Articles
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Lysine-modulated synthesis of enzyme-embedded hydrogen-bonded organic frameworks for efficient carbon dioxide fixation
Chem Synth 2023;3:5. DOI: 10.20517/cs.2022.28AbstractCarbonic anhydrase (CA) is an important carbon fixation enzyme. Immobilization of CA can expand its ... MORECarbonic anhydrase (CA) is an important carbon fixation enzyme. Immobilization of CA can expand its application in the realm of adsorption, catalysis, and so on. As a typical metal-free framework, hydrogen-bonded organic frameworks (HOFs) featuring mild synthesis process, exquisite framework structure and good enzyme compatibility have been used for enzyme embedding. However, the catalytic performance of CA-embedded HOFs (CA@HOFs) is limited by the micropore size of HOFs and the slow adsorption of CO2. Herein, CA@Lys-HOF-1 was synthesized by introducing lysine (Lys), a basic amino acid, during the coprecipitation of CA and HOFs for CO2 fixation. The addition of Lys enlarged the average pore size of HOF-1 from 1.8 to 3.2 nm, whereas the introduced -NH2 groups increased the initial adsorption of CO2 from 0.55 to 1.21 cm3 g-1. Compared to CA@HOF-1, the activity of CA@Lys-HOF-1 was enhanced by 71.25%, and the corresponding production of CaCO3 was enhanced by 12.7%. After eight reaction cycles, CA@Lys-HOF-1 still maintained an output of 9.97 mg of CaCO3 every 5 min, 83.7% of the initial production. It is hoped that the CA@Lys-HOF-1 reported offers a platform for efficient and continuous fixation of CO2. LESS Full articleResearch Article|Published on: 17 Jan 2023 -
Trapezohedral platinum nanocrystals with high-index facets for high-performance hydrazine electrooxidation
Chem Synth 2023;3:4. DOI: 10.20517/cs.2022.32AbstractDirect hydrazine fuel cell is a promising portable energy conversion device due to its high ... MOREDirect hydrazine fuel cell is a promising portable energy conversion device due to its high energy density and free of carbon emissions. To realize the practical applications, the design of highly efficient electrocatalysts for hydrazine oxidation reaction (HzOR) is crucial. Metal nanocrystals with high-index facets have abundant step sites with reactivity. In this study, we prepared trapezohedral Pt nanocrystals (TPH Pt NCs) enclosed by {311} high-index facets and investigated the catalytic performance for hydrazine oxidation. TPH Pt NCs possess a specific activity of 39.1 mA·cm-2 at 0.20 V, much higher than {111}-faceted octahedral (13.9 mA·cm-2) and {100}-faceted cubic Pt NCs (9.11 mA·cm-2). Meanwhile, TPH Pt NCs also show superior stability. Density functional theory (DFT) calculation indicates that Pt(311) facilitates the deprotonation of N2H4* to N2H3* (the rate-determining step) and improves the HzOR activity. This study is helpful for the design of advanced electrocatalysts for HzOR, especially high-index faceted Pt nanocatalysts. LESS Full articleResearch Article|Published on: 9 Jan 2023 -
Photothermal catalytic H2 production over hierarchical porous CaTiO3 with plasmonic gold nanoparticles
Chem Synth 2023;3:3. DOI: 10.20517/cs.2022.30AbstractThe synergistic promotion by photocatalysis and thermocatalysis is a promising approach for sustainable hydrogen (H2) ... MOREThe synergistic promotion by photocatalysis and thermocatalysis is a promising approach for sustainable hydrogen (H2) production. Herein, we rationally design a perovskite-based catalyst with three-dimensionally ordered macroporous structure (3DOM CaTiO3-Au) for photothermal catalytic H2 production from different substrates. The hierarchical 3DOM structure facilitates light harvesting and mass diffusion of the substrates, while the gold nanoparticles (Au NPs) promote charge separation. The photogenerated and hot electrons are oriented accumulated on the surface of Au NPs. The non-metallic gold species [Au(I)] show more activity for H2 evolution. As a result, 3DOM CaTiO3-Au exhibits excellent activity for H2 production from glycerol and other substrates with hydroxyl groups. The present work demonstrates a feasible approach to improve sustainable H2 production by rationally designing and fabricating efficient photothermal catalysts. LESS Full articleResearch Article|Published on: 6 Jan 2023 -
Recent advances in shape selectivity of MFI zeolite and its effect on the catalytic performance
