One-dimensional cobalt sulfide (CoS) acicular nanorod arrays (ANRAs) were obtained on a fluorine-doped tin oxide (FTO) substrate by a two-step approach. First, Co(3)O(4) ANRAs were synthesized, and then they were converted to CoS ANRAs for various periods. The compositions of the films obtained after various conversion periods were verified by X-ray diffraction, UV-visible spectrophotometry, and X-ray photoelectron spectroscopy; their morphologies were examined at different periods by scanning electron microscopic and transmission electron microscopic images. Electrocatalytic abilities of the films toward I(-)/I(3)(-) were verified through cyclic voltammetry (CV) and Tafel polarization curves. Long-term stability of the films in I(-)/I(3)(-) electrolyte was studied by CV. The FTO substrates with CoS ANRAs were used as the counter electrodes for dye-sensitized solar cells; a maximum power conversion efficiency of 7.67% was achieved for a cell with CoS ANRAs, under 100 mW/cm(2), which is nearly the same as that of a cell with a sputtered Pt counter electrode (7.70%). Electrochemical impedance spectroscopy was used to substantiate the photovoltaic parameters.
A new strategy for multi-molar absorption of CO2 is reported based on activating a carboxylate group in amino acid ionic liquids. It was illustrated that introducing an electron-withdrawing site to amino acid anions could reduce the negative inductive effect of the amino group while simultaneously activating the carboxylate group to interact with CO2 very efficiently. An extremely high absorption capacity of CO2 (up to 1.69 mol mol(-1) ) in aminopolycarboxylate-based amino acid ionic liquids was thus achieved. The evidence of spectroscopic investigations and quantum-chemical calculations confirmed the interactions between two kinds of sites in the anion and CO2 that resulted in superior CO2 capacities.
Because CO2 is the main greenhouse gas, its capture and catalytic conversion are thought to be significant issues to be solved at the current time. Given the thermodynamically stable and inert nature of CO2, it is highly desirable to develop advanced catalysts to facilitate the transformation of CO2 to other high-value-added chemicals under mild conditions. Within this regard, porous organic polymers (POPs), featuring large surface areas, high thermal stabilities, diverse building blocks, and tunable porous structures, are an ideal platform for the construction of heterogeneous catalysts for CO2 conversion. Incorporating active sites that are capable of activating CO2 and/or substrates into the frameworks of POPs can facilitate CO2 conversion. In this Review, the most recent advances in the design and synthesis of POP-based heterogeneous catalysts for the conversion of CO2 are summarized. We mainly focus on the synthetic strategies researchers have used for incorporating active sites into POP frameworks to prepare heterogeneous catalysts for CO2 conversion, including N-doping, metalation, and ionic functionalization. Problems remaining to be addressed in this field are analyzed, and future directions are outlined.
Acid catalysts are widely used in petrochemical reactions, the synthesis of fine chemicals, and biomass conversions in industry. To comply with the principles of green and sustainable chemistry, much attention is being paid to the replacement of traditional liquid acids with solid acid catalysts. Normally, solid acids exhibit hydrophilicity because of the unique hydrophilic nature of the acidic sites on their surfaces. Water, as a typical solvent, byproduct, or negative component in a variety of acid-catalyzed reactions, may be adsorbed on solid acids and then cause the deactivation of catalytic sites or hydrolysis of the frameworks. The development of solid acids with suitable hydrophobicity largely overcomes these issues and enhances their catalytic activities and reusability. This Review discusses some recent advances in the preparation of novel solid acids with controllable wettability and suitable hydrophobicity and highlights their application in catalyzing various reactions such as esterification, transesterification, acylation, condensation, hydration, and depolymerization of crystalline cellulose. In addition, this Review discusses how the hydrophobicity of solid acids is affected by their structures, surface characteristics, and acid centers, and determines the principles for designing solid acids with high catalytic activity and good reusability. It is instructive for researchers who are interested in designing new kinds of solid acids with improved efficiency and reusability for applications in green and sustainable chemistry.
in Wiley Online Library (wileyonlinelibrary.com)Amino acid ionic liquids (AAILs) are chemical solvents with high reactivity to CO 2 . However, they suffer from drastic increase in viscosity on the reaction with CO 2 , which significantly limits their application in the industrial capture of CO 2 . In this work, 1-ethyl-3-methylimidazolium acetate ([emim][Ac]) which also exhibits chemical affinity to CO 2 but low viscosity, and its viscosity does not increase drastically after CO 2 absorption, was proposed as the diluent for AAILs to fabricate hybrid materials. The AAIL1[emim][Ac] hybrids were found to display enhanced kinetics for CO 2 absorption, and their viscosity increase after CO 2 absorption are much less significant than pure AAILs. More importantly, owing to the fact that [emim][Ac] itself can absorb large amount of CO 2 , the AAIL1[emim][Ac] hybrids still have high absolute capacities of CO 2 . Such hybrid materials consisting of a chemical solvent plus another chemical solvent are believed to be a class of effective absorbents for CO 2 capture. a The mass fraction of [Ch][Pro] is 50%. b The mass fraction of [C 2 (N 114 ) 2 ][Gly] 2 is 40%. c The mass fraction of [N 1111 ][Gly] 2 is 40%. d The mass fraction of [C 2 OHmim][Gly] is 8%. e The mass fraction of [APmim][Gly] is 11%. f The mass fraction of DAIL is 50%. g The mass fraction of [DETA][Cl] is 36%. h The mass fraction of [P 4444 ][Gly] is 41%. i The mass fraction of [aP 4443 ][Gly] is 41%. j The mass fraction of [emim][Lys] is 49%. k The mass fraction of [emim][Gly] is 50%. l The mass fraction of MEA is 30%. m The mass fraction of MDEA is 50%. Figure 9. FTIR spectra of fresh and recycled [emim] [Gly]1[emim] [Ac].[Color figure can be viewed at wileyonlinelibrary.com]
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