Showing papers by "Zhen Hua Li published in 2017"
TL;DR: By using a dinuclear naphthalenediimide-based Cp*Rh acceptor and linear bipyridyl ligands, organometallic rectangles featuring dynamic behavior have been constructed and serve to illustrate a new approach to generating structurally and topologically nontrivial supramolecular architectures.
Abstract: Herein, we describe how to utilize stacking interactions to achieve selective supramolecular transformation and molecular Borromean rings (BRs). By using a dinuclear naphthalenediimide (NDI)-based Cp*Rh acceptor and linear bipyridyl ligands, organometallic rectangles featuring dynamic behavior have been constructed. Unique discrete aromatic stacking arrays were formed by inducing pyrene units as guest molecules. The topology of the BRs was realized by the use of a strategically chosen ligand which was capable of participating in D–A interactions and hydrogen bonding, as evidenced from single-crystal X-ray analysis and computational studies. These self-assembly processes underline the advantages of dynamic bonding and π–π stacking interactions, and serve to illustrate a new approach to generating structurally and topologically nontrivial supramolecular architectures.
92 citations
TL;DR: In this paper, a series of Cp*Rh- and Cp *Ir-based molecular Borromean rings (BRs) have been prepared with dihalogenated ligands (fluoranilic acid, chloranilic acid and bromianilic acid) and 4,4′-bipyridylacetylene.
82 citations
TL;DR: In this article, a Pt/W-SBA-15 catalysts with extremely low W/Si atomic ratios (≤1/80) exhibit excellent catalytic performance in the hydrogenolysis of glycerol to 1,3-PDO.
74 citations
TL;DR: In this paper, a three-component reaction of aryldiazonium tetrafluoroborates, DABCO•(SO2)2 and hydroxylamines under catalyst-free and additive-free conditions is developed, providing aryl O-aminosulfonates in good yields.
Abstract: A three-component reaction of aryldiazonium tetrafluoroborates, DABCO•(SO2)2 and hydroxylamines under catalyst-free and additive-free conditions is developed, providing aryl O-aminosulfonates in good yields. Sulfonamides could also be obtained via a one-pot process through a reaction of aryldiazonium tetrafluoroborates, DABCO·(SO2)2 and amines in the presence of N-hydroxybenzotriazole. A mechanism involved with the insertion of sulfur dioxide and hydrogen atom transfer is proposed, supported by theoretical calculations.
47 citations
TL;DR: A fluorescent probe, pep4-NP1, which can simultaneously detect H2O2 and caspase 3, the respective markers of ROS and apoptosis, is developed, providing additional information on the ROS production pathways.
41 citations
TL;DR: The palladium(II)-induced selective B(4)-H activation of an o-carboranylthioamide has been developed and proved to be a good precursor for target mononuclear or trinuclear B( 4)-H activated complexes.
Abstract: Palladium(II)-induced selective B(4)−H activation of an o-carboranylthioamide has been developed. A tetranuclear palladium(II) complex has been obtained in high yield with excellent regioselectivity. DFT calculations have confirmed that the B(4)-borometalate is lower in energy than the corresponding B(3)-borometalate. The product proved to be a good precursor for target mononuclear or trinuclear B(4)−H activated complexes.
19 citations
TL;DR: In this article, the adsorption and decomposition of formic acid (FA) on the Ga 2 O 3 (100) surface was studied with density functional theory, where the authors showed that the preferred adorption state of FA is a bridging formate with one O atom of formate filling the O(2) vacancy.
8 citations
TL;DR: Mechanistic studies suggest that the trans arrangement of the phosphite nucleophilic attack and hydrogen bond formation on the alkyne moiety is responsible for the observed Z-selectivity.
7 citations
TL;DR: It is shown that one oxygen atom of CO2 can be abstracted by silylboranes without catalysts or by diboranes in the presence of sallylborane catalysts with surprisingly low free-energy barriers so that the reaction can be realized under mild experimental conditions.
Abstract: A strategy for the reduction of CO2 to CO by or catalyzed by metal-free silylboranes has been proposed with the aid of density functional theory (DFT) computations. We showed that one oxygen atom of CO2 can be abstracted by silylboranes without catalysts or by diboranes in the presence of silylborane catalysts with surprisingly low free-energy barriers so that the reaction can be realized under mild experimental conditions. To achieve this, the reduction mechanism of CO2 by a hierarchy of silylboranes (R1)2BSi(R2)3 was systematically investigated. Several rules of thumb were obtained to guide the design of silylboranes with high activity toward CO2 reduction. After considering many factors, such as side reactions, the stability of the silylboranes, and the solvent effect, two silylboranes, (PFP)2BSi(CH2F)3 and Me2BSi(CH2F)3, suitable for the reduction of CO2 under mild experimental conditions were designed. The overall free-energy barriers for the reduction of CO2 by the two silylboranes are just 26.1–27.0 kcal mol−1 and 28.1–28.9 kcal mol−1, respectively, at 298.15 K in solution. We further showed that CO2 can be reduced to CO by diborane Me2BBMe2 using Me2BSi(CH2F)3 as the catalyst. The overall free-energy barrier for this catalytic reaction is just 30.6–30.7 kcal mol−1 at 298.15 K in solution.
5 citations
Patent•
15 Feb 2017
TL;DR: In this paper, a method for preparing a multi-ion embedded supercapacitor through adoption of an electrochemistry alkaline activation method is presented, which can improve the storage capacity of the ion embedded supercaptacitor electrode materials.
Abstract: The present invention discloses a method for preparing a multi-ion embedded supercapacitor through adoption of an electrochemistry alkaline activation method. A simple and rapid electrochemistry alkaline activation method is employed to perform activation or deactivation processing of the transition metal hydroxide containing cobalt or nickel to realize the intelligent regulation and control of storage capacity of metal cations through the hydroxide electrode materials, and is applied to an ion embedded supercapacitor. The present invention provides a universal method capable of improving the storage capacity of the ion embedded supercapacitor electrode materials, and the application range of the transition metal hydroxide electrode materials is further widened in the energy storage field.
3 citations
TL;DR: Thorough tests show that the generalized-switch-function (GSF) approach to smooth the PES computed by the MBE method can indeed give smooth potential-energy surface and is linear scaling but without losing much accuracy for very large water clusters with appropriately chosen cutoff distances.
Abstract: The many-body expansion (MBE) method is the basis of many fragment-based methods and is widely applied to the computation of large molecular systems. To reach linear-scaling computation, a cutoff must be used to discard those subsystems with long interfragment distances. However, this leads to a discontinuous potential energy surface (PES) that would cause various problems in geometry optimizations and molecular dynamics simulations. To solve this problem, we present a generalized-switch-function (GSF) approach to smooth the PES computed by the MBE method with the use of a cutoff distance. The GSFs are naturally normalized and are permutation invariant. This approach can be applied to adaptively computing any order of many-body correction energies with multilevel computational methods and is a dynamic subsystem approach. We have applied the two versions of our method, GSF-MBE(m)/L1 and GSF-MBE(m)/(L1:L2:L3), to water clusters. Thorough tests show that our method can indeed give smooth potential-energy sur...