Chem Synth 2023;3:2. DOI: 10.20517/cs.2022.31AbstractMFI zeolite characterized by uniform pore size, adjustable acidity, and high-temperature resistance has a broad ... MOREMFI zeolite characterized by uniform pore size, adjustable acidity, and high-temperature resistance has a broad application prospect in catalytic reactions. However, controlling the product distribution of zeolite as a catalyst is still confronting great challenges and applications. It is considered as an effective way to control the product distribution by developing and improving new zeolites to modulate their shape selective effect. In recent years, researchers have achieved remarkable successes in investigating the shape selective modulation of zeolites on catalytic reaction and molecular diffusion. The microporous channels of MFI zeolite are the main places for the entry and exit of reactants or product molecules. This review provides the research progress of the shape-selective modulation of MFI zeolite channels and its influence on a series of catalytic performances in recent years. The shape-selective modulation of microporous channels of zeolite, encapsulation of micropores to metals, catalysis of mesoporous zeolite, and the distribution of framework Al were all systematically discussed. The development of advanced catalysts still faces great challenges and potential applications. Finally, we discussed the problems to be addressed urgently in the field of zeolite catalysts in the future. LESS Full articleReview|Published on: 1 Jan 2023 -
Recent progress in strategies for preparation of metal-organic frameworks and their hybrids with different dimensions
Chem Synth 2023;3:1. DOI: 10.20517/cs.2022.24AbstractAs a new kind of organic-inorganic hybrid porous material, metal-organic frameworks (MOFs) exhibit a wide ... MOREAs a new kind of organic-inorganic hybrid porous material, metal-organic frameworks (MOFs) exhibit a wide application prospect in gas storage and separation, catalysis and sensing due to their characteristics of large specific surface area, high porosity and coordination unsaturation. As more and more types of MOFs were reported, the synthetic strategies of MOFs-based materials have become a hot research topic. According to the morphological dimension, MOFs can be roughly divided into one-dimensional, two-dimensional and three-dimensional structures. Herein, we summarize the synthetic methods and principles of MOFs from multi-dimensional perspectives, and explore the growth mechanism of MOFs with different morphologies based on dynamic and thermodynamic tuning. Finally, based on the above summaries, the challenges and opportunities of MOFs in the future are discussed. LESS Full articleReview|Published on: 1 Jan 2023 -
Chemical Synthesis: Happy Birthday!
Chem Synth 2022;2:22. DOI: 10.20517/cs.2022.39Editorial|Published on: 7 Dec 2022 -
Fundamentals of the catalytic conversion of methanol to hydrocarbons
Chem Synth 2022;2:21. DOI: 10.20517/cs.2022.26AbstractFor more than four decades, the methanol-to-hydrocarbons (MTH) reaction has been a successful route to ... MOREFor more than four decades, the methanol-to-hydrocarbons (MTH) reaction has been a successful route to producing valuable fuels and chemicals from non-petroleum feedstocks. This review provides the most comprehensive summary to date of recent research concerning the mechanistic fundamentals of this important reaction, covering different reaction stages. Mechanisms that have been proposed to explain the initial C-C bond formation during the induction stage of the MTH reaction are introduced, including the methoxymethyl cation, Koch carbonylation, carbene and methane-formaldehyde processes. At present, there is no consensus regarding these hypothetical mechanisms as a consequence of the limited amount of conclusive experimental evidence. The steady state of the MTH reaction is also examined with a focus on the widely accepted indirect hydrocarbon pool mechanism and the dual cycle concept that provides a mechanistic basis for the effects of zeolite structures and reaction conditions on product distribution. In the following section, advanced characterization techniques capable of providing new insights into the formation of coke species during the MTH reaction and innovative approaches effectively inhibiting coke formation are introduced. Finally, a summary is provided and perspectives on current challenges and the future development of this area are presented. LESS Full articleReview|Published on: 6 Dec 2022 -
Alkalinity-controlled zeolite nucleation and growth: ultrafast synthesis of total-morphology zeolite L mesocrystals and adsorption evaluation
Chem Synth 2022;2:20. DOI: 10.20517/cs.2022.25AbstractOwing to the intrinsic complexity of crystallization and the heterogeneity of precursors, the specific stages ... MOREOwing to the intrinsic complexity of crystallization and the heterogeneity of precursors, the specific stages and corresponding behaviors of an actual crystallization system remain ambiguous, which makes the univariate-controlled crystallization-kinetics-regulated synthesis and design of zeolite morphology and porosity an unrealized blueprint. In this study, a facile and univariate modulation (i.e., OH-/SiO2) strategy was developed to regulate zeolite crystallization kinetics, and zeolite L mesocrystals were synthesized rapidly (within 1-2 h) with almost all LTL morphologies (from cylindrical or disc-like shapes to nanoclusters or nanocrystals) in the simplest SiO2-Al2O3-K2O-H2O system. Using