamine)]. All complexes were characterized by NMR spectroscopy (1H NMR and 13C NMR), mass spectrometry (CSI-MS, ESI-HRMS) and elemental analysis. The single crystal X-ray diffraction analysis of [M1L22](NO3)2, [M1L23](NO3)2, [M1L23](PF6)2 and [M2L3](NO3)2 further confirmed the uniquely single bowl-shape and double bowl-shape structures. The anion binding properties within the metallacalixarenes as receptors were also investigated by NMR titration experiments in DMSO.
Proppant is a key material in the hydraulic fracturing process, which has been widely used in unconventional oil exploitation. Normal proppants are easy to sedimentate and accumulate at the entrance of shale fracture, which will block the diversion of water, oil and gas. Coated proppants (CPs) are fabricated by coating resin on normal ceramic proppants through a simple method, which is dramatically enhanced the supporting properties in shale fracture and easy to scale up. Compared with uncoated ceramic proppants, the self-suspension ability of CPs is ~11 times higher, which are able to migrate and distribute farther and deeper inside the fracture. At the same time, Coating enhanced the 23.7% of adhesive force in maximum, which makes the CPs easier to adhere on the fracture surface to supportthe shale fracture. Besides, the liquid conductivity of CPs is 60% higher than uncoated ceramic proppants at 13.6 MPa pressure. This method is expected to fabricated varieties of proppantsfor shale fracture supporting to improve the exploration of unconventional oil and gas resources.
Bis(4-fluorophenyl) substituted oxazole(2,5-Oxz) and C2(5)-C2'(5') linked bioxazole isomers(C2-C2'_BOxz, C2-C5'_BOxz and C5-C5'_BOxz) were concisely synthesized via palladium-catalyzed regioselective and sequential C—H arylation in 1–3 reaction steps along with 20%–83% of total yields from oxazole and 4-bromofluorobenzene.The linking orientation plays a key role in the packing geometry and photophysical properties of C2-C2'_BOxz, C2-C5'_BOxz and C5-C5'_BOxz. These bioxazole isomers in solid state showed significant differences in photoluminescence quantum yields (PLQY) (0.33, 0.25 and 0.04, respectively), delayed fluorescence properties and powder X-ray diffraction (PXRD) patterns, suggesting the divergence in intermolecular interactions. The theoretically calculated gradient isosurfaces and complexation energies indicate the existence of intense π-π interactions between molecular layers, which are in good agreement with the variation trend of optical properties.
A palladium-catalyzed [4 + 1] cycloaddition of prop-2-yn-1-ones with double isocyanides is developed herein. The transformation worked well to produce a series of 2-amino-4-cyanofurans with high efficiency and a broad reaction scope. Based on mechanism studies, it is believed that the palladium-catalyzed [4 + 1] imidoylative cycloaddition of prop-2-yn-1-ones was concerted. Treated with aryl amine and H2O, the [4 + 1] cycloaddition of prop-2-yn-1-ones with double isocyanides provided 2-amino-4-amidylpyrroles efficiently.
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