Publications by authors named "Shanlin Qiao"

A substantial challenge in employing covalent organic frameworks (COFs) for photoelectrochemical (PEC) water splitting lies in improving their solution-processability while concurrently facilitating the transfer of charges and mass to the catalytic sites. Herein, we synthesize a solution-processable conjugated reticular oligomers (CROs), and further embed ruthenium (Ru) into the CRO, forming a CRO-Ru with homo-nuclear hetero-atomic. Thereafter, CRO and CRO-Ru construct an organic-organic heterojunction membrane at the nanoscale.

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Covalent organic frameworks (COFs) face limited processability challenges as photoelectrodes in photoelectrochemical water reduction. Herein, sub-10 nm benzothiazole-based colloidal conjugated reticular oligomers (CROs) are synthesized using an aqueous nanoreactor approach, and the end-capping molecular strategy to engineer electron-deficient units onto the periphery of a CRO nanocrystalline lattices (named CROs-Cg). This results in stable and processable "electronic inks" for flexible photoelectrodes.

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Free-standing covalent organic framework (COFs) nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li in lithium-ion batteries, while simultaneously exposing affluent active sites in supercapacitors. The development of these nanofilms offers a promising solution to address the persistent challenge of imbalanced charge storage kinetics between battery-type anode and capacitor-type cathode in lithium-ion capacitors (LICs). Herein, for the first time, custom-made COF and COF nanofilms are synthesized as the anode and cathode, respectively, for an all-COF nanofilm-structured LIC.

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Due to ultrahigh theoretical capacity and ultralow redox poteneial, lithium metal is considered as a promising anode material. However, uneven lithium deposition, uncontrollable lithium dendrite formation, and fragile solid electrolyte interphase (SEI) lead to low lithium utilization, rapid capacity decay, and poor cycle performance. Herein, a robust artificial SEI film by coating the lithium surface with fibrous covalent organic framework (Fib-COF) was constructed, which effectively prevented dendrite penetration and battery short-circuits.

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Covalent organic framework (COF) film with highly exposed active sites is considered as the promising flexible self-supported electrode for in-plane micro-supercapacitor (MSC). Superlattice configuration assembled alternately by different nanofilms based on van der Waals force can integrate the advantages of each isolated layer to exhibit unexpected performances as MSC film electrodes, which may be a novel option to ensure energy output. Herein, a mesoporous free-standing A-COF nanofilm (pore size is 3.

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A series of crystalline, stable Metal (Metal = Zn, Cu, Ni, Co, Fe, and Mn)-Salen covalent organic framework (COF) complex are prepared to continuously tune the band structure of Metal-Salen COF , with the purpose of optimizing the free energy intermediate species during the hydrogen evolution reaction (HER) process. The conductive macromolecular poly(3,4-ethylenedioxythiophene) (PEDOT) is subsequently integrated into the one-dimensional (1D) channel arrays of Metal-Salen COF to form heterostructure PEDOT@Metal-Salen COF via the in situ solid-state polymerization method. Among the Metal-Salen COF and PEDOT@Metal-Salen COF complexes, the optimized PEDOT@Mn-Salen COF displays prominent electrochemical activity with an overpotential of 150 mV and a Tafel slope of 43 mV dec .

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Although reasonably specified and adjustable preparation of nanostructures with specific morphologies, ordered chemical compositions and electronic structures involving advanced energy chemistries is an important research area, high-efficiency, stable, and low-cost electrocatalysts for water splitting are greatly desirable and challenging. In this study, partially delocalized Co-S-Se ultra-thin nanosheets are obtained a liquid-liquid interface-mediated strategy at an oil-water interface. These Co-S-Se ultra-thin nanosheets exhibit different-sized lamellar structures and have an average thickness of 0.

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A series of covalent triazine frameworks (CTFs) are prepared via ionothermal synthesis for supercapacitors. Due to the feature of adjustable pore structure and rich nitrogen, CTFs with regular structure can be used as a group of model compounds to further investigate the influence of pore size and heteroatom on supercapacitors. By comparing the performance of CTFs with different pore structures and nitrogen contents, the experimental results show that BPY-CTF with high specific surface area of 2278 m g, mesopores structure, and suitable nitrogen content displays a specific capacitance of 393.

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The cycloaddition of carbon dioxide (CO) with epoxides to yield highly value-added cyclic carbonates is an effective way to chemically utilize and convert CO. Here, a heterogeneous catalyst of imidazole ionic liquid-decorated covalent organic framework with polyoxometalates (POM@ImTD-COF) was constructed by the covalent modification of ionic liquids to COFs and the electrostatic interaction between POMs and ionic liquids. The obtained POM@ImTD-COF shows high catalytic activity for CO cycloaddition reaction under mild conditions (1 atm and 80 °C) in the presence of a co-catalyst, and the catalytic activity of POM@ImTD-COF has no obvious decrease during reusing five times.