time-resolved analysis of the change in the solid-liquid Si/Al nutrient and crystallinity evolution, the intertwined and complex crystallization processes of zeolite L were clearly distinguished into four distinct stages: induction, nucleation, growth, and ripening. Under alkalinity-controlled conditions, the reactivity, Si/Al distribution, and state of aluminosilicates were critical to the formation of short-range order in the amorphous matrix, which greatly influenced the nucleation frequency and assembly state. Subsequently, these nucleation differences evoked correspondingly different kinetic growth behaviors. A putative alkalinity-controlled nonclassical crystallization mechanism was uncovered, and its validity was evaluated by analyzing morphology evolution, NH4F etching, and the effects of modifiers. Furthermore, adsorption tests demonstrated the high adsorption capacity of a series of zeolite L for guest molecules with various sizes and properties (e.g., gaseous aromatic hydrocarbon, aqueous dye, and protein). LESS Full articleResearch Article|Published on: 28 Nov 2022 -
Two-dimensional materials: synthesis and applications in the electro-reduction of carbon dioxide
Chem Synth 2022;2:19. DOI: 10.20517/cs.2022.20AbstractThe emission of CO2 has become an increasingly prominent issue. Electrochemical reduction of CO2 to ... MOREThe emission of CO2 has become an increasingly prominent issue. Electrochemical reduction of CO2 to value-added chemicals provides a promising strategy to mitigate energy shortage and achieve carbon neutrality. Two-dimensional (2D) materials are highly attractive for the fabrication of catalysts owing to their special electronic and geometric properties as well as a multitude of edge active sites. Various 2D materials have been proposed for synthesis and use in the conversion of CO2 to versatile carbonous products. This review presents the latest progress on various 2D materials with a focus on their synthesis and applications in the electrochemical reduction of CO2. Initially, the advantages of 2D materials for CO2 electro-reduction are briefly discussed. Subsequently, common methods for the synthesis of 2D materials and the role of these materials in the electrochemical reduction of CO2 are elaborated. Finally, some perspectives for future investigations of 2D materials for CO2 electro-reduction are proposed. LESS Full articleReview|Published on: 28 Nov 2022 -
β-cyclodextrin mediated construction of porous helical nanoribbons from oligoaniline derivatives
Chem Synth 2022;2:18. DOI: 10.20517/cs.2022.17AbstractA novel supramolecular self-assembly nanostructure of porous helical nanoribbons (PHNRs) was developed. PHNRs from oligoaniline ... MOREA novel supramolecular self-assembly nanostructure of porous helical nanoribbons (PHNRs) was developed. PHNRs from oligoaniline derivatives were fabricated through the chemical oxidation of aniline in ani-propanol/water mixture as mediated by β-cyclodextrin (β-CD). The role of β-CD was considered vital through the modulation of the addition time point of β-CD and the molar ratio of β-CD/aniline. In addition, at the early stage of polymerization, the host-guest complex between oligoaniline and β-CD was formed, which was involved in the initial supramolecular assembly process. However, with the reorganization of the oligoaniline assemblies during the polymerization time, the abscission of β-CD from the helical nanoribbons was observed, which eventually induced the formation of PHNRs. We believe the supramolecular host-modulated assembly strategy presented herein will be instructive for the fabrication of porous supramolecular nanostructures. LESS Full articleShort Communication|Published on: 31 Oct 2022
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Advances in radical phosphorylation from 2016 to 2021
Chem Synth 2021;1:9. DOI: 10.20517/cs.2021.07AbstractOrganophosphorus compounds are of great significance in organic chemistry. Therefore, the construction of phosphorus-containing compounds ... MOREOrganophosphorus compounds are of great significance in organic chemistry. Therefore, the construction of phosphorus-containing compounds has attracted significant attention from organic chemists. Radical phosphorylation has become a powerful strategy for building organophosphorus compounds and numerous achievements have been realized in recent years. In this review, we summarize the development of the generation and application of phosphorus radicals in organic chemistry since 2016. Special emphasis is given to various new transformations involving the generation of P-centered radicals via transition metal catalytic, photochemical and electrochemical means. Recent advances in the development of metal-free catalytic phosphorylations involving P-centered radicals are also reviewed. LESS Full articleReview|Published on: 26 Aug 2021 -
Recent advances on the construction of diarylethene-based supramolecular metallacycles and metallacages via coordination-driven self-assembly
Chem Synth 2021;1:2. DOI: 10.20517/cs.2021.05AbstractDuring the past few years, the construction of diarylethene (DAE)-based supramolecular metallacycles and metallacages has ... MOREDuring the past few years, the construction of diarylethene (DAE)-based supramolecular metallacycles and metallacages has gained increasing attention due to their distinctive photophysical and photochemical properties and potential applications in magnetic switching, smart soft materials, photodynamic therapy, etc. Surprisingly, no review on the construction of discrete DAE-based supramolecular metallacycles and metallacages via coordination-driven self-assembly has been summarized to the best of our knowledge. Considering the rapid development of this field, it is time to summarize the recent development of the construction of discrete DAE-containing polygons and polyhedra. In this review, the construction of diarylethene-based metallacycles and metallacages via coordination-driven self-assembly is briefly introduced. In addition, the properties and applications of these metallacycles and metallacages are also discussed. LESS Full articleReview|Published on: 8 Jul 2021 -
Future prospects in boron chemistry: new boron compounds and Lewis acids for catalysis and materials science
Chem Synth 2021;1:10. DOI: 10.20517/cs.2021.11AbstractBoron-containing compounds have a wide range of structures and rich and multifaceted reactivity patterns. As ... MOREBoron-containing compounds have a wide range of structures and rich and multifaceted reactivity patterns. As a result, these compounds are being increasingly used in organometallic, supramolecular, organic and inorganic chemistry, as well as in catalysis and materials science. This perspective describes recent ground-breaking studies and their implications for the future development of new catalysts and materials containing one or several trivalent boron atoms. LESS Full articlePerspective|Published on: 23 Sep 2021 -
Gas probes and their application in gas therapy
Chem Synth 2021;1:3. DOI: 10.20517/cs.2021.04AbstractAs an emerging field, gas therapy attracts increasing attention because of its distinguishing features in ... MOREAs an emerging field, gas therapy attracts increasing attention because of its distinguishing features in disease treatment. However, to achieve a therapeutic effect, the concentration of gas should be carefully controlled. Thus, a suitable and convenient technology is required to monitor the gas concentration in vivo. Besides, the transportation of gas into human body and in vivo biodistribution of gas also need to be evaluated. Among the technologies adopted in gas therapy, fluorescence imaging technology is the first choice due to its high specificity, high sensitivity, and non-invasion. And as the core of fluorescence imaging, the properties of fluorescent dyes directly determine the quality of imaging. So, it is critical to choose suitable gas probes for different purposes. Here, we review common gas detection methods, including a brief introduction of fluorescence, the distinctive properties of five fluorophore cores, and the detection mechanisms of common gas probes. Then, the applications of gas probes in gas delivery, gas release, and gas therapy are summarized. At last, we discuss the potential of developing further intelligent gas probes and fluorescence imaging technologies for gas therapy. LESS Full articleReview|Published on: 6 Jul 2021 -
Schizophrenic behavior of 2,3-oxidosqualene sterol cyclase from pig liver towards 2,3-oxidosqualene analogs
Chem Synth 2021;1:6. DOI: 10.20517/cs.2021.03AbstractWe report the unusual behavior of oxidosqualene sterol cyclase from pig liver towards 2,3-oxidosqualene analogs ... MOREWe report the unusual behavior of oxidosqualene sterol cyclase from pig liver towards 2,3-oxidosqualene analogs bearing two alkyl groups different from a methyl, at their Δ18-19 double bond: unambiguous structure determinations of the products and tentative rational for their formation are described. LESS Full articleResearch Article|Published on: 3 Aug 2021
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Customization of functional MOFs by a modular design strategy for target applications
Research Article|Published on: 28 Jul 2022 -
Two-dimensional manganese oxide on ceria for the catalytic partial oxidation of hydrocarbons
Research Article|Published on: 16 Mar 2022 -
Selenium confined in ZIF-8 derived porous carbon@MWCNTs 3D networks: tailoring reaction kinetics for high performance lithium-selenium batteries
Research Article|Published on: 28 Apr 2022 -
Recent advances in circularly polarized luminescence generated by inorganic materials
Review|Published on: 24 Feb 2022 -
Nanostructured heterogeneous photocatalyst materials for green synthesis of valuable chemicals
Review|Published on: 27 Apr 2022
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