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Due to strong interlayer interaction and ease of oxidation issues of black phosphorus (BP), the domain size of artificial synthesized few-layer black phosphorus (FL-BP) crystals is often below 10 µm, which extremely limits its further applications in large-area thin-film devices and integrated circuits. Herein, a hydrogen-free electrochemical delamination strategy through weak Lewis acid intercalation enabled exfoliation is developed to produce ultralarge FL-BP single-crystalline domains with high quality. The interaction between the weak Lewis acid tetra-n-butylammonium acetate (CH COOTBA) and P atoms promotes the average domain size of FL-BP crystal up to 77.

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The fluorination/sulfofication-induced effect in the photovoltaic polymer solar cells (PSCs) needs to be paid much attention. In this work, a new donor polymer PBDB-PS2F was synthesized by heavily fluorinated and decorated S atom on the side chain of benzo[1,2-b:4,5-b']dithiophene (BDT) unit to explore the internal combined effect of F&S on the photoelectric performance. It was found that the heavy fluorination on the side chain could make PBDB-PS2F achieve a low highest occupied molecule orbital (HOMO) energy level of -5.

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Most of the mesoporous chiral mesoporous silica (CMS) was synthesized by the chiral surfactant-directing method. In this study, a facile method was designed to synthesize CMS. In this method, achiral amphiphile was used as templating agents, and dilute ammonia solution was applied to induce the chirality of the CMS.

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Various two-dimensional (2D) side-chain-substituted benzo(1,2-:4,5-')dithiophene (BDT) blocks have been used to construct donor polymers, whereas the size effect of the side chains on the photovoltaic performance was overlooked in the past few years. In this work, three size-varied conjugated spaces (benzene, naphthalene, and biphenyl) were introduced into the corresponding polymers PBDB-Ph, PBDB-Na, and PBDB-BPh. This space engineering has a significant impact on the extent of phase separation in the active layer which blended with the polymer and the acceptor ITCPTC and preserved the desired morphology.

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Generally, low band gap material-based photovoltaic devices have reduced open circuit voltage (), and realizing the trade-off between the low band gap ( < 1.6 eV) and high (>0.9 V) could be critical to give efficient polymer solar cells, especially for high-performance semitransparent PSCs and tandem solar cells.

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Electrochemical water splitting is an important strategy for the mass production of hydrogen. Development of synthesizable catalysts has always been one of the biggest obstacles to replace platinum-group catalysts. In this work, a high quality crystal polymer covalent triazine framework [CTF; Brunauer-Emmett-Teller (BET) surface area of 1562.

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Low-dimensional organic materials have given rise to tremendous interest in optoelectronic applications, owing to their controllable photonic properties. However, the controlled-synthesis approaches for organic nano-/micro-architectures are very difficult to attain, because the weak interaction (van der Waals force) between the organic molecules cannot dominate the kinetic process of crystal growth. We report a simple method, which involves selective adhesion to the organic crystal plane by hydrogen-bonding interaction for modulating the crystal growth process, which leads either to the self-assembly of one organic molecule into two-dimensional (2D) microsheets with an obvious asymmetric light propagation or one-dimensional (1D) microrods with low propagation loss.

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Group IVB transition metal (Zr and Hf) dichalcogenide (TMD) monolayers can have higher carrier mobility and higher tunneling current density than group VIB (Mo and W) TMD monolayers. Here we report the synthesis of hexagonal ZrS2 monolayer and few layers on hexagonal boron nitride (BN) using ZrCl4 and S as precursors. The domain size of ZrS2 hexagons is around 1-3 μm.

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A new acceptor-donor-acceptor (A-D-A) small molecule, namely, BDT-PO-DPP, based on the alkoxyphenyl (PO)-substituted benzo[1,2-b:4,5-b']dithiophene (BDT) derivative and the diketopyrrolopyrrole (DPP) unit was synthesized as an electron donor for solution-processed small-molecule organic solar cells (SMOSCs). BDT-PO-DPP exhibited good thermal stability, with a 5 % weight-lost temperature at 401 °C under a nitrogen atmosphere. BDT-PO-DPP exhibited a lower HOMO energy level of -5.

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A new organic small molecule, DCA3TBDF, with a 2D benzo[1,2-b:4,5-b']difuran (BDF) moiety as the central core and octyl cyanoacetate units as the end-capped blocks, was designed and synthesized for solution-processed bulk heterojunction solar cells. DCA3TBDF possesses good solubility in common organic solvents such as toluene, CH2Cl2, chlorobenzene, and CHCl3 and good thermal stability with an onset decomposition temperature with 5% weight-loss occurring at 361 °C. The DCA3TBDF thin film showed a broad absorption at λ=320-700 nm and high crystallinity.

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A novel kind of functional organic microporous polymer is designed by introducing polar organic groups (P=O and P=S) and electron-rich heterocyclic into the framework to obtain high carbon dioxide capture capacity. The estimated Brunauer-Emmett-Teller (BET) surface areas of these polymers are about 600 m(2) g(-1) and the highest CO2 uptake is 2.26 mmol g(-1) (1.

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